Dissertations / Theses: 'Pump and probe techniques'

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Griessel, Annelle. "The investigation of resveratrol with conventional and ultrafast pump-probe spectroscopy techniques." Thesis, Stellenbosch : University of Stellenbosch, 2009. http://hdl.handle.net/10019.1/3098.

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Thesis (MSc (Physics))--University of Stellenbosch, 2009.
An ultrafast pump-probe spectroscopy experiment was developed in order to investigate the fast photoinduced isomerization reaction of the molecule resveratrol. Characteristics of the resveratrol molecule are discussed, including the photoisomerization reaction from trans- to cis-resveratrol. The experimental setup for the conventional spectroscopy measurement was developed and characterized in order to investigate and understand the conventional absorption and uorescence spectroscopy of resveratrol thoroughly. The absorption spectra for both trans- and cis-resveratrol, as well as the uorescence spectra were measured, discussed and explained. This therefore forms a foundation and serves as an initial step to develop a pump-probe spectroscopy experiment for resveratrol. A general overview of ultrafast pump-probe spectroscopy is presented, as well as an explanation of the nal developed experimental setup. The principles and characteristics of the chirped pulse ampli cation (CPA) femtosecond laser source and the tunable noncollinear optical parametric ampli er (NOPA) employed as the pump pulse are discussed. The process of white light continuum (WLC) generation was investigated to utilize as the ultrashort probe pulse. Two white light continuum generation experimental setups were developed and characterized for WLC generation in a transparent medium with the fundamental CPA laser light at 775 nm (in sapphire) and with the second harmonic (SH) of the CPA light at 387 nm (in quartz). A spectrometer was designed, built and characterized in conjuction with a line focus, for simultaneous measurement of the absorption in the pumped, unpumped and reference regions in the sample. In this way the photoisomerization of resveratrol could be measured with temporal resolution as a transient absorption signal. A 420 μg/ml resveratrol solution in ethanol was investigated in this pump-probe spectroscopy experiment and the results obtained are discussed accordingly.

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Nargelas, Saulius. "Investigation of carrier dynamics in InN, InGaN, and GaAsBi by optical pump-probe techniques." Doctoral thesis, Lithuanian Academic Libraries Network (LABT), 2013. http://vddb.laba.lt/obj/LT-eLABa-0001:E.02~2012~D_20130227_085934-75237.

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The thesis is dedicated to investigation of carrier dynamics in InN, InGaN, and GaAsBi heterostructures by using light-induced transient gratings and differential transmission techniques. The experimental studies in a wide range of excess carrier densities and temperatures revealed that trap-assisted Auger recombination is the dominant recombination mechanism in MBE-grown InN layers at room temperature. Investigation of carrier dynamics in In-rich InGaN alloys revealed that density of fast nonradiative recombination centers increases with Ga content. The correlation between excess carrier lifetime and diffusion coefficient in MOCVD-grown single InGaN layer with 13% In is governed by diffusive flow to the extended defects. Investigations of carrier lifetime and diffusivity dependence on excitation fluence indicated that both nonradiative and radiative recombination contribute to an increase of excess carrier recombination rate at high photo-excitation levels in MOCVD-grown InGaN multiple quantum wells. Transient grating measurements in MBE-grown GaAsBi layers with different Bi content revealed that Bi induced potential fluctuations determine the tenfold decrease in nonequilibrium hole mobility, if compare to GaAs.
Disertacija skirta nepusiausvirųjų krūvininkų dinamikos tyrimams InN, InGaN ir GaAsBi heterosandarose naudojant šviesa indukuotų dinaminių gardelių ir skirtuminio pralaidumo metodikas. Atlikti tyrimai plačiame nepusiausvirųjų krūvininkų tankių ir bandinio temperatūrų intervale parodė, kad krūvininkų rekombinacijos sparta MBE būdu užaugintuose InN sluoksniuose dominuojantis rekombinacijos mechanizmas kambario temperatūroje yra gaudyklių įtakota Ožė rekombinacija. Nustatyta koreliacija tarp krūvininkų gyvavimo trukmės ir difuzijos koeficiento MOCVD būdu užaugintame InGaN sluoksnyje su 13% In parodė, kad krūvininkų gyvavimo trukmę lemia difuzinė jų perneša link rekobinacijos centrų. Parodoma, kad MBE metodu užaugintuose InGaN sluoksniuose su dideliu In kiekiu (x>0,7) didėjant Ga kiekiui didėja nespindulinės rekombinacijos centrų tankis, o krūvininkų rekombinacijos sparta yra termiškai aktyvuojama. MOCVD metodu užaugintose InGaN kvantinėse sandarose dinaminių gardelių tyrimais parodoma, kad spartėjančią krūvininkų rekombinaciją didėjant sužadinimo intensyvumui lemia ne tik spindulinė rekombinacija, tačiau reikia atsižvelgti ir į nespindulinės rekombinacijos spartėjimą. Nustatyta, kad į GaAs įterpiant Bi atomus daugiau nei dešimt kartų sumažėja skylių judris dėl Bi atomų kuriamų valentinės juostos fliuktuacijų.

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Lakehal, Massil. "Out of Equilibrium Lattice Dynamics in Pump Probe Setups." Thesis, Université de Paris (2019-....), 2020. http://www.theses.fr/2020UNIP7039.

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L'étude de la dynamique hors équilibre des systèmes fortement corrélés, à l'aide de laser femtoseconde, a révélé une variété de phénomènes sans analogue en physique d'équilibre. Dans cette thèse, nous étudions théoriquement la dynamique hors équilibre des degrés de liberté du réseau et leur signature en spectroscopie pompe-sonde. Nous développons une description microscopique des phonons cohérents displacive excité par le laser. La théorie capture la rétroaction de l'excitation des phonons sur le fluide électronique, qui manque dans la formulation phénoménologique actuelle. Nous montrons que cette rétroaction conduit à une oscillation avec une fréquence qui dépend du temps aux temps courts, même si le mouvement des phonons est harmonique. Pour les temps longs, cette rétroaction apparaît comme une phase résiduelle dans le signal oscillatoire. Nous appliquons la théorie au BaFe2As2, nous expliquons l'origine de la phase du signal oscillatoire rapporté dans des expériences récentes, et nous prédisons que le système oscille avec une fréquence décalé vers le rouge pour les grandes fluences. Notre théorie ouvre également la possibilité d'extraire des informations d'équilibre à partir la dynamique des phonons cohérents. Un autre phénomène intéressant qui a été observé en spectroscopie pompe-sonde est l'oscillation des fluctuations du réseau au double de la fréquence d’un phonon du système étudié. Ces oscillations sont interprétées comme une signature d'états de phonons squeezé macroscopique. Dans ce travail, nous identifions d'autres mécanismes d'oscillations à une fréquence double autre que le squeezing. Nous montrons qu'un quench de la température du bain thermique induite par la pompe, à laquelle le phonon est couplé, ou l'excitation d'un phonon cohérent pour lequel l'anharmonicité cubique est permise par symétrie peut également produire de telles oscillations en spectroscopie sans que le phonon soit dans un état squeezé. Nous concluons que, contrairement à ce qui est communément admis, les oscillations à double fréquence phononique en spectroscopie de bruit ne sont pas nécessairement une signature des phonons squeezés. Nous soulignons ce qui peut être un critère fiable pour identifier un phonon squeezé en utilisant la spectroscopie pompe-sonde
The study of the out of equilibrium dynamics of strongly correlated systems, using ultrafast pulses, uncovered a plethora of phenomena with no analog in equilibrium physics. In this thesis, we theoretically investigate the out of equilibrium dynamics of the lattice degrees of freedom and their signature in pump-probe spectroscopy. We develop a Hamiltonian-based microscopic description of laser pump induced displacive coherent phonons. The theory captures the feedback of the phonon excitation upon the electronic fluid, which is missing in the state-of-the-art phenomenological formulation. We show that this feedback leads to chirping at short timescales, even if the phonon motion is harmonic. At long times, this feedback appears as a finite phase in the oscillatory signal. We apply the theory to BaFe2As2, explain the origin of the phase in the oscillatory signal reported in recent experiments, and we predict that the system will exhibit redshifted chirping at larger fluence. Our theory also opens the possibility to extract equilibrium information from coherent phonon dynamics. Another interesting phenomenon that have been reported in pump-probe spectroscopy is the oscillation of the lattice fluctuations at double phonon frequency. These oscillations are invariably interpreted as a signature of macroscopic squeezed phonon states. In this work, we identify other mechanisms of double phonon frequency oscillations that do not involve squeezing. We show that a pump induced temperature quench of the bath, to which the phonon is coupled to, or exciting a coherent phonon for which cubic anharmonicity is allowed by symmetry can also produce such oscillations in noise spectroscopy without squeezing the phonon state. We conclude that, in contrast with what is commonly believed, double phonon frequency oscillations in noise spectroscopy are not necessarily a signature of macroscopic phonon squeezing. We point out what can be a reliable criterion to identify a squeezed phonon using pump-probe spectroscopy

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隼人, 市橋, and Hayato Ichihashi. "Studies on optical spectroscopy techniques with surface plasmon resonance." Thesis, https://doors.doshisha.ac.jp/opac/opac_link/bibid/BB13127436/?lang=0, 2020. https://doors.doshisha.ac.jp/opac/opac_link/bibid/BB13127436/?lang=0.

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表面プラズモン共鳴型超音波センサは高分解能な光音響顕微鏡用超音波受波器として期待されている．本研究では，サブナノ秒パルスレーザを利用したポンププローブシステムを構築してサブナノ秒域における表面プラズモン共鳴センサの熱・弾性的な過渡応答を光学的に評価した。特にプローブ光の反射率変化として観測される過渡応答の発生メカニズムについて，実験と理論の両方のアプローチから検討しており，観測される過渡応答は金属薄膜のプラズマ周波数の変化に起因することを明らかにした。
Surface plasmon resonance (SPR) sensor has been expected as a ultrasonic sensor used in high resolution photoacoustic microscopy (PAM). In this thesis, thermoelastic transient responses in SPR sensor were evaluated by a pump probe system with a developed sub-nanosecond pulsed laser. Especially, the mechanism of the transient response to be observed as a reflectivity change of the probe light was studied by two approaches of the experiment and the theoretical estimation. As consequence of these approaches, it was revealed that the transient response was caused by the change of the plasma frequency in a thin metal film of SPR sensor.
博士(工学)
Doctor of Philosophy in Engineering
同志社大学
Doshisha University

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Wald, Hagen. "Ultrafast carrier dynamics investigated by a novel pump and probe terahertz technique." [S.l.] : [s.n.], 2003. http://deposit.ddb.de/cgi-bin/dokserv?idn=971803943.

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Lozan, Olga. "Surface plasmons and hot electrons imaging with femtosecond pump-probe thermoreflectance." Thesis, Bordeaux, 2015. http://www.theses.fr/2015BORD0021/document.

