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1
Polyutov, Sergey. "Electron-nuclear Dynamics in Nonlinear Optics and X-ray spectroscopy." Doctoral thesis, Stockholm : Bioteknologi, Kungliga Tekniska högskolan, 2007. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-4339.
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Liu, Ji-Cai. "Dynamics of multiphoton processes in nonlinear optics and x-ray spectroscopy." Doctoral thesis, KTH, Teoretisk kemi, 2009. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-11394.
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New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of microsecond pulses is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties. The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation. We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation.QC 20100729
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Lim, Daeyoung. "Nonlinear optical spectroscopy of silicon-boron and other silicon-adsorbate systems." Access restricted to users with UT Austin EID Full text (PDF) from UMI/Dissertation Abstracts International, 2001. http://wwwlib.umi.com/cr/utexas/fullcit?p3034931.
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McGuckin, Brendan T. "Linear and nonlinear optical spectroscopy of semiconductors using opticallypumped lasers." Thesis, Heriot-Watt University, 1985. http://hdl.handle.net/10399/1655.
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Barlow, Aaron M. "Spectral Distortions & Enhancements In Coherent Anti-Stokes Raman Scattering Hyperspectroscopy." Thesis, Université d'Ottawa / University of Ottawa, 2015. http://hdl.handle.net/10393/32388.
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Coherent anti-Stokes Raman scattering microscopy is a versatile technique for label-free imaging and spectroscopy of systems of biophysical interest. Due to the coherent nature of the generated signals, CARS images and spectra can often be difficult to interpret. In this thesis, we document how distortions and enhancements can be produced in CARS hyperspectroscopy as a result of the instrument, geometrical optical effects, or unique molecular states, and discuss how these effects may be suppressed or exploited in various CARS applications.
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Valley, John Francis. "Nonlinear optical experiments in sodium vapor and comparison with Doppler-broadened two-level-atom theory." Diss., The University of Arizona, 1989. http://hdl.handle.net/10150/184930.
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Two spectral regions of gain exist for a weak probe beam propagating through a medium of two-level-atoms pumped by a strong near-resonance field. Experimentally a cw ring-dye laser is used to explore this gain at the Na D₂ resonance in a vapor. Plane-wave calculations of probe-gain spectra which include the Doppler broadening inherent in a vapor agree well with experimental spectra obtained with a Fabry-Perot interferometer. Such two-beam-coupling gain might have applications as optical pre- or power amplifiers. The gain is also the primary step in four-wave-mixing. Mixing of the pump and sideband which experiences gain produces the medium polarization from which the fourth-wave arises. For phase-matched propagation the fourth-wave, which is at a frequency that experiences little or negative probe-gain (i.e., absorption), grows at nearly the same rate as the primary sideband. Together the two sidebands extract far more than twice as much energy from the pump than does the primary sideband acting alone. Experimentally four-wave-mixing which arises from noise at the gain-sideband-frequency is sometimes accompanied by conical emission at the fourth-wave sideband. Since this sideband is also seen on axis the explanation cannot be simply phase-matching. Simulations which include the full transverse nature of the experiment are currently running on a CRAY supercomputer. These simulations indicate that the radial variation of the medium index of refraction is responsible for conical emission.
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Грідякіна, Олександра Валеріївна, and Аркадій Петрович Поліщук. "Nonlinear-optical recording in ionic liquid crystalline medium." Thesis, Physikzentrum in Bad Honnef, 2017. http://er.nau.edu.ua/handle/NAU/32390.
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Odhner, Johanan. "INVESTIGATIONS OF TEMPORAL RESHAPING DURING FILAMENTARY PROPAGATION WITH APPLICATION TO IMPULSIVE RAMAN SPECTROSCOPY." Diss., Temple University Libraries, 2012. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/196129.
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ChemistryPh.D.
Femtosecond laser filamentation in gaseous media is a new source of broadband, ultrashort radiation that has the potential for application to many fields of research. In this dissertation filamentation is studied with a view to understanding the underlying physics governing the formation and propagation dynamics of filamentation, as well as to developing a method for vibrational spectroscopy based on the filament-induced impulsive vibrational excitation of molecules in the filamentation region. In pursuit of a better understanding of the underlying physical processes driving filamentation, the development of a new method for characterizing high intensity ultrashort laser pulses is presented, wherein two laser beams generate a transient grating in a noble gas, causing the pulse undergoing filamentation to diffract from the grating. Measuring the spectrum as a function of time delay between the filament and probe beams generates a spectrogram that can be inverted to recover the spectral and temporal phase and amplitude of the filamentary pulse. This technique enables measurement of the filamentary pulse in its native environment, offering a window into the pulse dynamics as a function of propagation distance. The intrinsic pulse shortening observed during filamentation leads to the impulsive excitation of molecular vibrations, which can be used to understand the dynamics of filamentation as well. Combined measurements of the longitudinally-resolved filament Raman spectrum, power spectrum, and fluorescence intensity confirm the propagation dynamics inferred from pulse measurements and show that filamentation provides a viable route to impulsive vibrational spectroscopy at remote distances from the laser source. The technique is applied to thermometry in air and in flames, and an analytical expression is derived to describe the short-time dynamics of the rovibrational wave-packet dispersion experienced by diatomic molecules in the wave of the filament. It is found that no energy is initially partitioned into the distribution of rovibrational states during the filamentation process. Filament-assisted impulsive stimulated Raman spectroscopy of more complex systems is also performed, showing that filament-assisted vibrational measurements can be used as an analytical tool for gas phase measurements and has potential for use as a method for standoff detection. Finally, a study of the nonlinear optical mechanisms driving the filamentation process is conducted using spectrally-resolved pump-probe measurements of the transient birefringence of air. Comparison to two proposed theories shows that a newly described effect, ionization grating-induced birefringence, is largely responsible for saturation and sign inversion of the birefringence at 400 nm and 800 nm, while the magnitude of contributions described by a competing theory that relies on negative terms in the power series expansion of the bound electron response remain undetermined.
Temple University--Theses
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Hu, Zhen Kimble H. Jeff Kimble H. Jeff. "Quantum optics with cold atoms--nonlinear spectroscopy and road toward single-atom trap /." Diss., Pasadena, Calif. : California Institute of Technology, 1995. http://resolver.caltech.edu/CaltechETD:etd-10112007-092812.
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Govani, Jayesh R. "Spectroscopic characterizations of organic/inorganic nanocomposites." To access this resource online via ProQuest Dissertations and Theses @ UTEP, 2009. http://0-proquest.umi.com.lib.utep.edu/login?COPT=REJTPTU0YmImSU5UPTAmVkVSPTI=&clientId=2515.
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Robertson, John Michael. "Nonlinear optical properties of absorbing molecular systems." Thesis, University of Essex, 2002. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.390961.
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Бордюг, Ганна Борисівна, and Аркадій Петрович Поліщук. "Fast photoconversion in viologen-doped lyotropic ionic liquid crystals." Thesis, Physikzentrum in Bad Honnef, 2017. http://er.nau.edu.ua/handle/NAU/32391.
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Peter, F. "Advanced emitters and detectors for terahertz time-domain spectroscopy." Forschungszentrum Dresden, 2010. http://nbn-resolving.de/urn:nbn:de:bsz:d120-qucosa-61479.