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Ce travail est consacré à l’étude de la dynamique ultrarapide d’électrons chauds photo-excité dans des structures plasmonique. L’intérêt particulier de ce domaine réside dans le fait que les SPs, en raison de leurs caractéristiques spatio-temporelles spécifique, offrent un nouvel attrait technologique pour les processus de transport d’information ultra-rapide aux nano-échelles. Dans ce contexte, ce manuscrit offre une compréhension et une exploitation de l’une des principales limitations des technologies à base de SP : les pertes par effet Joule. Nous exploitons le fait que le mécanisme d’absorption des plasmons dans les métaux est suivi par la génération d’électrons chauds à l’échelle femtoseconde, ainsi les pertes peuvent être considrées comme une conversion d’énergie plasmon-électrons chauds. Cette conversion d’énergie est mesurée à l’aide d’une technique pompe-sonde laser femtoseconde. Nous lançons des impulsions SP que nous sondons sur des centaines de femtosecondes grace aux variations de permittivité diélectrique induites par le gaz d’électrons chaud accompagnant la propagation de SP. Le profil de température électronique est par conséquent une image de la distribution de densité de puissance de plasmon (absorption) non élargi spatialement et temporellement par diffusion de porteurs d’énergie. Nous avons pu démontrer la capacité de relier la mesure de température électronique à l’absorption du SP, révélant une absorption anormale autour d’une fente nanométrique. Les résultats expérimentaux sont en accord quantitatif avec les prédictions théoriques de la distribution de densité de puissance. Dans une seconde partie, nous avons étudié les pertes plasmoniques et leurs caractéristiques lors de sa propagation sur un film métallique semi-infini. Nous avons déterminé la vitesse de l’onde thermique électronique et son atténuation. Dans la dernière partie, nous utilisons une structure en pointe pour guider adiabatiquement et focaliser le plasmon à l’extrémité. Nous avons démontré ainsi la génération d’un point chaud nanométrique et avons mis en évidence un retard dans l’échauffement des électrons à l’extrémité de la pointe. Les perspectives et les questions ouvertes sont également discutées
In this work we explored the ultrafast dynamics of photo-excited hot electrons in plasmonic structures. The particular interest of this field resides on the fact surface plasmons (SP), because of their unrivaled temporal and spatial characteristics, provide a technological route for ultrafast information processes at the nanoscale. In this context, this manuscript provides a comprehension and the harnessing of one of the major limitation of the SP-based technologies : absorption losses by Joule heating. We exploit the fact that the mechanism of plasmon absorption in metals is followed by generation of hot electrons at femtosecond time scale, thus losses can be seen as a plasmon-to-hot-electron energy conversion. This energy conversion is measured with femtosecond pump-probe technique. Femtosecond SP pulses are launched and probed over hundred femtoseconds through the permittivity variations induced by the hot-electron gas and which accompany the SP propagation. The measured electron temperature profile is therefore an image of plasmon power density distribution (absorption) not broadened spatially and temporally by energy carrier diffusion. As an important result we demonstrated the capability to link the electronic temperature measurement to the plasmonic absorption, revealing an anomalous light absorption for a sub- slit surroundings, in quantitative agreement with predictions of the power density distribution. In a second part we studied plasmon losses and their characteristics when they propagate on semi-infinite metal film. We determined the electronic thermal wave velocity and damping. In the last part we used a focusing taper-structure to adiabatically guide and focus the plasmon at the apex. Was demonstrated the generation of a nanoscale hot spot and put in evidence a delayed electron heating at the taper apex. Perspectives and the remaining open questions are also discussed

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Titimbo, Chaparro Kelvin Ruben. "CREATION AND DETECTION OF SQUEEZED PHONONS IN PUMP AND PROBE EXPERIMENTS: A FULLY QUANTUM TREATMENT." Doctoral thesis, Università degli studi di Trieste, 2015. http://hdl.handle.net/10077/10941.

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2013/2014
Femtosecond pump and probe techniques are standard experimental methodologies used for studying ultrafast dynamics in solids, in particular phonon oscillations in target materials. So far, only semiclassical methods have been employed in order to theoretically interpret the experimental data. In contrast, a fully quantum treatment will be presented here taking into account the quantum features of the generation mechanism of excited phonons by pump laser pulses, and of the process of accessing their behaviour by probe laser pulses. A single effective Hamiltonian will be used to model the interaction between photons and phonons both for the pumping and probing processes. In addition, as they interact with their environment, mainly electrons in the target, the excited phonons cannot be considered an isolated system. Their dynamics is then that typical of open quantum systems and generated by a master equation of Lindblad form, that takes into account the dissipative and noisy effects due to the environment.In this formalism, phonon oscillations can be analysed through suitable probe photon observables. Specifically, unlike in the existing literature, we will not focus only upon the scattered probe pulse intensity, namely on the probe photon number, but also on the number variance. Through the latter some quantum features of the phonon state can be accessed; in particular, specific signals of the presence of squeezed phonons can thus be identified.
Le tecniche di "pump and probe" impulsato sono metodologie sperimentali standard usate nello studio delle dinamiche ultraveloci nei solidi, in particolare delle oscillazioni di fononi. Usualmente l'interpretazione teorica dei dati sperimentali si basa su approssimazioni semiclassiche. Una descrizione completamente quantistica e` invece sviluppata nella presente trattazione: e` basata sull'introduzione di un'unica hamiltoniana di interazione tra fotoni e fononi, capace di descrivere in modo effettivo sia il processo di eccitazione che di rivelazione dei fononi. In generale, tali fononi non possono essere considerati come isolati, ma costituiscono un sistema quantistico aperto, cioe` in interazione debole con l'ambiente esterno, formato principalmente da elettroni e dagli altri costituenti del materiale in studio. La loro dinamica deve percio` venir descritta tramite una equazione master, che tenga conto di effetti di rumore e dissipazione. In questo formalismo, le proprieta` dei fononi eccitati dagli impulsi laser di "pump" possono essere analizzate attraverso lo studio di opportune osservabili caratterizzanti i fotoni di "probe". Piu` specificatamente, si e` analizzato il comportamento non solo dell'intensita` media della luce di "probe" riflessa, cioe` del numero medio di fotoni, ma anche della relativa varianza. In questo modo, si possono evidenziare alcune caratteristiche quantistiche dei fononi: in particolare, sono stati individuati segnali specifici della presenza di fononi "squeezed"
XXVII Ciclo
1986

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Liu, Yingliang. "Structural Dynamics of DNA Hydration Shell Studied by 2D IR and Pump-Probe Technique." Doctoral thesis, Humboldt-Universität zu Berlin, 2017. http://dx.doi.org/10.18452/18559.

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Biochemische Prozesse treten in wässriger Umgebung auf und Wechselwirkungen der Wasserhülle mit Biomolekülen spielt eine Schlüsselrolle für deren Struktur und Funktion. In dieser Arbeit wird die Strukturdynamik der Wassermoleküle und Gegenionen in der umgebenden Wasserhülle der DNA mit der Methode der zweidimensionalen Infrarotspektroskopie (2D IR) sowie Anrege-Abfrage-Spektroskopie untersucht. Die Ergebnisse der vorliegenden Arbeit zeigt das starke Potenzial von Schwingungsmoden an Grenzflächen für die Abbildung und das Verständnis von Wechselwirkungen zwischen Biomolekülen und ihrer Wasserhülle. In Zukunft soll dieses Konzept auch auf andere Biomoleküle angewendet werden.
Biochemical processes occur in an aqueous environment and interactions of the water shell with biomolecules play a key role for their structure and function. In this thesis, the structural dynamics of water molecules and counterions in the hydration shell of DNA is investigated by two-dimensional infrared (2D IR) spectroscopy and pump-probe transient spectroscopy. 2D IR spectroscopy is a powerful technique that can track molecular couplings between different vibrational modes and structural fluctuations of the chemical environment on a femto- to picosecond time scale. In the present study, vibrational modes of the DNA backbone serve as probes located at the DNA-water interface. The results of this thesis demonstrate the strong potential of interfacial vibrational modes for mapping and understanding interactions between biomolecules and their water shell. In future, this concept will be applied to other biomolecular systems.

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ARESTI, MAURO. "Ultrafast Optical Spectroscopy Techniques applied to colloidal nanocrystals." Doctoral thesis, Università degli Studi di Cagliari, 2014. http://hdl.handle.net/11584/266450.

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In this thesis I will describe my experimental work based on ultrafast optical spectroscopy techniques applied to colloidal nanocrystals. Colloidal semiconductor nanocrystals in recent years have attracted a lot of attention in particular in optoelectronic applications, because they present unique optical, electronic and charge carrier transport properties that can be easily modified via colloidal chemical synthesis. In the first chapter of this thesis, I will introduce the basic concepts of nanocrystals and their optical properties, I will consider some simple models to explain the physical properties of semiconductor nanocrystals. I will briefly describe the colloidal chemical synthesis of these nanocrystals and how we can change the optical properties by simply acting on the colloidal chemical synthesis. In the second chapter I will describe the basic concepts of ultra fast optical spectroscopy techniques used in my experimental work. I will describe the basic principles and the experimental set-up of the two main techniques that I used: time-resolved photoluminescence spectroscopy (TR-PL) and transient absorption spectroscopy or also called Pump Probe. These two techniques allow to investigate in a very precise way the main optical properties and dynamics of charge carriers in nanocrystals. In the third chapter I will describe my experimental work based on timeresolved photoluminescence spectroscopy applied to CdSe=CdS core=shell nanocrystals. These nanocrystals are a reference nanocrystals and their optical properties are extensively investigated, however, some aspects are not fully understood, for example, the instability or blinking of the light emission under constant illumination in these nanocrystals is still an unsolved problem that limits the real applications. The particular spectroscopic technique that I have used variable pulse rate photoluminescence spectroscopy revealed the causes of this issue, and will give us a solution to resolve it. In the fourth chapter I will discuss novel nanostructures of CdSe=CdS multi branched shape, in this case octapod shaped nanocrystals consist of eight arms made of CdS grown on a CdSe core, these present a large crosssection for light absorption and efficient charge separation ideally suited for applications of photocatalysis. The optical spectroscopy technique used to investigate the properties of these nanocrystals are the transient absorption spectroscopy. In the fifth chapter I will discuss experimental work on Bi2S3 semiconductor nanocrystals and I will describe related optical techniques used to study the optical and electronic properties. This nanocrystal has excellent properties of optical absorption of solar radiation and can be used for the realization of solar cells. Another important property of Bi2S3 is its nontoxicity that will allow in the future to achieve efficient solar cells and easy disposal and simultaneously not damaging to the environment.

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Giese, Christian [Verfasser], and Frank [Akademischer Betreuer] Stienkemeier. "Vibrational structure and dynamics of triatomic alkali molecules and RbHe exciplexes on helium nanodroplets investigated with femtosecond and picosecond pump-probe techniques = Vibrationsstruktur und Dynamik von dreiatomigen Alkalimolekülen und RbHe Exziplexen auf Helium Nanotröpfchen, untersucht mit Femtosekunden und Picosekunden Pump-Probe Techniken." Freiburg : Universität, 2012. http://d-nb.info/1123469385/34.

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Plogmaker, Stefan. "Techniques and Application of Electron Spectroscopy Based on Novel X-ray Sources." Doctoral thesis, Uppsala universitet, Yt- och gränsskiktsvetenskap, 2012. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-168799.