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The idea of terahertz-time-domain spectroscopy (THz-TDS) is to exploit a single cycle, spectrally broad THz radiation pulse to gain insight into the response of matter. Photoconductive devices and nonlinear crystals are utilized in both the generation as well as the coherent detection of THz radiation. The relatively high cost and the complexity of commonly used titanium-sapphire lasers hinder a more widespread use of pulsed THz systems for commercial applications. Er-doped femtosecond fiber lasers operating at 1.55 μm could offer a viable alternative. In this thesis nonlinear crystals and photoconductive emitters are discussed for excitation in the near infrared (NIR) window of between 800 nm to 1550 nm. The main focus of this thesis is a detailed study of substrate materials for an interdigitated photoconductive antenna. Photoconductive antennas with microstructured electrodes provide high electric acceleration fields at moderate voltages because of small electrode separations. The scalability of these devices allows for large active areas in the mm^2 range, which are sufficient for excitation at large optical powers. In comparison with conventional emitter structures, these antennas have more favourable characteristics regarding THz power, spectral properties, and ease of handling. Depending on the utilized substrate material, photoconductive antennas can then be operated using different excitation wavelengths. By employing substrates with short carrier trapping times these antennas can be operated as THz-detectors. Moreover the design of electrode structures for generating radially and azimuthally polarized THz waves are presented. A second topic deals with the signal analysis and signal interpretation of THz pulses transmitted through several material systems. These experiments show the potential for tomographic and spectroscopic applications. The third part deals with THz emission by frequency mixing in nonlinear organic and inorganic crystals. Hereby the focus is on polaritonic phase matching in GaAs. Furthermore, indications of THz tunability by the excitation wavelength were found by utilizing waveguide structures. However, the observed tuning range is much lower then theoretically predicted. Specific reasons for this are discussed.
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Грідякіна, Олександра Валеріївна, and Ганна Борисівна Бордюг. "Nonlinear helical winding in highly viscous chiral thin films." Thesis, NANO-2017, 2017. http://er.nau.edu.ua/handle/NAU/32389.
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Kimberg, Victor. "Pulse Propagation in Nonlinear Media and Photonic Crystals." Doctoral thesis, Stockholm, 2006. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-3886.
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Fu, Jie. "Molecular Structure-Nonlinear Optical Property Relationships for a Series of Polymethine and Squaraine Molecules." Doctoral diss., University of Central Florida, 2006. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/3941.
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This dissertation reports on the investigation of the relationships between molecular structure and two-photon absorption (2PA) properties for a series of polymethine and squaraine molecules. Current and emerging applications exploiting the quadratic dependence upon laser intensity, such as two-photon fluorescence imaging, three-dimensional microfabrication, optical data storage and optical limiting, have motivated researchers to find novel materials exhibiting strong 2PA. Organic materials are promising candidates because their linear and nonlinear optical properties can be optimized for applications by changing their structures through molecular engineering. Polymethine and squaraine dyes are particularly interesting because they are fluorescent and showing large 2PA. We used three independent nonlinear spectroscopic techniques (Z-scan, two-photon fluorescence and white-light continuum pump-probe spectroscopy) to obtain the 2PA spectra revealing 2PA bands, and we confirm the experimental data by comparing the results from the different methods mentioned. By systematically altering the structure of polyemthines and squaraines, we studied the effects of molecular symmetry, strength of donor terminal groups, conjugation length of the chromophore chain, polarity of solvents, and the effects of placing bridge molecules inside the chromophore chain on the 2PA properties. We also compared polymethine, squaraine, croconium and tetraon dyes with the same terminal groups to study the effects of the different additions inserted within the chromophore chain on their optical properties. Near IR absorbing squaraine dyes were experimentally observed to show extremely large 2PA cross sections ([approximately equal to] 30000GM). A simplified three-level model was used to fit the measured 2PA spectra and detailed quantum chemical calculations revealed the reasons for the squaraine to exhibit strong 2PA. In addition, two-photon excitation fluorescence anisotropy spectra were measured through multiple 2PA transitions. A theoretical model based on four-levels with two intermediate states was derived and used for analysis of the experimental data.Ph.D.
Other
Optics and Photonics
Optics
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Averett, Shawn C. "Advancements in the Understanding of Nonlinear Optics and Their Use in Material Analysis." BYU ScholarsArchive, 2017. https://scholarsarchive.byu.edu/etd/6507.
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Adhesion, heterogeneous catalysis, electrochemistry, and many other important processes and properties are driven by interactions at surfaces and interfaces. Vibrational sum frequency generation spectroscopy (VSFG) is an increasingly popular analytical technique because it can provide information about the nature and physical orientation of functional groups at these surfaces and interfaces. Analysis of VSFG data can be complicated by the presence of SFG signal that is not associated with a resonant vibration. This nonresonant sum frequency generation (NR-SFG) signal can interfere with the resonant signal and influence the detected spectrum. Methods have been developed to remove NR-SFG signal; however, these methods tend to be complicated and expensive. In fact many SFG practitioners do not have the ability to remove NR-SFG signal components, and systems designed to remove NR-SFG signal contributions may not be able to do so for some materials. We have worked to help develop a better understanding of NR-SFG. As part of this work, a better understanding of the temporal and phase behavior of NR-SFG signal has been developed, based on the behavior of NR-SFG signal from Si(111) wafers. This work calls into question some assumptions underlying nonresonant suppression methods based on time-domain detection. A new method for nondestructively testing (NDT) materials has been developed that uses nonresonant second harmonic generation, the degenerate form of SFG. This new NDT technology has the potential to detect several forms of material damage, such as aluminum sensitization, and plastic deformation of materials, which are largely invisible to current NDT technologies. Methods for extracting functional group orientation from VSFG data that contains NR-SFG contributions are also demonstrated and used to investigate how the surface of high density polyethylene changes in response to mechanical deformation. This work shows that the inability to remove NR-SFG contributions from VSFG spectra does not mean that these instruments cannot be used to make important discoveries. It simply means that NR-SFG contributions must be properly understood and accounted for during experimental design, and kept in mind during the analysis of VSFG spectra.
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Olszak, Peter D. "Nonlinear absorption and free carrier recombination in direct gap semiconductors." Doctoral diss., University of Central Florida, 2010. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/4620.
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Nonlinear absorption of Indium Antimonide (InSb) has been studied for many years, yet due to the complexity of absorption mechanisms and experimental difficulties in the infrared, this is still a subject of research. Although measurements have been made in the past, a consistent model that worked for both picosecond and nanosecond pulse widths had not been demonstrated. In this project, temperature dependent two-photon (2PA) and free carrier absorption (FCA) spectra of InSb are measured using femtosecond, picosecond, and nanosecond IR sources. The 2PA spectrum is measured at room temperature with femtosecond pulses, and the temperature dependence of 2PA and FCA is measured at 10.6[micro]meters using a nanosecond CO[sub]2 laser giving results consistent with the temperature dependent measurements at several wavelengths made with a tunable picosecond system. Measurements over this substantial range of pulse widths give results for FCA and 2PA consistent with a recent theoretical model for FCA. While the FCA cross section has been generally accepted in the past to be a constant for the temperatures and wavelengths used in this study, this model predicts that it varies significantly with temperature as well as wavelength. Additionally, the results for 2PA are consistent with the band gap scaling (Eg[super]-3) predicted by a simple two parabolic band model. Using nanosecond pulses from a CO?éé laser enables the recombination rates to be determined through nonlinear transmittance measurements. Three-photon absorption is also observed in InSb for photon energies below the 2PA band edge. Prior to this work, data on three-photon absorption (3PA) in semiconductors was scarce and most experiments were performed over narrow spectral ranges, making comparison to the available theoretical models difficult. There was also disagreement between the theoretical results generated by different models, primarily in the spectral behavior.; Therefore, we studied the band gap scaling and spectra of 3PA in several semiconductors by the Z-scan technique. The 3PA coefficient is found to vary as (Eg[super]-7), as predicted by the scaling rules of simple two parabolic band models. The spectral behavior, which is considerably more complex than for 2PA, is found to agree well with a recently published theory based on a four-band model.ID: 029050684; System requirements: World Wide Web browser and PDF reader.; Mode of access: World Wide Web.; Thesis (Ph.D.)--University of Central Florida, 2010.; Includes bibliographical references.
Ph.D.
Doctorate
Optics and Photonics
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Rasekh, Payman. "Kerr Effect at the THz Frequencies." Thesis, Université d'Ottawa / University of Ottawa, 2020. http://hdl.handle.net/10393/41085.
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This doctoral dissertation focuses on the nonlinear optical response of water vapour as well as some solids at terahertz (THz) frequencies. In this study, the propagation of broadband single-cycle THz pulses through a medium with the third-order nonlinear optical response is theoretically investigated. Also, a technique to measure the nonlinear response of transparent materials based on the time-domain THz spectroscopy is developed, which provides frequency dispersion curves of the nonlinear Kerr coefficient (n₂).
A numerical model is used to simulate the THz pulse propagation. This model takes
into account non-paraxial effects, self-focusing, and diffraction, as well as dispersion,
in both the linear and nonlinear optical regimes. The contribution of non-instantaneous
Kerr-type nonlinearity to the overall instantaneous and delayed Kerr effect at the THz
frequencies is investigated. It is shown how increasing the nonlinear relaxation time and its dispersion modifies the THz pulse after the propagation through a transparent medium. The effect of linear dispersion on self-action during pulse propagation is also discussed.
Moreover, the nonlinear spectroscopy of water vapour at THz frequencies is reported. Atmospheric water vapour has a rich spectrum with several strong resonances at frequencies below 3 THz, falling within the range of operation of most existing THz sources. An extremely large nonlinear response to THz radiation is observed at the positions of these resonances. Using the optical Kerr model for the nonlinear response, a minimum nonlinear refractive index of the order of 10² m²/W is estimated. The results provide insight into the energy levels of the water molecule and give a more accurate picture of its response to electromagnetic radiation, paving the way to more accurate THz spectroscopy, imaging, and sensing systems, and thereby facilitating future emerging THz technologies.
Finally, the nonlinear response of solids at THz frequencies is studied. It has been
shown that a phonon-induced THz Kerr effect can result in a larger nonlinear refractive
index than the nonlinear refractive index at the visible or near-infrared range (optical
Kerr effect). This pronounced nonlinear optical behavior is verified using a time-domain characterization approach. The results indicate a large delay occurred to the THz fields as they transmit through some of the material samples. In the frequency domain, the induced nonlinear phase shift of the intense THz field is shown to be relatively large of the order of 0.1 rad. From the phase information, the nonlinear phase is extracted by which the dispersion profile of n₂ is obtained.
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Shah, Anjali. "External cavity diode lasers and non-linear optical frequency conversion in spectroscopic applications." Thesis, St Andrews, 2006. http://hdl.handle.net/10023/142.
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Peceli, Davorin. "Absorptive and Refractive Optical Nonlinearities in Organic Molecules and Semiconductors." Doctoral diss., University of Central Florida, 2013. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/5687.
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The main purpose of this dissertation to investigate photophysical properties, third order nonlinearity and free carrier absorption and refraction in organic materials and semiconductors. Special emphasis of this dissertation is on characterization techniques of molecules with enhanced intersystem crossing rate and study of different approaches of increasing triplet quantum yield in organic molecules. Both linear and nonlinear characterization methods are described. Linear spectroscopic characterization includes absorption, fluorescence, quantum yield, anisotropy, and singlet-oxygen generation measurements. Nonlinear characterization, performed by picosecond and femtosecond laser systems (single and double pump-probe and Z-scan measurements), includes measurements of the triplet quantum yields, excited-state absorption, two-photon absorption, nonlinear refraction and singlet and triplet-state lifetimes. The double pump-probe technique is a variant of the standard pump-probe method but uses two pumps instead of one to create two sets of initial conditions for solving the rate equations allowing a unique determination of singlet- and triplet-state absorption parameters and transition rates. The advantages and limitations of the the double pump-probe technique are investigated theoretically and experimentally, and the influences of several experimental parameters on its accuracy are determined. The accuracy with which the double pump-probe technique determines the triplet-state parameters improves when the fraction of the population in the triplet state relative to the ground state is increased. Although increased accuracy is in principle achievable by increasing the pump fluence in the reverse saturable absorption range, it is shown that the DPP is optimized by working in the saturable absorption regime. Two different approaches to increase intersystem crossing rates in polymethine-like molecules are presented: traditional heavy atom substitution and molecular levels engineering. Linear and nonlinear optical properties of a series of polymethine dyes with Br- and Se- atoms substitution, and a series of new squaraine molecules, where one or two oxygen atoms in a squaraine bridge are replaced with sulfur atoms, are investigated. A consequence of the oxygen-to-sulfur substitution in squaraines is the inversion of their lowest lying ??' and n?' states leading to a significant reduction of singlet-triplet energy difference and opening of an additional intersystem channel of relaxation. Experimental studies show that triplet quantum yields for polymethine dyes with heavy-atom substitutions are small (not more than 10%), while for sulfur-containing squaraines these values reach almost unity. Experimental results are in agreement with density functional theory calculations allowing determination of the energy positions, spin-orbital coupling, and electronic configurations of the lowest electronic transitions. For three different semiconductors: GaAs, InP and InAsP two photon absorption, nonlinear refraction and free carrier absorption and refraction spectrums are measured using Z-scan technique. Although two photon absorption spectrum agrees with the shape of theoretical prediction, values measured with picosecond system are off by the factor of two. Nonlinear refraction and free carrier nonlinearities are in relatively good agreement with theory. Theoretical values of the third order nonlinearities in GaAs are additionally confirmed with femtosecond Z-scan measurements. Due to large spectral bandwidth of femtosecond laser, three photon absorption spectrum of GaAs was additionally measured using picosecond Z-scan. Again, spectral shape is in excellent agreement with theory however values of three photon absorption cross sections are larger than theory predicts. ?Ph.D.
Doctorate
Optics and Photonics
Optics and Photonics
Optics
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Delmonte, Valentin. "Spectroscopie cohérente des excitons dans des nanostructures semi-conductrices innovantes." Thesis, Université Grenoble Alpes (ComUE), 2018. http://www.theses.fr/2018GREAY015/document.
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L'évolution des technologies liées aux semi-conducteurs a amené à l'étude de la cohérence des Bits Quantiques (Qbits) dans l'objectif de réduction de la taille des composants. A l'aide de la spectroscopie cohérente non-linéaire, j'ai pu étudier les propriétés de cohérences des excitons confinés dans des boites quantiques (BQ), eux-même intégrées dans différentes nano-structures. L'intérêt des nano-structures est d'augmenter le ratio signal-sur-bruit, indispensable dans notre expérience. L'utilisation des nano-structures est aussi indispensable dans l'objectif de la mise en place d'un couplage radiatif à longue distance entre 2 BQs. Il fut tout d'abord nécessaire de caractériser des nano-structures déterministes permettant d'augmenter le rendement d 'échantillons utilisables en conservant l'intensité de signal émit par les BQs. De plus, j'ai développé mon expérience afin d'affiner notre capacité d'étudier le couplage proches entre BQs intégrées dans une micro-cavité. Ensuite Nous avons testé plusieurs formes de nano-structures 1D (trompettes et ridges) afin de d'amplifier le couplage à longue distance et et comprendre les obstacles auxquels nous auront à faire face . Enfin une caractérisation de nouveaux matériaux 2D fut réalisée, en vue de d'améliorer notre compréhension des dynamiques des excitons dans ce type de matériauxThe evolution of technologies related to semiconductors has led to the study of the coherence of Quantum Bits (Qbits) in order to reduce the size of the components. Using nonlinear coherent spectroscopy, I was able to study the coherence properties of excitons confined in quantum dots (BQs), themselves integrated into different nano-structures. The interest of nanostructures is to increase the signal-to-noise ratio, essential in our experience. The use of nano-structures is also essential for the purpose of setting up a long-distance radiative coupling between 2 BQs.First of all, it was necessary to characterize deterministic nano-structures that make it possible to increase the yield of usable samples by preserving the signal intensity emitted by the BQs. In addition, I developed my experience to refine our ability to study close-coupling between BQs embedded in a micro-cavity. Then we tested several forms of 1D nano-structures (trumpets and ridges) in order to amplify the long-distance coupling and to understand the obstacles we will have to face. Finally a characterization of new 2D materials was realized, in order to improve our understanding of exciton dynamics in this type of materials
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Johnson, Magnus. "Vibrational Sum Frequency and Infrared Reflection/Absorption Spectroscopy Studies of the Air/Liquid and Liquid/Metal Interfaces." Doctoral thesis, Stockholm, 2005. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-455.