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The curiosity of researchers to find novel characteristics and properties of matter constantly pushes for the development of instrumentation based on X-radiation. I present in this thesis techniques for electron spectroscopy based on developments of X-ray sources both in time structure and energy. One part describes a laser driven High-Harmonic Generation source and the application of an off-plane grating monochromator with additional beamlines and spectrometers. In initial experiments, the source is capable of producing harmonics between the 13th and 23rd of the fundamental laser 800 nm wavelength. The intensity in the 19th harmonic, after monochromatization, was measured to be above 1.2·1010 photons/second with a repetition rate of 5 kHz. The development of a chopper system synchronized to the bunch clock of an electron storage ring is also presented. The system can be used to adjust the repetition rate of a synchrotron radiation beam to values between 10 and 120 kHz, or for the modulation of continuous sources. The application of the system to both time of flight spectroscopy and laser pump X-ray probe spectroscopy is shown. It was possible to measure triple ionization of Kr and in applied studies the valence band of a laser excited dye-sensitized solar cell interface. The combination of the latter technique with transient absorption measurements is proposed. The organic molecule maleic anhydride (MA) and its binding configuration to the three anatase TiO2 crystals (101), (100), (001) has been investigated by means of Xray Photoelectron Spectroscopy (XPS) and Near Edge X-ray Absorption Fine structure Spectroscopy (NEXAFS). The results provide information on the binding configuration to the 101 crystal. High Kinetic Energy Photoelectron Spectroscopy was used to investigate multilayers of complexes of iron, ruthenium and osmium. The benefit of hard X-rays for ex-situ prepared samples is demonstrated together with the application of resonant valence band measurements to these molecules.

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Liu, Yingliang [Verfasser], Thomas [Gutachter] Elsässer, Klaus [Gutachter] Rademann, and Kannan [Gutachter] Balasubramanian. "Structural Dynamics of DNA Hydration Shell Studied by 2D IR and Pump-Probe Technique / Yingliang Liu ; Gutachter: Thomas Elsässer, Klaus Rademann, Kannan Balasubramanian." Berlin : Humboldt-Universität zu Berlin, 2017. http://d-nb.info/1189327031/34.

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Zhang, Bo. "Experimental Studies of Quantum Dynamics and Coherent Control in Homonuclear Alkali Diatomic Molecules." Doctoral thesis, KTH, Physics, 2002. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-3420.

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The main theme covered in this thesis is experimentalstudies of quantum dynamics and coherent control in homonuclearalkali diatomic molecules by ultrafast laser spectroscopy iththe implementation of pump-probe techniques.

A series of experiments have been performed on the Rb2molecules in a molecular beam as well as in a thermal oven. Thereal-time molecular quantum dynamics of the predissociatingelectronically excited D(3)¹Πu state of Rb₂, which couples to/intersects several otherneighbouring states, is investigated using wavepackets. Thepredissociation of the D state, explored by this wavepacketmethod, arises from two independent states, the (4)³Σ_u⁺and (1)³∆_u, for which the second corresponds to a much fasterdecay channel above a sharp energy threshold around 430 nm. Thelifetime of the D state above the energy threshold is obtained,τ ≈ 5 ps, by measuring the decay time of thewavepacket in a thermal oven. Further experimentalinvestigation performed in a molecular beam together withquantum calculations of wavepacket dynamics on the D state haveexplored new probe channels of wavepacket evolution: theD′(3)1Σu+ channel, which exhibits vibrational motionin a shelf state and the (4)³Σu+ channel, where direct build-up of thewavefunction is observed due to its spin-orbit oupling to the Dstate.

The real-time quantum dynamics of wavepackets confined totwo bound states, A¹Σ_u⁺(0_u⁺) and b³Π_u(0_u⁺), have been studied by experiment andcalculations. It is shown that these two states are fullycoupled by spin-orbit interaction, characterised by itsintermediate strength. The intermediate character of thedynamics is established by complicated wavepacket oscillationatterns and a value of 75 cm^-1is estimated for the coupling strength at thestate crossing.

The experiments on the Li₂molecule are performed by coherent control ofrovibrational molecular wavepackets. First, the Deutsch-Jozsaalgorithm is experimentally demonstrated for three-qubitfunctions using a pure coherent superposition of Li₂rovibrational eigenstates. The functionscharacter, either constant or balanced, is evaluated by firstimprinting the function, using a phase-tailored femtosecond(fs) pulse, on a coherent superposition of the molecularstates, and then projecting the superposition onto an ionicfinal state using a second fs pulse at a specific delay time.Furthermore, an amplitude-tailored fs pulse is used to exciteselected rovibrational eigenstates and collision induceddephasing of the wavepacket signal, due to Li₂-Ar collisions, is studied experimentally. Theintensities of quantum beats decaying with the delay time aremeasured under various pressures and the collisional crosssections are calculated for each well-defined rovibrationalquantum beat, which set the upper limitsfor ure dephasingcross sections.

Keywords:Ultrafast laser spectroscopy, pump-probetechnique, predissociation, wavepacket, pin-orbit interaction,coherent control, (pure) dephasing

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Panov, Maxim S. "Early Events in Photochemistry of Aryl Azides Used as Photoaffinity Labeling Agents." Bowling Green State University / OhioLINK, 2011. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1321571677.

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Popov, Oleg Igorevich. "Quantum beat spectroscopy of hyperfine structure in the 8p2P3/2 level of atomic cesium." Miami University / OhioLINK, 2012. http://rave.ohiolink.edu/etdc/view?acc_num=miami1344713056.

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Balducci, Lodovico. "Dynamics of hemeproteins by femtosecond X-ray techniques." Thesis, Rennes 1, 2019. http://www.theses.fr/2019REN1S115.

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Récemment, la mise au point de techniques de radiographie à résolution temporelle a ajouté la dimension temporelle à la recherche dans le domaine de la biologie structurale et celles-ci se sont avérées être d'excellents outils pour suivre l'évolution structurale des protéines lors d'une réaction. En particulier, les sources de rayons X de 4ème génération (appelées lasers à électrons libres et à rayons X), avec des impulsions de l'ordre de la femtoseconde et des fluences extrêmement élevées, sont capables de sonder des ensembles de molécules essentiellement gelées dans le temps dans des conditions physiologiques. Après un aperçu des études publiées dans la littérature scientifiques, une introduction de base des techniques utilisées est présentée, accompagnée d'une description du dispositif expérimental et du flux de réduction des données. Les deux derniers chapitres sont consacrés à la présentation des résultats obtenus au cours de deux séries d'expériences réalisées au LCLS (SLAC, Menlo Park, CA, USA), pour étudier les changements structuraux des protéines dans la réaction de photodissociation prototypique du monoxyde de carbone chez des hemoprotéines. Au cours de la première expérience, la modification structurelle globale de trois hemoprotéines a été sondée par une technique de diffusion à résolution temporelle, afin d'observer d'éventuelles différences dans ce que l'on appelle le ''protein quake'' lié à la structure de la protéine. Dans la deuxième expérience, le site actif de la myoglobine a été sondé au cours de la même réaction par absorption de rayons X. Les spectres XANES à résolution temporelle ont été comparés à des calculs théoriques, dans le cadre de la théorie de la diffusion multiple, afin d'obtenir une image détaillée de la dynamique ultrarapide. Un bref projet secondaire portait à mesurer précisément des modèles de diffusion statique de la carboxyhémoglobine, afin de définir ses structures d'équilibre multiple par comparaison avec des combinaisons linéaires de structures cristallographiques connues. En conclusion, dans cette thèse de doctorat, nous avons essayé d'apporter quelques petits éléments dans la compréhension de la dynamique ultrarapide des protéines, en appliquant à la fois des méthodes d'analyse standard (Guinier), mais aussi des méthodes presque inexplorées (calculs de diffusion multiple sur des données à résolution temporelle). Selon le système et le niveau de détail requis, ces méthodes, appliquées ici aux à des systèmes modèles, peuvent être considérées d'excellents outils dans la recherche ultérieure sur des protéines plus complexes
Recently, the development of time resolved X-ray techniques has added the time dimension to structural biology studies, and have proven to be great tools to track proteins during the course of a reaction, or a specific conformational change. In particular the 4th generation X-ray sources (so called X-ray Free-Electron Lasers), with femtosecond pulses and extremely high fluences, are capable of probing ensembles of molecules essentially frozen in time under physiological conditions. After an overview of the past studies in the field, a basic introduction of the used techniques, the description of the experimental set-up and the flow of data reduction are presented. The last two chapters are devoted to present the results obtained during two separate sets of experiments, conducted at the XPP beamline of the Linac Coherent Light Source (SLAC, Menlo Park, CA, USA), to study the protein's structural changes, upon prototypical photo-dissociation reaction of carbon monoxide from heme proteins. During the first experiment, the global structural modification of three heme proteins has been probed by means of time resolved scattering technique, in order to observe eventual differences in the so called “protein-quake” depending on the protein's structure. In the second experiment, the active site of myoglobin was probed, during the same reaction, by X-ray absorption. The time resolved XANES spectra have been compared with theoretical calculations, in the framework of the multiple scattering theory, in order to retrieve a detailed picture of the ultra-fast dynamics. A further small side-project dealt with the precise measurement of static scattering patterns of carboxy hemoglobin with the goal of defining its multiple equilibrium structures by comparison with linear combinations of known crystallographic structures. In conclusion, in this Ph.D. thesis we tried to add some small pieces in the understanding of ultra-fast proteins dynamics by applying both standard (Guinier) and almost unexplored (multiple scattering calculations on time resolved data) analysis methods: depending on the system and the level of details required, these methodologies, here applied on model systems, can be considered excellent tools for further research on more complicated proteins

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Volte, Alix. "Photo-induced cooperativity in bistable volume-changing materials." Thesis, Rennes 1, 2020. http://www.theses.fr/2020REN1S037.