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Isaienko, Oleksandr. "Development of ultra-broadband ultrafast infrared sources and applications to nonlinear vibrational spectroscopy of interfaces." Diss., Temple University Libraries, 2011. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/141408.
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ChemistryPh.D.
Interfaces play a crucial role in the exchange of energy and matter in various physical, chemical and biological systems. A particular interest has been to study interfaces between aqueous phases and various minerals because of their importance in understanding geochemical phenomena as well as for applications such as enhanced oil recovery. The nonlinear optical technique of vibrational sum-frequency generation (SFG) spectroscopy, introduced over 20 years ago, has become a powerful tool to investigate various surfaces, in particular, mineral-water interfaces. One of the challenges of the SFG spectroscopy of aqueous surfaces is the need to tune the central frequency of relatively narrowband IR lasers through the broad range of the OH-stretch frequencies of water molecules (3000 - 4000 cm-1). We have developed a novel ultrabroadband IR laser source that generates infrared pulses in the ~2800-6000 cm-1 range (lambda~3300-1800 nm) with bandwidths Delta(nu)>1000 cm-1, and bandwidths >2000 cm-1 in the near-IR range (lambda~1000-2000 nm). Pulse front tilt of signal pulse has been corrected allowing for compression of signal pulses down to 25 fsec. Such ultrabroadband IR pulses allow us to perform SFG spectroscopy of aqueous surfaces over the entire frequency range of water molecule spectrum (extending from ~2900 cm -1 to ~3800 cm -1) simultaneously, without tuning the laser ("in one shot"). We have used this novel ultrabroadband IR source to investigate the vibrational SFG spectra of silica/water interfaces. The high signal-to-noise ratio of our spectroscopic setup has allowed us to study low-intensity features that were not studied in detail, or recognized previously in the SFG-spectroscopy investigations, including: 1) non-hydrogen bonded OH vibrations at hydrophilic silica/water interfaces; 2) combination [stretch+bend] bands of water at the silica surface appearing at ~5000-5200 cm -1. 3) Overtones of water stretching modes at silica/water interfaces. The most important conclusions from these studies are outlined below. 1. Non-hydrogen bonded hydroxyls at silica/water interface. Typically SFG-studies of mineral/water interfaces (in particular, silica/water) have focused on the most pronounced features - peaks of H-bonded hydroxyls at ~3150 and ~3450 cm -1. We have been able to systematically observe and study a weaker peak at ~3670 - 3700 cm -1. This peak becomes more pronounced as the pH of aqueous phase decreases, as well as the ionic strength increases, indicating that the hydroxyls corresponding to this spectral feature are situated in a very close proximity to the surface. Isotopic dilution experiments indicate that the 3700 cm -1 feature is not due to asymmetric OH stretches as was suggested before. Based on our results, we suggest that this spectral feature corresponds to hydroxyls of water molecules at the silica surface that cannot hydrogen bond with silanol groups because of the lower density of silanols compared to H2O. We believe this to be the first surface-specific study of non-hydrogen bonded hydroxyls at silica, a surface widely accepted as hydrophilic. 2. SFG spectroscopy of [ν(OH)+δ(HOH)] combination bands of water at silica surface. We have extended SFG spectroscopy of the interfacial hydroxyls at mineral/water surfaces into the near-IR frequency range. The studies of overtones of interfacial OH(OD) groups will provide information on the anharmonicity of such species, and thus on the energy of dissociation. In addition, the positions of the overtone frequencies of the hydroxyls are more sensitive to interactions with the environment than the fundamental stretch frequencies. Our particular focus has been to study the stretch+bend combination band nu comb nu;(OH)+delta;(HOH) of liquid water which occurs in the near-IR spectral range at ~5000-5200 cm -1. It is typically much weaker in the FTIR absorption spectra than the fundamental transitions of the OH stretches or HOH bending, similar to overtones of these modes. We have performed, what we believe to be, the first surface-specific vibrational SFG spectroscopic measurements of combination bands of water molecules at silica surfaces. SFG spectroscopy of water combination band allows access to the water bending mode (delta~1600 cm -1), which still has not been observed in sum-frequency.
Temple University--Theses
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Поліщук, Аркадій Петрович, Олександра Валеріївна Грідякіна, and Ганна Борисівна Бордюг. "Matrix effec on the electrooptical properties of heptylviologen." Thesis, XXIII ISSSMC, 2017. http://er.nau.edu.ua/handle/NAU/32388.
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Atherton, Kathryn Jane. "Coherent Raman studies of optical nonlinearities in conjugated molecules and polymers." Thesis, Imperial College London, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.298790.
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Maugeri, Pearson Thomas Maugeri. "Applications of resonance Raman spectroscopy to the study of bioinorganic macromolecules." The Ohio State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=osu1512093478871388.
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Khan, Md Rubel. "Adsorption and Self-Assembly of Surfactants at Air-Liquid and Liquid-Metal Interfaces Studied by Sum Frequency Generation (SFG) Spectroscopy." Ohio University / OhioLINK, 2009. http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1620212735093219.
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Khan, Md Rubel. "Adsorption and Self-Assembly of Surfactants at Air-Liquid and Liquid-Metal Interfaces Studied by Sum Frequency Generation (SFG) Spectroscopy." Ohio University / OhioLINK, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1620212735093219.
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Lydiatt, Francis Peter. "Vibrational sum-frequency spectroscopy : towards understanding adsorbate behaviour on substrates relevant to the nuclear fuel cycle." Thesis, University of Manchester, 2014. https://www.research.manchester.ac.uk/portal/en/theses/vibrational-sumfrequency-spectroscopy-towards-understanding-adsorbate-behaviour-on-substrates-relevant-to-the-nuclear-fuel-cycle(3a81bdcc-75d9-4fed-a949-ad43198625be).html.
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The primary goal of this thesis was to commission an instrument for vibrational sum frequency spectroscopy (VSFS), and exploit it for the study of solid/gas interfaces; of ultimate interest is characterisation of substrate surfaces in humid environments. Such effort is motivated by interest in understanding the potential for atmospheric corrosion in dry storage facilities of spent nuclear fuels or other nuclear-related wastes. VSFS is a non-linear, interface specific, vibrational spectroscopy, in which two photons of different energies (infrared (IR) and visible (VIS)) impinge upon a surface at the same point at the same time, leading to the generation of a third (sum-frequency generation (SFG)) photon. Features in VSFS spectra can be assigned to vibrational modes of interfacial species, and so enable details of interfacial structure and chemistry to be elucidated. An instrument for such measurements has been developed using laser facilitates located in the Photon Science Institute (PSI) of The University of Manchester. More specifically, an ultra-fast (femtosecond) laser has been employed as a light source, enabling acquisition of spectra (~250 cm-1 in width at a resolution of ~11 cm-1) without the need for scanning the energy of either IR or VIS beams, i.e. so called broad-band VSFS. To test performance, data have been acquired from self-assembled monolayers of alkanethiols (octadecanethiol) on gold substrates, which demonstrate the utility of the instrument. Subsequent to commissioning, the VSFS instrument was initially exploited to study the interaction of two organic molecules, acetonitrile and acetic acid, with a single crystal TiO2(110) substrate; measurements were performed with the sample exposed to the vapour of each organic species under ambient conditions. Surface adsorption was identified through the appearance of the CH3 symmetric stretch. Furthermore, spectra as a function of light (IR/VIS/SFG) polarization combinations have been recorded to explore adsorbate angular geometry. Finally, VSFS measurements have been undertaken from a number of substrates (GaAs, Au, Zn, Fe, Cr, stainless steel), as a function of relative humidity; D2O was employed to overcome the issue of loss of IR beam intensity due to interaction with atmospheric H2O. Signal quality varies significantly with substrate, with the most insight being gained for the interaction of D2O with polycrystalline Zn. Clear vibrational resonances due to both hydroxyls (OD) and molecular water (D2O) are observed, which vary with relative humidity, indicating that there are significant changes in interface structure with relative humidity.
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Dewan, Shalaka. "IONS AND THE STRUCTURE AND DYNAMICS OF INTERFACIAL WATER AT CHARGED SURFACES." Diss., Temple University Libraries, 2015. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/334453.
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ChemistryPh.D.
The distinct structure and dynamics of interfacial water are due to a break in the extended hydrogen bonding network present in bulk water. At solid-aqueous interfaces, the presence of surface charge, which induces a static electric field, and the electrolytes, which are present in most naturally relevant systems, can additionally perturb the hydrogen bonding environment due to polarization. The interplay between the surface-charge-induced electric field and the ions in changing the structure of interfacial water has important consequences in the chemistry of processes ranging from protein-water interactions to mineral-water reactivity in oil recovery. Accessing information about the first few layers of water at buried interfaces is challenging. Vibrational sum-frequency generation (vSFG) spectroscopy is a powerful technique to study exclusively the interfacial region and is used here to investigate the role of interfacial solvent structure on surface reactivity. It is known that the rate of quartz dissolution increases on addition of salt at neat water pH. The reason for this enhancement was hypothesized to be a consequence of perturbations in interfacial water structure. The vSFG spectra, which is a measure of ordering in the interfacial water structure, shows an enhanced effect of salt (NaCl) at neat pH 6~8. The trend in the effect of salt on vSFG spectra versus the bulk pH is remarkably consistent with the enhancement of rate of quartz dissolution, providing the first experimental correlation between interfacial water structure and silica dissolution. If salt alters the structure of interfacial water, it must affect the vibrational energy transfer pathways of water, which is extremely fast in bulk water (~130 fs). Thus far, the role of ions on the vibrational dynamics of water at charged surfaces has been limited to the screening effects and reduction in the depth of the region that contributes to vSFG. Here, we measure the ultrafast vibrational relaxation of the O-H stretch of water at silica at different bulk pH, using time-resolved (TR-vSFG). The fast vibrational dynamics of water (~200 fs) observed at charged silica surfaces (pH 6 and pH 12), slows down (~600 fs) on addition of NaCl only at pH 6 and not at pH 12. On the other hand at pH 2 (neutral surface), the vibrational relaxation shows an acceleration at high ionic strengths (0.5 M NaCl). The TR-vSFG results suggest that there is a surface-charge dependence on the sensitivity of the interfacial dynamics to ions and that reduction in the probe depth of vSFG alone cannot explain the changes in the vibrational lifetime of interfacial O-H. This is further supported by the cation specific effects observed in the TR-vSFG of the silica/water interface. While the vibrational relaxation of O-H stretch slows on addition of all salts (LiCl, NaCl, RbCl, and CsCl), the degree of slowing down is sensitive to the cation identity. The vibrational lifetime of O-H stretch in the presence of different cations follows the order: Li+ < Na+ < Rb+, consistent with previous Hofmeister effect reported in vSFG spectroscopy as well as AFM measurements at silica/water interface. To provide molecular insight on the effect of surface charge density and ionic strength on the changes in interfacial water structure, Molecular Dynamics (MD) simulations were performed on water at different types of surfaces. It was shown that the properties of water near the interface, e.g., a net orientation and the depth to which this persists, depend on the degree of specific adsorption of the counter ions. Our vSFG results, along with the insights from MD simulations, highlight the importance of considering the role of ions on the solvent structure within the electric double layer region, beyond the screening effects predicted by classical electrochemical models.
Temple University--Theses
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Liebel, Matz. "Understanding molecular dynamics with coherent vibrational spectroscopy in the time-domain." Thesis, University of Oxford, 2014. http://ora.ox.ac.uk/objects/uuid:e0289d80-f6e3-4e6f-817e-f8dd55d15bc4.
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This thesis describes the development of several spectroscopic methods based on impulsive vibrational spectroscopy as well as of the technique itself. The first chapter describes the ultrafast time domain Raman spectrometer including the development of two noncollinear optical parametric amplifiers for sub-10 fs pulse generation with 343 or 515 nm pumping. In the first spectroscopic study we demonstrate, for the first time, that impulsive vibrational spectroscopy can be used for recording transient Raman spectra of molecules in excited electronic states. We obtain spectra of beta-carotene with comparable, or better, quality than established frequency domain based nonlinear Raman techniques. The following two chapters address the questions on the fate of vibrational coherences when generated on a reactive potential energy surface. We photoexcite bacteriorhodopsin and observe anharmonic coupling mediated vibrational coherence transfer to initially silent vibrational modes. Additionally, we are able to correlate the vibrational coherence activation with the efficiency of the isomerisation reaction in bR. Upon generation of vibrational coherence in the second excited electronic state of beta-carotene, by excitation from the ground electronic state, we are able to follow the wavepacket motion out of the Franck-Condon region. We observe vibrationally coherent internal conversion, through a conical intersection, into the first excited electronic state and are hence able to demonstrate that electronic surface crossings can occur in a vibrationally coherent fashion. Additionally, we find strong evidence for vibronic coupling mediated back and forth crossing between the two electronic states. As a combination of this work we develop a IVS based technique that allows for the direct recording of background and baseline free Raman spectra in the time domain. Several proof of principle experiments highlight the capabilities of this technique for time resolved Raman spectroscopy. In the final chapter we present work on weak-field coherent control. Here, we address the question of whether a photochemical reaction can be controlled by the phase term of an electric excitation field, in the one photon excitation limit. We study the systems rhodamine 101, bacteriorhodopsin, rhodopsin and isorhodopsin and, contrary to previous reports, find no evidence for one photon control.
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Rouxel, Jérémy. "A rigorous multipolar framework for nanoparticles optical properties description : theory and experiments." Thesis, Troyes, 2015. http://www.theses.fr/2015TROY0013/document.
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Les propriétés optiques linéaires et non-linéaires de nanoparticules métalliques de tailles non-négligeables comparées à celles des longueurs d’onde excitatrices sont étudiées dans cette thèse. Les informations issues de la symétrie sont mises en avant afin de décrire des nanoparticules appartenant à des groupes ponctuels. Pour cela, un formalisme totalement irréductible est mis en place afin de prendre en compte l’extension spatiale des objets étudiés. Dans ce formalisme, le tenseur de réponse non-linéaire possède un nombre fini de valeurs significatives reliant les composantes multipolaires des champs incidents et sortants. Ce formalisme est alors appliqué analytiquement à l’étude de la réponse non- linéaire du second ordre de nano-étoiles d’or en interprétant des mesures de SHG résolue en polarisation. Finalement, des expériences de spectroscopies multidimensionnelles sont utilisées dans le but de connecter les propriétés spatiales et les propriétés spectrales de ces objets. L’introduction de modes propres définis par la symétrie des objets permet encore une fois de donner un sens physique aux comportements électroniques mis en jeuUsing metallic nanoparticles with a threefold symmetry thorough the study, the impact of the symmetry on the nonlinear properties is investigated. Interpretations of polarization-resolved SHG experiments indicate the importance of multipolar resonances, in particular quadrupole and octupole, to explain the strong values of the nonlinear susceptibilities in such systems. A fully irreducible formalism is then developed to treat extended objects like nanoparticles. In this formalism, the nonlinear response tensor is a discrete set of values easily constrained by symmetries instead of a field. This formalism permits to describe simply linear and nonlinear optical response from nanoparticles. Finally, time-domain experiments are conducted with the aim to connect spatial and spectral properties. These experiments allow to interpret the spectra in terms of eigenmodes
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LIBRANTZ, ANDRE F. H. "Estudo comparativo da emissoes do Nd(3+) nas configuracoes 4fsup(2)5d e 4fsup(3) induzidas pela excitacao multifotonica em cristais de YLF, GLF, LLF." reponame:Repositório Institucional do IPEN, 2000. http://repositorio.ipen.br:8080/xmlui/handle/123456789/10830.