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Le domaine des transitions de phase ultra-rapides est fondé sur de remarquables développements des sources d’impulsion disponibles, des THz aux rayons X. Actuellement, les techniques pompe-sonde atteignent le régime temporel de la femtoseconde, i.e. une échelle de temps plus courte que celle des déplacements atomiques. Typiquement, un laser de pompe porte un système dans un état électroniquement excité, tandis que l’évolution temporelle de la dynamique structurale est suivie grâce à une impulsion de sonde retardée temporellement. De plus, les sources laser peuvent générer des impulsions intenses, avec un nombre de photons approchant le nombre d’entités potentiellement excitées. De telles impulsions peuvent induire des états hautement excités, impliquant un nombre macroscopique d’atomes ou molécules et portant le système loin de son état d’équilibre. Ces effets précurseurs peuvent être suivis par l’établissement d’un nouvel ordre électronique et structural, et peuvent donc amener à une transition de phase du système excité. Cette approche représente une nouvelle opportunité de modifier les fonctionnalités d’un matériau : agir temporellement sur un état atomique ou moléculaire excité, plutôt qu’effectuer la commutation d’un état d’équilibre à un autre en jouant sur un paramètre de contrôle statique. De plus, les déplacements atomiques peuvent advenir selon un mouvement collectif et cohérent, d’une façon fondamentalement différente de ce qui se passe lors d’une excitation thermique incohérente. L’objectif de cette thèse était d’explorer, à l’aide de la diffraction ultrarapide de rayons X, les aspects de la dynamique couplée entre contrainte et transformation, dans le cadre des transitions de phase induite par impulsion laser dans les matériaux à changement de volume. Ce projet se situe à la croisée du domaine des transitions de phase photo-induites, de la physique des phénomènes photo-acoustiques et non-linéaires, ainsi que de l’étude des effets élastiques dans les matériaux à électrons corrélés. Nous nous attendons à ce que cet effet élastique coopératif photo-induit soit particulièrement efficace dans les matériaux bistables, montrant un changement de volume significatif à la transition. C’est le cas des composés étudiés ici, notamment dans les matériaux à transition de spin, où la coopérativité est gouvernée par le champ élastique à longue portée, émergeant du gonflement des molécules lors du passage d’un état de spin à l’autre. D’autres candidats prometteurs dans le cadre de l’exploration de l’universalité de la coopérativité élastique photo-induite, sont les isolants de Mott, qui présentent une commutation de l’état de résistivité, ainsi que les nano-cristaux d’oxydes de métaux, montrant un régime bistable à température ambiante
The field of ultrafast structural dynamics is based on remarkable developments of available pulse sources, from THz to x-rays. Currently, pump-probe techniques operate on the femtosecond time scales, i.e. faster than atomic motions. Typically, a laser pump pulse drives a system onto an electronically excited state, while the structural dynamics temporal evolution is tracked with a delayed probe pulse. Moreover, laser light sources can generate intense pulses with a number of photons approaching the number of potentially photo-excited species. Such pulses can induce highly excited states, involving a macroscopic number of atoms or molecules and driving the system far from equilibrium. These precursor effects may be followed by the establishment of a new electronic and structural order and thus may bring about a phase transition of the excited system. This represents a new approach to direct materials functionalities: timely acting on an atomic or molecular excited state, rather than switching from an equilibrium state to another by tuning a static control parameter. Moreover, such induced atomic displacements may occur in a collective coherent motion, in a fundamentally different way from incoherent thermal excitation.The goal of this PhD was to explore through ultrafast x-ray diffraction some aspects of the coupled strain-transformation dynamics, in the frame of phase transitions induced by a laser pulse in volume-changing materials. This project stands between the field of photo-induced phase transitions, the physics of photo-acoustics and non-linear wave phenomena, as well as the study of the elastic field effects in correlated electrons materials. We expect this photo-induced elastic cooperative process to be particularly efficient in bistable materials showing significant volume change at the transition, as those investigated here. It is the case of spin crossover materials, where cooperativity is governed by long-range elastic field arising from the swelling of molecules between the two spin states. Other promising candidate materials to explore the universality of photo-induced elastic cooperativity are Mott insulators exhibiting resistive switching, and metal oxide nano-crystals with a bistable regime at room temperature

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Mondal, Rajib. "Synthesis and Study of Higher Poly(Acene)s: Hexacene, Heptacene, and Derivatives." Bowling Green, Ohio : Bowling Green State University, 2007. http://rave.ohiolink.edu/etdc/view?acc%5Fnum=bgsu1187812264.

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Cyril, Jean. "Confinement élastique au sein de nanostructures : le nanofil isolé, un système modèle." Thesis, Paris 6, 2017. http://www.theses.fr/2017PA066728/document.

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Dans ce travail de thèse, nous étudions expérimentalement la dynamique vibrationnelle de nano-objets uniques métalliques ou semi-conducteurs par des techniques pompe/sonde femtosecondes. Nous démontrons d’abord que l’observation de nanofils uniques, suspendus au-dessus de tranchées permet à la fois de s’affranchir de l’effet d’étalement inhomogène des propriétés acoustiques et d’augmenter le confinement acoustique. Grâce à l’enrichissement du paysage vibrationnel ainsi obtenu, nous explorons les propriétés élastiques de nombreux systèmes : métalliques, semi-conducteurs, poreux, alliages, cœur/coquille, etc. Ensuite, nous tirons parti de l’augmentation du confinement acoustique pour observer la propagation d’ondes acoustiques gigahertz guidées le long de nanofils ou de nanopoutres. Nous montrons que la propagation de ces ondes acoustiques dans ces guides d’ondes nanométriques permet d’obtenir des informations indépendantes sur les propriétés élastiques des objets. A contrario, nous mettons en évidence que lorsque le nanofil est en contact avec un substrat, il agit comme une source acoustique monochromatique d’ondes longitudinales qui rayonne dans le substrat. Nous réalisons en transmission l’imagerie spatio-temporelle de ce champ acoustique généré et détectons acoustiquement l’orientation du nanofil sous-jacent grâce à l’anisotropie de forme du champ acoustique. Enfin, nous envisageons une preuve de concept d’un système de microscopie acoustique de résolution spatiale nanométrique en utilisant une pointe de microscopie à force atomique
Vibrational dynamics of individual nano-objects is studied experimentally using pump and probe time-resolved spectroscopy. First, suspended and individual nano-objects avoid the inhomogeneous broadening of the acoustic properties and increase the acoustics confinement inside the nano-object. Elastic properties of metallic, semiconducting, porous, alloys or core-shell nanowires are thus studied in this advantageous geometry. The increased acoustic confinement in the suspended geometry also lead us to the observation of gigahertz coherent guided acoustic phonons in single copper nanowires and gold nanobeams. We show that the observation of propagating acoustic waves in nanoscale waveguides provide additional elastic informations. Furthermore, it gives the opportunity to unambiguously discriminate which mode is excited and detected using pump and probe time-resolved spectroscopy. On the contrary, nanowires can be used as monochromatic acoustic sources of longitudinal waves when deposited on a substrate. As the acoustic source radiates longitudinal waves inside the substrate, the spatiotemporal imaging of the generated acoustic field is undergone and the nanowire’s orientation is detected in transmission thanks to the acoustic field’s anisotropy. Finally, as another step toward acoustic microscopy with nanoscale spatial resolutions, an atomic force microscopy tip is used as a waveguide and an acoustic transducer with nanometric spatial extension

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Costa, Felicissimo Viviane. "Infrared - X-ray pump probe spectroscopy." Licentiate thesis, Stockholm : Theoretical Chemistry, Royal Institute of Technology, 2005. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-324.

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Spencer, Ben. "Pump-probe spectroscopy of photovoltaic materials." Thesis, University of Manchester, 2011. https://www.research.manchester.ac.uk/portal/en/theses/pumpprobe-spectroscopy-of-photovoltaic-materials(f4b7f755-338a-4fad-814c-4dcc95d5b72d).html.

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The study of photovoltaic materials is important so as to develop new solar energy technologies: in particular, quantum-confined semiconductors could offer increased quantum efficiencies at a much lower manufacture cost. This thesis contains results from a number of pump-probe experiments designed to probe the carrier dynamics in bulk and quantum-confined photovoltaics. A THz time-domain spectrometer was designed, built and commissioned. The THz refractive indices and absorption coefficients of toluene and hexane were determined, and the spectrometer was benchmarked using a photoexcited GaAs wafer. Results are presented of time-resolved THz spectroscopy of photoexcited bulk InP as a function of laser excitation wavelength. These data were used to extract the quantum efficiency of bulk InP in order to compare with recent results for InP quantum dots. The quantum efficiency in quantum dots increases when the incident photon energy is at least twice the band gap energy, whereasthe efficiency of the bulk material is found to decrease. This is because of surface recombination, and these measurements therefore verify the potential superiority of quantum dot materials over bulk materials for use in solar energy applications. Initial measurements of quantum dots using THz spectroscopy highlighted the various experimental challenges involved and the upgrades required to study such samples in the future.The time-dependence of the photoinduced surface photovoltage (SPV) in Si was studied on nanosecond timescales by synchronizing an ultrafast laser system to a synchrotron radiation source (the SRS at Daresbury, UK), and measuring the resulting shift in the photoelectron spectrum. The equilibrium band bending was determined, and the decay of the SPV was attributed to the recombination of charge carriers across the band gap. Results are presented for the SPV in bulk ZnO and for PbS quantum dot chemically attached to ZnO. The fact that the PbS quantum dots were chemically attached to the surface without becoming oxidized was verified using X-ray photoelectron spectroscopy (XPS). The changes caused by photoexcitation occur on much longer timescales in ZnO than Si (sub-milliseconds rather than nanoseconds), and these timescales were conveniently accessed using the time-resolved XPS facility at the TEMPO beamline at Synchrotron SOLEIL (Paris, France). This is due to oxygen adsorption and desorption processes at the ZnO surface affectingthe transfer of charge carriers. The addition of PbS quantum dots to the ZnO surface was found to increase the speed of this charge transfer due to injection of carriers directly from the PbS quantum dot to the bulk ZnO conduction band.

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Faleiros, Marcelo Meira. "Espectroscopia ultrarrápida do polímero semicondutor luminescente MEH-PPV com excitação no ultravioleta." Universidade de São Paulo, 2012. http://www.teses.usp.br/teses/disponiveis/76/76132/tde-06122012-084909/.