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Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP
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Zhou, Dapeng. "The Excited State Behavior of Iminium Derivatives and Their Reduced Forms." Bowling Green State University / OhioLINK, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1370525481.
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Smirni, Salvatore. "Nonlinear dynamics of microcirculation and energy metabolism for the prediction of cardiovascular risk." Thesis, University of Dundee, 2018. https://discovery.dundee.ac.uk/en/studentTheses/c551cbef-6f00-48ef-b753-ad76ac93daf4.
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The peripheral skin microcirculation reflects the overall health status of the cardiovascular system and can be examined non-invasively by laser methods to assess early cardiovascular disease (CVD) risk factors, i.e. oxidative stress and endothelial dysfunction. Examples of methods used for this task are the laser Doppler flowmetry (LDF) and laser fluorescence spectroscopy (LFS), which respectively allow tracing blood flow and the amounts of the coenzyme NAD(P)H (nicotamide adenine dinucleotide) that is involved in the cellular production of ATP (adenosine triphosphate) energy. In this work, these methods were combined with iontophoresis and PORH (post-occlusive reactive hyperaemia) reactive tests to assess skin microvascular function and oxidative stress in mice and human subjects. The main focus of the research was exploring the nonlinear dynamics of skin LDF and NAD(P)H time series by processing the signals with the wavelet transform analysis. The study of nonlinear fluctuations of the microcirculation and cell energy metabolism allows detecting dynamic oscillators reflecting the activity of microvascular factors (i.e. endothelial cells, smooth muscle cells, sympathetic nerves) and specific patterns of mitochondrial or glycolytic ATP production. Monitoring these dynamic factors is powerful for the prediction of general vascular/metabolic health conditions, and can help the study of the mechanisms at the basis of the rhythmic fluctuations of micro-vessels diameter (vasomotion). In this thesis, the microvascular and metabolic dynamic biomarkers were characterised in-vivo in a mouse model affected by oxidative stress and a human cohort of smokers. Data comparison, respectively, with results from control mice and non-smokers, revealed significant differences suggesting the eligibility of these markers as predictors of risk associated with oxidative stress and smoke. Moreover, a relevant link between microvascular and metabolic oscillators was observed during vasomotion induced by α-adrenergic (in mice) or PORH (in humans) stimulations, suggesting a possible role of cellular Ca2+ oscillations of metabolic origin as drivers of vasomotion which is a theory poorly explored in literature. As future perspective, further exploration of these promising nonlinear biomarkers is required in the presence of risk factors different from smoke or oxidative stress and during vasomotion induced by stimuli different from PORH or α-adrenergic reactive challenges, to obtain a full picture on the use of these factors as predictors of risk and their role in the regulation of vasomotion.
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Figueira, David da Silva Leocadio 1980. "Desenvolvimento de fontes de radiação coerente na região azul com lasers semicondutores para experimentos de resfriamento e aprisionamento de átomos de cálcio." [s.n.], 2004. http://repositorio.unicamp.br/jspui/handle/REPOSIP/277775.
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Orientador: Flavio Caldas da CruzDissertação (mestrado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin
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Resumo: Esta tese apresenta o desenvolvimento de fontes de radiação coerente na região do azul baseadas em lasers semicondutores para excitar a transição de resfriamento e aprisionamento 1 S0-1P1 do Cálcio, em 423nm. Foi construído um laser de diodo em cavidade estendida emitindo em g =846 nm que foi empregado em uma configuração de Cavidade Estendida de Littman, estabilizada em freqüência pela técnica de Side-of-Fringe. Parte da potência deste laser foi amplificada por um amplificador óptico semicondutor. Potências superiores a 700mW em g =846nm foram obtidas. Parte desta potência do amplificador óptico (450mw) foi duplicada em frequência para g =423nm em um cristal de niobato de potássio(KNbO3), utilizado dentro de uma cavidade óptica ressonante com a freqüência do laser. A estabilização da cavidade óptica duplicadora de freqüência foi feita pela técnica de Hansch-Coulliaud . O sistema desenvolvido alcançou potências de 60mW de radiação coerente azul. Esta fonte laser portátil deverá ser utilizada para espectroscopia, resfriamento e aprisionamento de Cálcio
Abstract: This thesis presents the development of sources of coherent radiation in the blue region of the spectrum, based on semiconductors lasers, to excite the cooling and trapping 1S0-1P1 transition of neutral calcium atoms at 423nm. A diode laser emitting at g =846 nm was employed in an extended cavity Littman configuration, and stabilized in frequency by the Side-of-Fringe technique. Part of the laser power was amplified by an optical semiconductor amplifier. Output powers above 700mW at g =846nm were obtained. Part of this amplified power (450mW) was frequency doubled to g =423nm in a potassium niobate (KNbO3) crystal, placed inside a resonant optical cavity. The lock of the doubling optical cavity was made by the Hansch-Coulliaud technique. The developed system reached powers near 60mW of blue coherent radiation at 423nm. This portable laser source will be used for spectroscopy, cooling and trapping of calcium
Mestrado
Física
Mestre em Física
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ALVAREZ, Ammis Sánchez. "Armadilha magneto ótica de rubídio e mistura de quatro ondas no vapor atômico." Universidade Federal de Pernambuco, 2016. https://repositorio.ufpe.br/handle/123456789/18556.
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Facepe
Neste trabalho apresentamos a caracterização de uma armadilha magneto ótica de átomos de Rb construída em nosso laboratório, juntamente com o seu princípio de funcionamento. O resfriamento é feito com lasers de diodo e tem como mecanismo básico a força de pressão de radiação, que é gerada pelos processos de absorção e emissão de fótons, juntamente com a ação de um campo magnético e a polarização dos feixes. O sistema consiste em três pares de feixes contrapropagantes nas direções x, y e z, com polarizações s+ e s, e um campo magnético que varía linearmente no espaço. Conseguimos armadilhar aproximadamente 108 átomos com um tempo de carga da ordem de 2 seg. Em paralelo realizamos medidas de mistura de quatro ondas degenerada em um vapor de átomos de Rb, na configuração de feixes quase-copropagantes. O sinal gerado no processo não linear foi estudado em função da frequência de um dos feixes enquanto o outro tinha sua frequência fixa; e se mostrou independe de qual dos feixes esta sendo sintonizado. Medidas simultâneas da transmissão do feixe de prova indicam que o processo não linear ocorre só na transição cíclica e envolve o grupo de átomos selecionados pelo feixe de frequência fixa.
In this work we present a characterization of magneto optical trap of 87Rb atoms built in our lab, along with its operating principle. The cooling is done with a diode laser and its basic mechanism is the force of radiation pressure, which is generated by the processes of absorption and emission of photons, together with the action of a magnetic field and polarization of the beams. The system consists of three pairs of counterpropagating beams in the x, y and z directions with s+ and s polarizations, and a magnetic field that varies linearly in space. We were able to trap about 108 atoms with a charging time of approximately 2 sec. In parallel we performed degenerate four wave mixing measures in a Rb vapor atoms using a quasi-copropagating beams configuration. The signal generated in the nonlinear process was studied as a function of one of laser’s while keep the other with a fixed frequency; and it showed independent of which of the beams is being tuned. Simultaneous measurements of the transmission of the probe beam indicates that the nonlinear process occurs only in the cyclic transition and involves the group of atoms selected by the beam with fixed frequency.
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Neveu, Pascal. "Propagation de lumière dans l'hélium métastable : stockage, amplification, fluctuations et bruit quantique." Thesis, Université Paris-Saclay (ComUE), 2019. http://www.theses.fr/2019SACLN044/document.