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A indústria optoeletrônica passa por um período de transformação em que os materiais inorgânicos estão sendo substituídos pelos orgânicos, oligômeros e polímeros, na fabricação de alguns tipos de dispositivos. No entanto, fatores como baixa eficiência e tempo de vida impedem que os aparelhos com base nos polímeros entrem definitivamente no mercado. Para resolver estas questões, é necessário um conhecimento profundo da estrutura eletrônica desses materiais. Apesar do avanço científico, ainda existem pontos a esclarecer. Por exemplo, não existe um consenso sobre a natureza das excitações óticas primárias e dos processos não radiativos nos polímeros conjugados, principalmente com excitação no ultravioleta. Tais processos limitam a eficiência e podem influenciar nos processos fotoquímicos, determinando o tempo de vida de um dispositivo. Esses fenômenos ocorrem em alguns picossegundos e, portanto, a espectroscopia ultrarrápida é a técnica mais adequada para o seu estudo. Neste trabalho, foi implementado o aparato para espectroscopia de bombeio e prova em filmes finos de polímeros conjugados, no qual podem ser usados dois métodos de aquisição de dados, sensível à fase e pulso-a-pulso. O primeiro é o método padrão citado na literatura, no qual o feixe de excitação é modulado por um chopper e os sinais são medidos por amplificadores lock-in. No segundo, o condicionamento de sinais é feito por circuitos amplificadores e o processamento dos sinais é feito pulso-a-pulso. É um método que a princípio fornece melhor estatística, pois as flutuações do laser são normalizadas pulso-a-pulso, e não na média. Além disso, apresenta menor custo e torna o experimento de bombeio e prova mais simples, pois os únicos procedimentos críticos passam a ser a sobreposição dos feixes na amostra e a determinação do atraso zero entre bombeio e prova. Foi projetado e construído o circuito eletrônico de condicionamento de sinais e o software de aquisição foi desenvolvido em linguagem LabVIEW. Entretanto, o método pulso-a-pulso forneceu uma sensibilidade inadequada para o estudo de filmes poliméricos, (ΔT⁄T ~ 0,7%, limitada pelo ruído elétrico na amplificação dos pulsos detectados), em contraste com ΔT/T ~ 0,1% que foi alcançada pelo método sensível à fase. Desta maneira, foi usado o último método para o estudo da evolução do espectro e da dinâmica de emissão estimulada de um filme de MEH-PPV, com excitação no visível e no ultravioleta, permitindo o estudo da dinâmica de relaxação dos estados de mais alta energia. Os resultados no visível são compatíveis com os da literatura, o que demonstra a confiabilidade do aparato quanto à sensibilidade e resolução temporal e espectral. Os resultados com excitação no UV indicam que a transferência de energia de bandas mais energéticas para a banda π - π∗ (conversão interna) ocorre em aproximadamente 300 fs, confirmando as suposições da literatura quanto à relaxação energética ultrarrápida (regra de Kasha), além de sugerir a existência de bandas ainda mais energéticas do que as já conhecidas. Pretende-se futuramente determinar a eficiência de tal transferência energética, pois ela pode ser um fator limitante na eficiência de fotoluminescência em polímeros conjugados com excitação no ultravioleta.
The optoelectronics industry is currently undergoing a transition period in which inorganic materials are being replaced by organic materials, oligomers and polymers, in the fabrication of some types of devices. However, factors such as low efficiency and low lifetime prevent polymer based devices on entering the market definitely. The solution of these issues requires a thorough knowledge of the electronic structure of these materials, but despite of scientific advances, there are still points to be clarified. For example, there is no consensus on the nature of the primary optical excitations and non-radiative processes in conjugated polymers, specially with ultraviolet excitation. Such processes limit the efficiency and can influence the photochemical processes, determining the device lifetime. These phenomena occur on a femtosecond timescale and therefore, ultrafast spectroscopy is the most appropriate technique for their study. In this work, we implemented the apparatus for pump-probe ultrafast spectroscopy on thin films of conjugated polymers, which can be used with two methods of data acquisition, phase-sensitive and shot-by-shot. The first is the standard method reported in the literature in which the excitation beam is modulated by a chopper and the signals measured by lock-in amplifiers. In the second, the detector signal conditioning is done by conventional amplifier circuits, followed shot-to-shot signal processing. This method provides the best statistics, in principle, because the laser fluctuations are normalized for each pulse, instead of using the average. In addition, the apparatus has a lower cost and the experiment is simpler, having as critical procedures the alignment of the beams on the sample and the determination of zero delay, with all other procedures done via software. The electronic circuitry for signal conditioning was designed and built and data acquisition software that enables measurements with both methods was developed in the LabVIEW programming language. However, the shot-by-shot method provided an inadequate sensitivity for the study of polymeric films (ΔT⁄T ~0.7%, limited by electronic noise in the amplification of detector signals), compared with ΔT⁄T ~ 0.1%, which was achieved by the phase sensitive method, and was the goal at the beginning of the project. Thus, the latter method was used to study the evolution of the spectrum and dynamics of stimulated emission of a film of MEH-PPV, with excitation in the visible and UV, allowing the study of the dynamics of higher lying electronic states. The results in the visible are consistent with those reported in the literature, which demonstrates the performance of the apparatus with respect to sensitivity and time/spectral resolution. The results with UV excitation indicate that the energy transfer among the more energetic bands to the π - π* band (internal conversion) occurs in about 300 fs, confirming the assumptions of the literature on the ultrafast energy relaxation processes (Kashas rule), besides suggesting the existence of even more energetic bands than those currently known. As future work, we plan to measure the efficiency of this energy transfer process, since it may be the limiting step in determining the overall photoluminescence efficiency of conjugated polymers with ultraviolet excitation.

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Costa, Felicissimo Viviane. "Principles of Infrared - X-ray Pump-probe Spectroscopy." Doctoral thesis, KTH, School of Biotechnology (BIO), 2006. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-4245.

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The present thesis concerns theoretical studies of molecular interactions investigated by infrared and X-ray spectroscopic techniques, with emphasis on using these two techniques combined in pump-probe experiments. Four main types of studies are addressed: the use of near-edge X-ray absorption fine structure spectra (NEXAFS) to manifest through-bond and through-space interactions; the role of hydrogen bonding in the formation of X-ray photoelectron spectra as evidenced by simulations of the water dimer; the development of theory, with sample applications, for infrared X-ray pump-probe spectroscopy; and molecular dynamics simulations of light-induced fragmentation of water clusters.

Ab initio calculations indicate that NEXAFS spectra give direct information about the through-bond and through-space interactions between vacant non-conjugated π* orbitals. It is found out that the X-ray photoelectron spectrum of the water dimer differs dramatically from the monomer spectrum in that two bands are observed, separated by the chemically shifted ionization potentials of the donor and the acceptor. The hydrogen bond is responsible for the anomalously strong broadening of these two bands. The studies show that X-ray core electron ionization of the water dimer driven by an infrared field is a proper technique to prove the proton transfered state contrary to conventional X-ray photoelectron spectroscopy.

The physical aspects of the proposed new X-ray spectroscopic method - phase sensitive Infrared - X-Ray Pump-Probe Spectroscopy - are examined in detail using the wave packet technique in three applications; the NO molecule and the dynamics of proton transfer in core ionized water dimer and glyoxalmonoxime. It is found out that the phase of the infrared pump field strongly influences the trajectory of the nuclear wave packet on the ground state potential, which results in a phase dependence of the X-ray pump-probe spectra. A proper choice of the delay time of the X-ray pulse allows the direct observation of the X-ray transition in the proton transfered well of the core excited potential. It is found out that the glyoxalmonoxime molecule possesses an important feature; proton transfer accompanied by core hole hopping. Special attention is paid to the quantum control of the populations of vibrational level which is of crucial importance to shape the wave packet of desirable size.

The wave packet technique becomes computationally very expensive when the number of nuclear degrees of freedom is large. Molecular dynamics is used instead in studies of light-induced nuclear kinetics in the water hexamer cluster. We predict a novel mechanism of the mechanical action of light on atoms and molecules. This mechanism is based on the rectification of the Lorentz force, which gives a unique opportunity of direct site selective mechanical action of light on atoms and molecules inside large systems like clusters or biomolecules.

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Costa, Felicíssimo Viviane. "Principles of infrared - x-ray pump-probe spectroscopy /." Stockholm : Royal Insitute of Technology, 2006. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-4245.

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Reinertsen, Johannes F. "Simulation of Ultrafast Pump-Probe Measurements for Semiconductors." Thesis, Norges teknisk-naturvitenskapelige universitet, Institutt for elektronikk og telekommunikasjon, 2012. http://urn.kb.se/resolve?urn=urn:nbn:no:ntnu:diva-19336.

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Ultrafast pump-probe spectroscopy is a powerful technique for measuring decay times for an optically excited system, e.g. a semiconductor, on the pico- to femtosecond time scale. We present both a classical approach and a quantum mechanical density matrix approach to simulate the pump-probe signal and compare the two. The main features of a typical pump-probe experiment are explained and the "coherent artifact" is accounted for. With a three-level density matrix approach we explain some experimental features from pump-probe studies of gallium arsenide (GaAs). A simple model for simulating pump-probe of semiconductors is introduced, and the relation to the density matrix approach is derived. We also show how the semiconductor model reproduces the main features of experimental data from pump-probe studies of GaAs.

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Specht, Marion. "Comportement mécanique de films minces de chalcogénures sous irradiation de photons." Thesis, Rennes 1, 2017. http://www.theses.fr/2017REN1S087/document.

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Ce travail est dédié à la compréhension de phénomènes photoinduits dansles verres de chalcogénure. Ces phénomènes, bien que connus depuis des années,ne sont pas encore bien compris. Travailler sur des couches minces, fabriquées icipar co-pulvérisation cathodique, ajoute une diffculté supplémentaire : il y a peude matière qui interagit avec la lumière et il faut composer avec la présence dusubstrat. Afin d'étudier les phénomènes photoinduits, il a été nécessaire d'adapterdes techniques expérimentales déjà existantes telles que la spectroscopie pompe-sonde, qui permet d'étudier la dynamique électronique ultra-rapide (inférieure à lananoseconde) et les capteurs au quartz piezoélectrique qui permettent de mesurerla masse volumique et les modules mécaniques du matériau déposé à leurs surface.Des essais préliminaires de résonance en transmission ont été également réalisés etsont prometteurs. Une machine de DMA (Dynamical Mechanical Analysis) a étéspécialement conçue au laboratoire afin de réaliser une étude dynamique des verres de chalcogénures sous formes de fibres et de films minces. Toutes ces techniquesexpérimentales permettent d'étudier les effets photoinduits à différentes échelles detemps et de mieux les expliquer
This work aims to understand photoinduced phenomena in chalcogenide glasses. These phenomena are known for years but yet not fully understood. Studying thin films, deposited by co-sputtering here, adds an other difficulty : the light-matter interaction takes place in a small amount of matter and it is inevitable to deal with the substrate. To study these photoinduced effects, it was necessary to adapt some already existing methods such as pump-probe spectroscopy which measures ultrafast electronic dynamics (less than a nanosecond), piezoelectric quartz sensors which gives density and mechanical modulus of the materials deposited on. Preliminary tests were run to investigate optical transmission resonance and are promising. A DMA machine (Dynamical Mechanical Analysis) was especially designed in the laboratory to study the behaviour of fibers and films. All these experimental setups allow to study photoinduced phenomena at various timescale and to better understand them

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FLE, Guillaume. "Extending the pump energy range for a pump-probe system using High Harmonics Generation." Thesis, Uppsala universitet, Molekyl- och kondenserade materiens fysik, 2015. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-266350.

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Dominguez, Pablo Nahuel. "Pump-probe measurements of reaction centers from Rhodobacter sphaeroides." Diss., Ludwig-Maximilians-Universität München, 2014. http://nbn-resolving.de/urn:nbn:de:bvb:19-185735.

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Walke, Daniel John. "New instrumentation and methods for ultrafast pump-probe spectroscopy." Thesis, Imperial College London, 2016. http://hdl.handle.net/10044/1/48040.

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Recent advances have led to the demonstration of trains of attosecond pulses and isolated attosecond pulses in the vacuum ultraviolet (VUV) and extreme ultraviolet (XUV) regions of the electromagnetic spectrum in a number of laboratories. This has raised the possibility of direct time resolved measurements of correlation driven electron dynamics within molecules, with a long term aim of unprecedented control over the dynamics of matter at atomic and molecular length scales. Particular interest has arisen towards the possibility of a charge migration mechanism within molecules, in which purely electron driven processes result in the movement of charge around an excited molecule in the absence of any nuclear dynamics. However, even once these sources have been established, using them in time resolved experiments is challenging. This is due to extremely short time-scales involved, the complexity of the processes under study, and the limitations of currently available attosecond sources. In this thesis I describe the development of novel instrumentation and methods for attosecond pump – probe experiments on electron dynamics in molecules. Strategies for the experimental study of charge migration are reviewed in detail which motivates the design and implementation of a purpose built instrument combining an electron velocity map imaging (VMI) spectrometer and an ion time of flight (iTOF) spectrometer. This instrument is designed in tandem with the development and characterisation of an isolated pulse at the new photon energy of 20eV. This 20eV pulse is intrinsically synchronized with another attosecond pulse at 90eV. Together, the new instrument and light source represent a unique capability for the investigation of electron dynamics in molecules. Finally, the first experimental results are presented and perspectives for future studies using the new developments are discussed.

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Henriksen, Lisa Grav. "Pump-probe experiments of multicrystalline silicon for solar cell applications." Thesis, Norges teknisk-naturvitenskapelige universitet, Institutt for fysikk, 2012. http://urn.kb.se/resolve?urn=urn:nbn:no:ntnu:diva-19207.