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Un état quantique de lumière est caractérisé par la statistique de son nombre de photons. Lorsque qu'un champ électromagnétique se propage dans un milieu, ses statistiques peuvent être modifiées, notamment en présence de phénomènes cohérents. Cette thèse s'intéresse expérimentalement et théoriquement à la propagation d'états quantiques de lumière dans une vapeur d'hélium métastable à température ambiante. Dans un premier temps, on étudie la propagation de lumière en présence d'oscillations cohérentes de populations ultrafines et montre qu'elles permettent de stocker efficacement une quadrature spécifique d'un champ lumineux. Néanmoins, ce protocole ne permet pas de stocker les deux quadratures d'un mode du champ électromagnétique, et les conditions de propagation dans le milieu dégradent leurs propriétés statistiques, empêchant son utilisation pour des applications quantiques. Ce travail montre ensuite qu'il est possible de générer des états comprimés à deux modes dans ce même système, par mélange à 4 ondes. Les états fortement comprimés (9 dB) peuvent être générés en exploitant les fortes non-linéarités induites par piégeage cohérent de population via une transition optique, ainsi que par la proximité d'une autre transition optique voisine. Enfin, une dernière partie s'intéresse au transfert de bruit par effet Faraday entre les fluctuations de spin atomique du milieu et les fluctuations de polarisation d'un champ lumineux. L'étude de ces fluctuations par spectroscopie de bruit de spin a mis en évidence des comportements originaux qui pourraient par la suite être utilisés dans d'autres milieuxA quantum state of light is characterized by its statistics of number of photons. These statistics can change in the presence of coherent phenomena. This PhD focuses both experimentally and theoretically on the propagation of quantum states within a room temperature vapor of metastable helium. First, we show that ultranarrow coherent population oscillations allow to efficiently store a specific quadrature of a light wave. Nevertheless, this protocol cannot be use to store the two quadratures of a light field. Indeed, the propagation conditions deteriorates its statistical properties, forbidding its use for quantum application. Secondly, we show that it is possible to generate twomode squeezed states of light in that system. High amplification can be achieved (9 dB), exploiting the strong nonlinearities enabled by coherent population trapping of a transition, and because of the energy level structure. Finally, we study atomic spin noise transfer to light polarization noise via Faraday effect. These fluctuations, probed by spin noise spectroscopy, show original behaviors that may be useful in another systems
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Picot-Clémente, Jérémy. "Etude de sources supercontinuum à fibres optiques en verre de tellurite pour la spectroscopie d'absorption moyen infrarouge appliquées à la détection de gaz." Thesis, Dijon, 2015. http://www.theses.fr/2015DIJOS040/document.
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Ce manuscrit de thèse présente le développement et l’étude d’une source supercontinuum dans l’infrarouge moyen pour une application de détection de gaz par spectroscopie d’absorption. L’étude des sources supercontinuum est basée sur la propagation non-linéaire d’impulsions ultracourtes dans un verre de tellurite de composition 80TeO2-10ZnO-10Na2O (% molaire) et utilisé sous trois formes différentes, à savoir un échantillon massif sous la forme d’une pastille, puis une fibre microstructurée à cœur suspendu fabriquée à partir de ce même verre, et enfin cette dernière fibre ultérieurement effilée (aussi appelée « taper »). Ces trois options d’utilisation s’adaptent à différents types de sources lasers disponibles commercialement et permettent d’optimiser la génération d’une source de lumière recouvrant une gamme très large de fréquences. Chaque observation expérimentale est accompagnée de simulations numériques correspondantes qui mettent en évidence les différents mécanismes physiques et dynamiques de la génération de supercontinuum. La première étude reporte la mise en œuvre d’une source supercontinuum induite par filamentation dans l’échantillon massif, à l’aide d’un laser femtoseconde de forte énergie (plusieurs micro-Joules), et associée à une caractérisation spectro-angulaire complète. Puis, l’accent a été mis sur la génération de supercontinuum dans les fibres optiques microstructurées à cœur suspendu (avec ou sans taper) à l’aide de sources lasers femtosecondes nano-Joules. Une étude complète de fabrication et d’optimisation des propriétés de ces fibres avec ou sans taper a été menée, notamment pour améliorer les contributions linéaires et non-linéaires du guidage sur la propagation et les conversions de fréquences associées. Une source supercontinuum s’étalant de 0.6 à 3.3 µm (équivalent à 400 THz de largeur spectrale) est obtenue avec une fibre d’une longueur de 10 cm. Enfin, une source s’étalant de 0.9 à 2.6 µm, à l’aide d’un laser à fibre plus compact, a été développée grâce aux fibres microstructurées effilées pour une application de détection de gaz. Le principal objectif étant d’explorer les raies d’absorption au-delà de 2 µm, qui sont reconnues comme étant bien plus intenses et donc plus faciles à détecter. Un dispositif expérimental de spectroscopie d’absorption par source supercontinuum dans une cellule multi-passage compacte a été mis en place avec succès pour la détection de méthaneThis work focuses on the development of mid-infrared supercontinuum light sources and their application for gas detection through absorption spectroscopy. The study of supercontinuum sources is based on nonlinear ultrashort pulse propagation in tellurite glass (80TeO2-10ZnO-10Na2O) and used in three different forms, namely a thin bulk sample, a microstructured suspended-core fiber, and a tapered suspended-core fiber. These technical means adapt themselves to distinct laser sources commercially available, thus optimizing the implementation of ultrawide-band infrared light sources. Experimental observations are compared to corresponding numerical simulations, thus pointing out the different underlying physical mechanisms of supercontinuum generation. The first study reports the filamentation-induced supercontinuum source in the tellurite glass bulk sample by means of a high-energy femtosecond laser (several micro-Joules) and associated with a complete spectro-angular mapping of light distribution. Then, the main task is related to supercontinuum generation in microstructured suspended-core fibers (with or without tapering) using nano-Joule femtosecond laser sources. A complete analysis of the fiber design was performed, especially to enhance linear and nonlinear wave propagation for efficient frequency conversion processes. As a result, a supercontinuum source covering the 0.6-3.3 µm region (i.e., 400-THz spectral bandwidth) is obtained in a 10-cm tapered fiber segment. Finally, another supercontinuum source covering the 0.9-2.6 µm region, pumped by a very compact fiber laser, was developed, in particular for its application in a gas detector system. The main goal is to explore absorption lines beyond 2 µm, which are known to be more intense and then easier to detect. A complete experimental setup for supercontinuum absorption spectroscopy based on a compact multi-pass cell was successfully developed for methane detection
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Noblet, Thomas. "Etude optique du couplage vibroélectronique à l'interface entre boîtes quantiques semiconductrices et molécules organiques." Thesis, Université Paris-Saclay (ComUE), 2019. http://www.theses.fr/2019SACLS272.