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In order to make cost effective solar cells from mc-Si materials, the negative contributions from defects and impurities should be reduced. The analysis of the photogenerated carrier properties is therefore of great importance for characterising carrier processes and hence, for improving the material performance.In this work, pump-probe measurement of a range of silicon wafers have been performed, using anultrafast laser of 800 nm wavelength and 85 fs pulses. The optical response in the samples were analysed by measuring the reflected probe beam initial transient.The purpose of this theses was to explore the use of pump-probe experiment to study carrier dynamics in mc-Si. Measurements of single c-Si samples were used as a basis for developing good experimental skills as well as achieving knowledge about carrier dynamics in c-Si. The initial Delta R/R was studied for a range of input parameters, aiming to characterise important contributions to the measurements.The effects of passivation has been studied, indicating a significant contribution to R~R. Etchingoff the passivated layer of an oxide (SiO2) wafer, showed a radically increased in pump beam reflectivity, from 9% to 32%, and a reduced DeltaR~R from 47×10-6 to 37×10-6 was be observed. Analysis has showed that incident angle may be chose such that the pump reflection loss is at a minimum for the given passivation thickness.The final results showed a R~R is in the range of (14-41)e-6 for bare c-Si, and (47-171)e-6 for passivated c-Si wafers.Ultrafast initial recovery has been observed for mc-Si samples, and attributed to trapping of carriers. Decay times in the range of 1-6 ps are deduced and trapping densities are found as (1:3 - 4:3) × 10^18 cm-3, which is in the same order as the excitation densities.A methodology for using pump-probe measurements to analyse mc-Si samples is established, and the technique is used in characterising the observed defect states, which is of great interest for improving solar cell materials.

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Ehrler, Oli T. "Ultraschnelle zeitaufgelöste Pump-Probe-Photoelektronenspektroskopie an isolierten und massenselektierten Anionen." Karlsruhe : Univ.-Verl. Karlsruhe, 2006. http://www.uvka.de/univerlag/volltexte/2006/181/.

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32

Wu, Jing. "Optical pump-probe studies of spin dynamics in ferromagnetic materials." Thesis, University of Exeter, 2001. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.364427.

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Matía, Hernando Paloma. "Attosecond pump-probe methods for measurement of molecular hole dynamics." Thesis, Imperial College London, 2017. http://hdl.handle.net/10044/1/50155.

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The generation of few-cycle pulses at near-infrared wavelengths is now a robust technology, as is their application to the efficient production of high-order harmonics in the extreme ultraviolet region with temporal confinement to hundreds of attoseconds. Recent years have seen considerable efforts directed to the study of electron dynamics in complex molecules in real time, with relevance to processes such as photosynthesis and radiation damage of proteins and DNA. This work describes the development of new and unique sources suited for the study of such dynamics, together with novel instrumentation and experimental methodology. This includes a pair of synchronised attosecond pulses at different photon energies in the VUV and XUV regions, which we have generated via high harmonic generation from a few-cycle NIR source and characterised with attosecond streaking. We have also explored the possibilities of sub-cycle control of these attosecond pulses by adding a second harmonic field to the high- harmonic generation process, and simultaneously characterised this second harmonic field with a novel characterisation technique known as ARIES, capable of waveform sampling at arbitrary optical wavelengths. In parallel, we have developed a few-cycle short-wavelength IR source for a UK user facility, to take advantage of the favourable wavelength scaling of the maximum photon energy achievable via high-harmonic generation. Using a commercial optical parametric amplifier and a hollow-core fibre compression system, we have generated sub-2-cycle pulses at 1750 nm, characterised via third-harmonic autocorrelation and a novel implementation of the dispersion scan technique. We have commissioned a beamline for attosecond pump-probe studies in the gas phase, including a purpose-built dual spectrometer with capabilities for simultaneous measurement of mass spectra of ions and velocity-map imaging of electrons. We have performed initial VUV-NIR pump-probe experiments on a small organic molecule, namely isopropanol, and identified a time- dependent signature as an IR-induced coupling. Finally, we have considered perspectives for future studies in attosecond pump-probe experiments with the demonstration of a two-VUV-photon process in helium performed with a moderate energy, high repetition rate attosecond source.

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Fabris, Davide. "Ultrafast light sources and methods for attosecond pump-probe experiments." Thesis, Imperial College London, 2015. http://hdl.handle.net/10044/1/25283.

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In this thesis I describe the development of novel light sources to be applied in attosecond pump-probe experiments, together with new methods dedicated to their characterisation and optimisation. Femtosecond pulses are a necessary tool to enter the attosecond domain. For this reason their development is a key element to unlock more capabilities in pump-probe attosecond experiments. The dynamics of generation and compression of few-cycle femtosecond pulses has been studied in a hollow core fibre system. The carrier envelope phase stability performance under increasing input power to the fibre system has been examined systematically, showing the effects of ionisation on the carrier envelope phase stability. Two characterisation techniques have been developed to measure ultrafast femtosecond pulses. A version of the d-scan technique has been demonstrated in the single shot regime for the first time, extending the utility of this diagnostic. An all optical technique (ARIES) for the characterisation of the full waveform of a femtosecond pulse has been developed, exploiting the high harmonics generation process and the sensitivity of the cut-off emission to the instantaneous amplitude of the generating electric field. The main results of the thesis are concerned with the generation of isolated attosecond pulses in new spectral regions. Vacuum ultraviolet few-femtosecond and attosecond pulses have been generated by filtering with metallic foils the high harmonics emission driven by sub-4 fs pulses, and were characterised with the attosecond streaking technique. When using indium as spectral filter a pulse duration of 1.7±0.1 fs was measured at a photon energy of 15 eV. When using tin as spectral filter a pulse duration of 585±31 as was measured at a photon energy of 20 eV. The experimental techniques developed in this thesis allow these pulses to be generated simultaneously with a XUV pulse with a measured duration of 270±25 as. This work will open new opportunities for pump-probe experiments, for example studies of ultrafast charge migration in large molecules.

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Ombinda-Lemboumba, Saturnin. "Femtosecond pump probe spectroscopy of light harvesting complexes and Phthalocyanines." Thesis, Stellenbosch : Stellenbosch University, 2011. http://hdl.handle.net/10019.1/17894.

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Thesis (PhD)--Stellenbosch University, 2011.
ENGLISH ABSTRACT: The generation of ultrafast light pulses and the development of time resolved spectroscopic techniques, such as the femtosecond pump probe spectroscopy technique, have facilitated the study of ultrafast energy transfer in the photosynthetic systems of green plants and photodynamic therapy drugs. It has allowed the investigation of biological and chemical processes that take place on the ultrafast timescale and has allowed us to obtain spectral and kinetic information on energy transfer. In addition, it has allowed time resolved experiments in which the transient absorption of species under investigation was observed and has elucidated molecular dynamics. In the present work this was done with a temporal resolution of approximately 200 fs and covering a pump-to-probe delay range of 300 fs to 2 ns. The main aims of this study were to characterise the femtosecond pump probe spectroscopy system, to investigate the energy transfer in the natural light harvesting complex II (LHC II) in view of future expansion to the study of synthesized arti cial functional light harvesting complexes and nally to study ultrafast processes in zinc phthalocyanine (ZnPc) systems. In photosynthetic organisms, LHC II is the most abundant light harvesting complex and it plays an important role in light harvesting and photoprotection. The light energy is absorbed by light harvesting complexes and transferred to a reaction centre (RC) in an ultrafast timescale. Phthalocyanines are a new class of photosensitiser used for photodynamic therapy. These drugs are used to treat small and super cial tumours. The energy transfer from the singlet excited state to the triplet excited state occurs on an ultrafast timescale. However, recent work done on zinc phthalocyanine has proved that the determination of the ultrafast component remains a challenge. Several ultrafast studies carried out on ZnPc in solvents have been not only unsuccessful to give a clear picture of the ultrafast dynamics but have also produced divergent results. In this study, a characterisation of the femtosecond pump probe spectroscopy setup was done. The samples under investigation were probed by a white light continuum. The generation of the white light continuum introduced chirp, which in uenced the temporal evolution of the transient absorption results. The technique used to correct the chirp introduced by white light generation is discussed in detail. Our femtosecond pump probe spectroscopy setup was benchmarked by using a well known dye, namely malachite green. In addition, the investigation of the transient absorption change of LHC II, an active component in photosynthesis, as extracted from spinach leaves and the ultrafast dynamics of a promising photosensitiser ZnPc in dimethyl sulfoxide (DMSO) as well as in dimethyl formamide (DMF) was done. The spectral and dynamic results obtained using these three samples are described and exponential ts to the absorbance decay curves used to estimate the timescales of the energy transfer processes are presented. In this experiment, the dynamics and measured time constants related to the energy transfer between the different types of chlorophyll in LHC II was monitored, whereas with ZnPc, the dynamics and the measured time constants associated with solvation dynamics and vibrational relaxation was examined.
AFRIKAANSE OPSOMMING: Die vorming van ultravinnige lig pulse en die ontwikkeling van tyd opgelosde spektroskopiese tegnieke, soos die femtosekonde pomp proef spektroskopie tegniek, het die studie van ultravinnige energie oordrag in fotosintetiese stelsels van groen plante en chemiese prosesse gefasiliteer, wat kan plaasvind op die ultravinnige tyd skaal en laat dit toe om spektrale en kinetiese informasie oor die energie oordrag te kan bepaal. Dit het ook dit moontlik gemaak om tyd opgelosde eksperimente te kan doen waarin ons veranderlike absorbsie van die monster kon ondersoek en die molekulere dinamika kon ontrafel. In hierdie werk is dit gedoen met n tyd resolusie van omtrent 200 fs termyl 'n pomp-tot-proef tydvertraging van 300 fs tot 2 ns gebruik is. Die hoof doelwitte van hierdie werk was om 'n femtosekonde pomp proef spektroskopie stelsel te karakteriseer, die energie oordrag in die natuurlike ligoes kompleks II te ondersoek met die toekomstige uitbreiding van die studie na sintetiese lig-oes komplekse as oogmerk en laastens om ultravinnige prosesse in Sink Ftalosianiene stelsels te ondersoek. In fotosintetiese organismes, is lig oes kompleks II die mees volop lig oes kompleks en speel 'n belangrike rol in lig oes en foto skerming. Die lig energie word geabsorbeer deur lig oes komplekse en dan oorgedra na reaksie middelpunte in 'n ultravinnige tydskaal. Ftalosianiene is 'n nuwe klas fotosensiteerder wat gebruik word in fotodinamiese terapie. Hierdie dwelms word gebruik om klein en oppervlakkige gewasse te behandel. Die energie oordrag van die opgewekte singlet tot die triplet toestand vind plaas op die ultravinnige tydskaal. Onlangse navorsingswerke het getoon dat die bepaling van die ultravinnige komponent 'n uitdaging bly. Verskeie vorige ondersoeke is gedoen op Sink Ftalosianiene in verskeie oplosmiddels, en nie net het hierdie studies nie 'n helder prentjie verskaf van die ultravinnige dinamika nie, maar het ook divergerende resultate opgelewer. In hierdie werk word 'n karakterisering van die femtosekonde pomp proef spektroskopie stelsel gedoen. Die monsters is ondersoek met 'n wit lig kontinuum proef. Die vorming van die wit lig kontinuum het tjirp veroorsaak, wat die tyd evolusie van die veranderlike absorbsie resultate beinvloed het. Die tegniek wat gebruik was om die tjirp te korregeer word bespreek. Ons femtosekonde pomp proef spektroskopie stelsel is gestandardiseer deur die welbekende kleurstof malachiet groen. Ons het ook die veranderlike absorbsie van lig oes kompleks II ondersoek, 'n aktiewe komponent in fotosintese, soos dit onttrek is uit spinasie blare, asook die ultravinnige dinamika van die belowende photosensitizer Sink Ftalosianiene in DMSO asook DMF. Die spektrale en dinamiese resultate verkry vanaf hierdie drie monsters word beskryf en eksponensiele passings aan die absorbsie verval kurwes is gebruik om die tydskale van die energie oordrag prosesse te skat. In hierdie eksperiment is dinamika en gemete tydkonstantes waargeneem wat toegeskryf kan word aan die energie oordrag tussen verskillende soorte chloro l in lig oes kompleks II. In die Sink Ftalosianien eksperimente is dinamika en gemete tydkonstantes waargeneem wat toegeskryf kan word aan solverings dinamika asook vibrasionele ontspanning.

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Cheng, Yu-Hsiang. "Photoinduced dynamics studied by ultrafast single-shot pump-probe spectroscopy." Thesis, Massachusetts Institute of Technology, 2019. https://hdl.handle.net/1721.1/122684.

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This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
Thesis: Ph. D., Massachusetts Institute of Technology, Department of Electrical Engineering and Computer Science, 2019
Cataloged from student-submitted PDF version of thesis.
Includes bibliographical references (pages 155-168).
This thesis focuses on the development of dual-echelon single-shot spectroscopy and its applications to study irreversible photoinduced dynamics. First, the ultrafast laser sources and the related control and characterization techniques are discussed. In particular, we have invented a two-stage dual-beam noncollinear optical parametric amplifier to provide tunable sources for pump-probe spectroscopy. Next, the experimental setup of dual-echelon single-shot spectroscopy is illustrated with great detail and possible noise sources and correction methods are explored. Using the single- shot technique, we studied photoinduced dynamics in three different materials. In bismuth, we found a transition into a transient symmetric phase at high fluences. We showed the coherent control of phonon parameters with pump-pump-probe experiments. We also simulated the carrier and phonon dynamics using a modified two-temperature model. In tellurium, we demonstrated that the amorphization of crystalline tellurium induced by femtosecond pulses is a thermal process. We also estimated the lattice temperature by the change in phonon frequency. In a strained manganite film, we observed a photoinduced persistent insulator-to-metal transition and showed the partial recovery of the generated metallic phase to the insulating phase.
by Yu-Hsiang Cheng.
Ph. D.
Ph.D. Massachusetts Institute of Technology, Department of Electrical Engineering and Computer Science

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Harper, Matthew R. "Control and measurement of ultrafast pulses for pump/probe-based metrology." Thesis, St Andrews, 2007. http://hdl.handle.net/10023/430.

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38

Issenmann, Daniel [Verfasser]. "Studium der Phononendynamik mit Pump-Probe-Experimenten im Röntgenbereich / Daniel Issenmann." Konstanz : Bibliothek der Universität Konstanz, 2014. http://d-nb.info/1050348818/34.

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Chung, Dutch D. 1969. "Femtosecond pump-probe spectroscopy of chemical reactions in liquids and crystals." Thesis, Massachusetts Institute of Technology, 1998. http://hdl.handle.net/1721.1/10022.

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40

Bacon, David Robert. "Time-resolved pump-probe investigation of the terahertz quantum cascade laser." Thesis, University of Leeds, 2017. http://etheses.whiterose.ac.uk/17968/.

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The terahertz (THz) region of the electromagnetic spectrum remains relatively underdeveloped and unexploited. This is due to the lack of compact and high-power sources which are able to output radiation between 100 GHz and 10 THz. In this thesis two separate methods of generating THz radiation are considered; the quantum cascade laser (QCL) and the photoconductive (PC) emitter. THz-QCLs generate radiation through the intersubband transition of electrons within quantum wells. Electrons are then transported into the adjacent quantum well, where they are recycled. Alternatively, PC emitters generate THz radiation through the excitation, acceleration and recombination of electron-hole pairs in semiconducting material, leading to the emission of short pulse THz radiation. In this work, the gain dynamics of two different designs of THz-QCL are investigated using well-established time domain spectroscopy (TDS) techniques. The gain recovery time of a bound-to-continuum (BTC) device, a property known to be responsible for the prevention of mode-locking in the laser, is recovered through use of THz-pump-THz-probe TDS. This was performed multiple times, both with and without anti-reflective coating applied to the QCL facets. This coating prevents the QCL from lasing. Furthermore, this approach was then used to investigate the carrier dynamics of a hybrid active region device, which yielded some interesting preliminary results. To facilitate these measurements, a new form of quartz-mounted PC device was designed and fabricated. This entails removing the LT-GaAs active layer from its SI-GaAs growth substrate and bonding it directly to a layer of z-cut quartz. In emission, this device has been shown to produce significantly higher THz output fields, when compared to the previously used PC devices. In addition to this, the use of an optically transparent substrate provides the ability to perform back-side illumination, which is shown to improve the output characteristics of the device. Furthermore, when used in detection, the newly fabricated devices have shown significantly increased sensitivity, when compared to other methods of detection.

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Kim, Yang-Hyo. "Wide-field structured illumination microscopy for fluorescence and pump-probe imaging." Thesis, Massachusetts Institute of Technology, 2018. https://hdl.handle.net/1721.1/121846.

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Thesis: Ph. D., Massachusetts Institute of Technology, Department of Mechanical Engineering, 2019
Cataloged from PDF version of thesis.
Includes bibliographical references.
The optical resolution of microscopy is limited by the wave-like characteristic of the light. There are many recent advances in overcoming this diffraction limited resolution, but mostly focused on fluorescent imaging. Furthermore, there are few non-fluorescence wide-field super-resolution techniques that can fully utilize the applicable laser power to optimize imaging speed. Structured illumination microscopy is a super-resolution method that relies on patterned excitation. This thesis has presented novel applications of structured illumination microscopy to surface plasmon resonance fluorescence and pump-probe scattering imaging. First, structured illumination microscopy was introduced to surface plasmon resonance fluorescence imaging for high signal-to-noise and high resolution. Secondly, a theoretical framework for three-dimensional wide-field pump-probe structured illumination microscopy has been developed to increase the lateral resolution and enable depth sectioning. Further, structured illumination wide-field photothermal digital phase microscopy is proposed as a high throughput, high sensitivity super-resolution imaging tool to diagnose ovarian cancer. Finally, I have derived the exact analytical solution to the heat conduction problem in which a sphere absorbs temporally modulated laser beam for photothermal microscopy. The proposed method also has a great potential to be applied to other pump-probe modalities such as transient absorption and stimulated Raman scattering.
Funding sources and sponsors: National Institutes of Health (9P41EB015871-26A1, 5R01NS051320, 4R44EB012415, and 1R01HL121386-OlAl), National Science Foundation (CBET-09395 11), Hamamatsu Corporation, Singapore-Massachusetts Institute of Technology Alliance for Research and Technology (SMART) Center, BioSystems and Micromechanics (BioSyM), and Samsung Scholarship
by Yang-Hyo Kim.
Ph. D.
Ph.D. Massachusetts Institute of Technology, Department of Mechanical Engineering

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42

Pincelli, T. "PROBING ELECTRON CORRELATION DYNAMICS: A MULTI-TECHNIQUE STUDY APPLIED TO THE HALF-METALLIC OXIDE LA1-XSRXMNO3." Doctoral thesis, Università degli Studi di Milano, 2017. http://hdl.handle.net/2434/543731.

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This thesis completes my work as doctoral student of the Scuola di Dottorato in Fisica, Astrofisica e Fisica Applicata at the Università degli Studi di Milano that has been carried out, starting in November 2014, mostly at the Laboratorio TASC of IOM-CNR in the premises of the Elettra - Sincrotrone Trieste and FERMI@Elettra infrastructures, in the framework of the NFFA and APE-beamline facilites, as well as by accessing international large scale infrastructures and laboratories. The activity has addressed the development of experimental methodologies and novel instrumentation oriented to the study of the dynamical properties of highly correlated materials after high energy excitation. The science programme has been carried out by exploiting ultrafast femtosecond probes from the optical regime (Ti-Sa lasers, fibre laser oscillators) to the extreme UV-soft X rays at FERMI, to the picosecond hard X-rays from the SPring-8 and Diamond synchrotron radiation source. The sample synthesis of correlated oxides and its characterization has been performed within the NFFA facility and APE-group collaboration in Trieste as well as the design and construction of the all new laser High Harmonic Generation beam line NFFA-SPRINT and its end station for time resolved vectorial electron spin polarimetry. This report concentrates on the main scientific concern of my work that has been the relaxation of external perturbations in a correlated electron material both in the time and space domain. I have employed Photoelectron Spectroscopy (PES) mostly in the Hard X-ray regime (HAXPES), pushing the boundaries of its application to achieve a coherent perspective. The material I have mainly focused on is La0.67Sr0.33MnO3 (LSMO), of high interest for spintronics. This system is prototypical, yielding the highest simplicity in the class of transition metal oxides. In the spatial investigation, I have controlled with high precision the PES probing depth and I have observed the evolution of one spectral feature. I have identified it as probe of electronic hybridization and long-range ordering. I have studied LSMO films of 40 nm in three substrate-induced strain states (1% tensile in-plane, relaxed, 1% compressive in-plane) and a 18 nm film of (Ga,Mn)As (GMA), a well-studied diluted magnetic semiconductor. I have found that the electronic properties to be modified at significant distances from the surface, 4 nm for LSMO and 1.2 nm for GMA, while strain had no detectable effects. In the temporal study, I have employed HAXPES in pump-probe mode (TR-HAXPES) to observe the evolution of the electronic structure after intense optical excitation. A detailed dynamical characterization with optical techniques has allowed me to identify the characteristic time of the collapse of long-range magnetic order to be significantly longer than the one of elemental transition metals. I have ascribed this effect to the half-metallic character of LSMO. With TR-HAXPES I have observed that the whole electronic band-structure evolution is bottlenecked by the slow response of the magnetization, proceeding on hundreds of picoseconds timescales. Finally, I have described the techniques and the instrumentation that can be used to push these investigations to shorter spatial and temporal scales. This has been realized in the form of the NFFA-SPRINT laboratory, a facility open to users, which I participated in designing and developing.

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Flögel, Martin [Verfasser]. "Raising the XUV Intensity towards Attosecond-Attosecond Pump-Probe Experiments / Martin Flögel." Berlin : Freie Universität Berlin, 2017. http://d-nb.info/1133492347/34.

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Souther, Nathan Jon. "Light Shift Measurements of Cold Rubidium Atoms using Raman Pump-Probe Spectroscopy." Miami University / OhioLINK, 2009. http://rave.ohiolink.edu/etdc/view?acc_num=miami1250622906.

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Stangoni, Maria Virginia. "Scanning probe techniques for dopant profile characterization /." [S.l.] : [s.n.], 2005. http://e-collection.ethbib.ethz.ch/show?type=diss&nr=16024.

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Taylor, Christopher George. "Novel fluorescence techniques to probe protein aggregation." Thesis, University of Cambridge, 2018. https://www.repository.cam.ac.uk/handle/1810/276197.

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The self-assembly of amyloidogenic proteins to form cytotoxic species that give rise to brain deterioration underlies numerous neurodegenerative disorders such as Alzheimer’s and Parkinson’s diseases. Increasing evidence indicates that it is the rare, low-molecular-weight species (oligomers) rather than the more abundant high-molecular-weight fibrils of certain proteins that are the most cytotoxic in several neurodegenerative diseases. However, these species have proven difficult to study using traditional methods due to their transient nature and the heterogeneity of aggregation mixtures. In this thesis, I describe my work to develop advanced methods where I combine single-molecule and ensemble fluorescence techniques with microfluidic strategies to enable the study of protein aggregation, spanning small, transient oligomers to large, insoluble aggregates. In Chapter 1 I give an overview of the biological context and relevance of this work, including the background of neurodegenerative disease, amyloidogenic aggregation and key proteins involved. I then briefly review fluorescence microscopy techniques and the field of microfluidics. In Chapter 2 I describe how complex microfluidics can be integrated with single-molecule confocal techniques to provide a highly sensitive method to continuously probe protein aggregation in vitro. I show, for the first time, that the dilution of aggregating mixtures may be automated, by up to five orders of magnitude, down to the picomolar concentrations suitable for single-molecule measurements. By incorporating this microfluidic dilution device I greatly improve the temporal resolution of the technique and facilitate the observation of more transient species through the ability to rapidly dilute and take fluorescence measurements of samples. In Chapter 3 I overcome the need for in situ labels to monitor amyloidogenic aggregation using single-molecule confocal microscopy. I describe my work to adapt the single-molecule confocal technique to achieve the ultrasensitive detection of individual aggregate species under flow without covalently-attached labels. I have demonstrated the ability of this new method to monitor the aggregation of label-free amyloidogenic proteins using extrinsic labels ex-aggregation, opening the way for biological samples to be probed in a high-throughput manner. In Chapter 4 I describe my work to combine the high precision of confocal microscopy with a microfluidic device developed to directly characterise the sizes and interactions of biomolecules in the continuous phase. By monitoring the spatial and temporal mass transport on the micron scale, the diffusion coefficient, and thus hydrodynamic radius, of species may be determined. The technique delivers much greater sensitivity for size quantification, allowing scarce and other challenging samples to be characterised, and provides significant steps towards accurate sizing for single-molecule aggregation experiments under flow. In Chapter 5 I describe my work to determine the microscopic driving force for the spatial propagation of amyloid-beta. The epifluorescence instrument I built has enabled the proliferation of aggregate species to be monitored over a macro distance on a timescale of minutes. This has greatly improved the scope of the experimental data attained, which will be used in conjunction with Monte Carlo simulations to deliver a model for the propagation of amyloid-beta in vitro. Together this thesis represents my work developing the above novel fluorescence techniques to improve their temporal and size resolution, sensitivity and adaptability to study highly complex and fundamental protein aggregation linked to neurodegenerative disease.

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Attwood, Simon. "Nanoscale chemical specification using scanning probe techniques." Thesis, University of Cambridge, 2010. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.608912.

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Bene, J. G. (József Gergely). "Pump schedule optimisation techniques for water distribution systems." Doctoral thesis, Oulun yliopisto, 2013. http://urn.fi/urn:isbn:9789526202662.

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Abstract This thesis deals with the pump schedule optimisation of regional water distribution systems. The aims and the possible applications of the presented methods differ from each other; all of them are intended to solve a particular but realistic problem. The developed techniques use the capacity of the water reservoirs in order to find the optimal pump-schedule of the system. The optimisation task is always deterministic and discrete in time; the stochastic behaviour of the water consumptions is approximated by expected values. A so-called neutral genetic algorithm equipped with new constraint handling is presented first. The method is able to solve the scheduling problems of real-size and complex networks, e.g. the network of Budapest with coupled hydraulic simulations where both variable and fixed speed pumps are in the network. The results are compared to other ones obtained by widely used genetic algorithms and state-of-the-art general purpose optimisation solvers. A dynamic programming based method was also carried out which provides the global optimum of the so-called ’combinatorial’ pump scheduling problems. This modelling type is very common in the industry, which can be used if the operation points of the pumps take discrete values. The basic idea of the method is exploiting the ’permutational invariance’ of the model which results in a perfect discretisation of the state space without any loss of information. An approximate dynamic programming technique is also presented which solves the same type of problems as the formerly mentioned genetic algorithm does. The technique splits the water network model into smaller units, namely into the so-called well fields and the main distribution system. The state space of the main distribution system was further decreased while the quality of the results does not decay. A part of the test examples is the same as in the case of the former presented genetic algorithm; thus, the two methods can be compared. Finally, a small water network fed by a single variable speed pump was investigated. The presented methods are based on the minimisation of the specific energy consumption. The gained results are compared to ones obtained using a high-resolution discrete dynamic program. Novel optimisation techniques for water distribution network pump scheduling were developed in this work. A particular focus was put on the dynamics between pumping, water reservoirs, and water use. The work shows the applicability of the approach via numerous realistic simulation case studies
Tiivistelmä Työ käsittelee alueellisten vedenjakelujärjestelmien pumppauksen aikataulutuksen optimointia. Esitettyjen menetelmien tavoitteet ja mahdolliset sovellukset poikkeavat toisistaan. Kaikki on kuitenkin tarkoitettu tiettyjen todellisten ongelmien ratkaisemiseen. Kehitetyt tekniikat käyttävät vesivarastojen kapasiteettia optimaalisen pumppausohjelman löytämiseksi. Jokainen optimointitehtävä on aikadiskreetti ja deterministinen, vedenkulutuksen stokastista käyttäytymistä on approksimoitu odotusarvoilla. Ensimmäiseksi työssä esitetään ns. neutraaleja geneettisiä algoritmeja varustettuna rajoitusten käsittelyllä. Menetelmällä voidaan ratkaista skedulointiohjelmia reaalimittakaavaisille ja monimutkaisille verkostoille (esim. Budapestin verkosto varustettuna hydraulisilla simuloinneilla, sekä muuttuvanopeuksisilla että vakionopeuksisilla verkoston pumpuilla). Tuloksia verrataan toisiin yleisesti käytössä olevilla geneettisillä algoritmeilla saatuihin, sekä johtavilla yleiskäyttöisillä optimointitekniikoilla saatuihin tuloksiin. Työssä käytettiin myös dynaamiseen ohjelmointiin pohjaavaa menetelmää, jolla saadaan globaali optimi ns. "kombinatoorisille" pumppauksen aikataulutusongelmille. Tällainen mallinnustapa on hyvin yleistä teollisuudessa. Sitä voidaan käyttää, jos pumppujen toimintapisteet saavat diskreettejä arvoja. Menetelmän perusajatuksena on "permutationaalisen invarianssin" hyväksikäyttäminen, josta seuraa tila-avaruuden virheetön diskretointi ilman informaation häviämistä. Työssä esitellään myös approksimoidun dynaamisen ohjelmoinnin tekniikka, jonka avulla voidaan ratkaista samantyyppisiä ongelmia kuin yllämainituilla geneettisillä algoritmeilla. Tämä tekniikka jakaa vesijohtoverkoston mallin pienempiin yksiköihin: lähdekenttiin ja pääjakeluverkostoon. Pääjakeluverkoston tila-avaruutta voitiin edelleen pienentää ilman, että tulosten laatu heikkeni. Osa käsitellyistä esimerkkitapauksista on samoja kuin edellämainittujen geneettisten algoritmien osalla, joten tuloksia voidaan verrata. Lopuksi tutkittiin pienen muuttuvanopeuksisella pumpulla syötetyn vesijohtoverkoston toimintaa. Esitetyt menetelmät perustuvat ominaisenergiankulutuksen minimointiin. Saatuja tuloksia verrataan korkearesoluutioisella diskreetillä dynaamisella ohjelmoinnilla saatuihin tuloksiin. Työssä kehitettiin uusia optimointitekniikoita vedenjakelujärjestelmien pumppauksen aikataulutuksen optimintiin. Erityisesti työssä keskityttiin pumppauksen, vesitornien ja kuluttajien käyttäytymisen väliseen dynamiikkaan. Työssä osoitettiin tekniikoiden toimivuus realististen esimerkkisimulointien avulla
Kivonat Jelen doktori disszertáció regionális ivóvízellátó-hálózatok üzemvitel-optimalizációjával foglalkozik. A bemutatott módszerek alkalmazhatósági köre rendszerint eltér egymástól, mindegyik egy-egy speciális, de a való életben is előforduló problémára kíván megoldást nyújtani. A kidolgozott módszerek a medencék tárolókapacitását kihasználva, az optimális szivattyú-menetrendet keresve kívánják megtalálni az adott vízműhálózat üzemviteloptimumát. Az optimalizáció egy időben diszkrét, ugyanakkor determinisztikus feladat megoldását igényli, a vízfogyasztások sztochasztikus viselkedését a várható értékekkel közelítettem. Elsőként egy új mellékfeltétel-kezeléssel ellátott, ún. neutrális genetikus algoritmus bemutatása a cél. A kidolgozott módszer alkalmas nagy, valós méretű (pl. Budapest) és bonyolultságú (kapcsolt hidraulikai szimulációk, frekvenciaváltós és direkt szivattyúk a hálózatban) ivóvízhálózatok napi üzemvitel optimalizálására. Az eredményeket más genetikus algoritmusokkal és a világ élvonalába tartozó, de általános célú optimalizációs módszerekkel hasonlítottam össze. Kidolgozásra került egy dinamikus programozás alapú, a valós, globális optimumot adó módszer is. Az algoritmus a gyakorlatban elterjedt, ún. "kombinációs" hálózatként modellezhető vízműhálózat típusokra alkalmazható, ahol a szivattyúk munkapontjai diszkrét értékek. A megoldás alapját az ún. "permutációs invariancia" jelensége adja, mely lehetővé teszi az állapottér információveszteség nélküli, tökéletes diszkretizációját. Egy, a korábban bemutatott genetikus algoritmuséhoz hasonló problémakört megoldó, de közelítő dinamikus programozás alapú módszer is bemutatásra kerül. Az algoritmus a hálózat kisebb részegységekre (víztermelő területekre és fő elosztó hálózatra) való felbontásával és a fő elosztó hálózat állapotterének önkényes, de a megoldás jóságán jelentősen nem rontó csökkentésével éri el a program futtatásához szükséges számítási igény csökkentését. A tesztfeladatok egy része megegyezik a genetikus algoritmus tesztfeladataival, így azok közvetlenül összehasonlíthatóak. Végül bemutatásra kerül egy kisméretű, mindössze egy darab változtatható fordulat- számú szivattyúval táplált rendszer energetikai vizsgálata. Az itt bemutatott módszerek mind a fajlagos energiafelhasználás minimalizálásán alapulnak. Az eredményeket egy nagyfelbontású dinamikus programozás alapú módszerhez hasonlítottam

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49

Cavanagh, Molly Christine. "Using the ultrafast pump-probe spectroscopy of atomic anions and the solvated electron to probe solvent structure and solvation dynamics." Diss., Restricted to subscribing institutions, 2008. http://proquest.umi.com/pqdweb?did=1581642021&sid=1&Fmt=2&clientId=1564&RQT=309&VName=PQD.

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50

Kruglyak, Volodymyr. "Femtosecond optical pump-probe investigations of ultrafast electron and spin dynamics in metals." Thesis, University of Exeter, 2004. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.410811.

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Dissertations / Theses on the topic 'Pump and probe techniques'

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