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Les processus physico-chimiques se produisant au sein des nanoparticules que sont les boîtes quantiques semiconductrices (QDs) sont à l'origine d'une nouvelle classe de sondes fluorescentes trouvant des applications en catalyse, en reconnaissance moléculaire et en imagerie. Le confinement quantique des électrons aux sein de ces objets luminescents, qui donne lieu à leur structure excitonique si particulière, permet de tirer simultanément profit de leurs propriétés optiques d'absorption et d'émission dans la gamme spectrale visible, et ce, dans le but de faciliter la détection et l’identification des espèces chimiques situées dans leur environnement proche. Dans ce contexte, nous nous sommes intéressés à des QDs de 3 à 4 nm de diamètre, composées d’un alliage ternaire de cadmium, de tellure et de soufre, et fonctionnalisées par des ligands mercaptocarboxyliques. De manière à déterminer l’ensemble de leurs propriétés structurales, chimiques et optoélectroniques, nous les avons tout d’abord caractérisées à l’état de solutions colloïdales par diverses techniques expérimentales : microscopie électronique, zêta-métrie, analyse par diffusion dynamique de la lumière, spectroscopies de rayons X, d’absorption UV-visible et d’émission de fluorescence. Ceci nous a permis de déduire la composition chimique des nanocristaux, leur structure cristalline, leur taille, leur dispersion en taille, la composition chimique de leurs ligands, les énergies propres de leurs états électroniques, leur moments dipolaires de transition et leur section efficace d’absorption. Fort de ces connaissances, nous avons pu développer un modèle analytique pour calculer la susceptibilité diélectrique des QDs et extraire de cette manière leur fonction de réponse linéaire, véritable carte d’identité optoélectronique. Nous avons ensuite optimisé la conception par voie chimique d’interfaces composées de QDs et de différentes espèces moléculaires organiques, dépôts réalisés sous forme de monocouches ou de films épais sur des substrats solides plans de silicium, de verre et de fluorure de calcium fonctionnalisés par des organosilanes. Ces interfaces substrat/QDs/molécules ont alors été étudiées par spectroscopie linéaire d’absorption UV-visible et par spectroscopie optique non-linéaire de génération de fréquence-somme (SFG). La première nous a permis de déterminer la densité superficielle des QDs déposés et d’en caractériser la stabilité temporelle, et la seconde, qui combine deux lasers visible et infrarouge, d’identifier la signature vibrationnelle des ligands recouvrant les QDs. Grâce à ces échantillons, nous avons alors montré par spectroscopie SFG deux couleurs l’existence d’un couplage vibroélectronique entre les QDs et leur environnement moléculaire. En particulier, nous avons démontré que l’amplitude de vibration des modes moléculaires associés aux ligands des QDs et aux organosilanes greffés sur les substrats est maximale lorsque les QDs sont eux-mêmes stimulés par la lumière visible dans leur premier état excitonique. Cette démonstration expérimentale s’accompagne par ailleurs d’une démonstration théorique : en utilisant les diagrammes de Feynman dans l’espace des fréquences imaginaires de Matsubara, nous avons déterminé l’expression analytique de la susceptibilité non-linéaire d’ordre 2 du complexe QD/molécule. Nous avons alors vérifié que l’hypothèse d’un couplage dipolaire entre QDs et molécules menait à une modélisation de la réponse vibrationnelle SFG compatible avec les mesures expérimentales. De cette manière, l’existence d’un couplage vibroélectronique de nature dipolaire entre boîtes quantiques et molécules est attestéThe different physico-chemical processes occurring within semiconductor quantum dots (QDs) give rise to a new class of fluorescent probes and a wide range of applications in catalysis, molecular recognition and imaging. Within these luminescent nanoparticles, the quantum confinement of electrons, which leads to their very special excitonic structure, allows us to benefit from both their absorption and emission optical properties, with the specific aim of fostering the detection and the identification of the chemical species located in their direct environment. Within this framework, we were interested in 3 to 4-nm-sized QDs composed of ternary alloys of cadmium, telluride and sulfur, and functionalized by mercaptocarboxylic ligands. In order to determine their structural, chemical and optoelectronic properties, we first characterized them thanks to several experimental techniques: electron microscopy, zeta potentiel measurements, dynamic light scattering analysis, X-ray, UV-visible and fluorescence spectroscopies. This enabled us to deduce the chemical composition of the nanocrystals, their crystal structure, size, size-dispersion, the chemical composition of their ligands, the eigenenergies of their electronic states, their transition dipole moments and absorption cross-sections. Given all those results, we succeeded in deriving an analytical model of the QD dielectric susceptibility and extracting in this way their linear response function. Then, we optimized the chemical synthesis of nanostructured interfaces made of QDs and various molecular species through the use of flat solid substrates of silicon, glass and calcium fluoride functionalized with organosilanes. These substrate/QDs/molecules interfaces were studied by linear UV-visible absorption spectroscopy and by sum-frequency generation non-linear optical spectroscopy (SFG). The former allowed us to determine the surface density of the deposited QDs and to characterize their stability over time, while the later, which combines two visible and infrared lasers, enabled us to identify the vibrational signature of the QD ligands. Thanks to those samples probed by two-colour SFG spectroscopy, we therefore shew the existence of a vibroelectronic coupling between QDs and their molecular surroundings. Especially, we demonstrated that the vibration amplitudes associated to the molecular modes of the QD ligands and the organosilanes grafted on the substrates are maximum when the QDs are excited by visible light into their first excitonic state. This experimental demonstration is further supported by theoretical considerations: Feynman diagrams in Matsubara imaginary-time representation were used to determine the analytical expression of the second-order nonlinear susceptibility of the QD/molecule bipartite system. We thus verified that the hypothesis of a dipolar coupling between QDs and molecules resulted in a modeling of the vibrational SFG response which proved to be in complete agreement with the experimental measurements. Thus, we evidenced the existence of a dipolar vibroelectronic coupling between quantum dots and molecules
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Armougom, Julie. "Nouvelles sources optiques pour la détection d’espèces chimiques dans la bande III." Thesis, Université Grenoble Alpes (ComUE), 2018. http://www.theses.fr/2018GREAT077/document.
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La spectrométrie laser d'absorption différentielle est une technique bien connue pour la détection à distance d'espèces chimiques dans l'atmosphère. À ce titre, la bande III qui s'étend entre 8 et 12 µm est une région particulièrement intéressante, car les bandes d'absorption de nombreuses espèces chimiques y sont intenses et se recouvrent peu entre elles. Afin de détecter ces espèces à distance dans la bande III, il est nécessaire de disposer de sources dont le rayonnement est fin spectralement, largement accordable, et énergétique. Les sources basées sur l'optique non linéaire du second ordre constituent la seule technologie capable de répondre à ces besoins. Dans ce travail de thèse, nous présenterons des résultats expérimentaux portant sur deux architectures de sources paramétriques permettant d'émettre un rayonnement dans la bande III adapté à la spectrométrie différentielle en configuration lidar. La première architecture consiste à émettre un faisceau directement dans la bande III grâce au pompage de cristaux non linéaire par des sources laser à 2 µm. La seconde architecture, consiste à amplifier les ondes signal et complémentaire issues d'un OPO à 2 µm, avant de les convertir dans la bande III par différence de fréquences. Ces sources sont basées sur l'association de technologies émergentes et sont susceptibles d'offrir des solutions viables au manque de sources émettant dans la bande IIILaser spectrometry by differential absorption is a well-known technique for standoff detection of chemical species in the atmosphere. The longwave infrared region (LWIR), ranging from 8 to 12 µm is particularly interesting because the absorption bands of many chemical species are intense and non-overlapping. In order to detect those species in the LWIR, there is a need for sources that are spectrally narrow, widely tunable, and delivers high energies. The sources based on second order nonlinear optics are the only technology able to meet those requirements. In this work, we will present the experimental results on two parametric architectures that allows emission in the LWIR for lidar measurements. The first one consists in emitting a beam directly in the LWIR by pumping nonlinear crystals with 2 µm pump lasers. The second architecture consists in amplifying the signal and idler beams coming from a 2 µm OPO, before converting them into the LWIR by difference frequency generation. Those sources are based on the association of new technologies and have the potential to offer a viable solution to a lack of sources emitting in the LWIR
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Cheminal, Alexandre. "Ultrafast energy conversion processes in photosensitive proteins and organic nanostructures for photovoltaic applications." Thesis, Strasbourg, 2015. http://www.theses.fr/2015STRAE012/document.
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Les techniques de spectroscopie femtoseconde permettent d’étudier les processus de conversion d’énergie dans les système organiques. Elles permettent d’étudier les populations photo-générées et leur évolution à l’échelle de ces photoréactions. Elles permettent de comprendre les transferts d’énergie et de charge intra- et inter-moléculaires à l’origine du fonctionnement de ces systèmes.La protéine de rétinal Anabaena sensroy Rhodopsin est un photocommutateur naturel, qui est étudié afin de comprendre les paramètres à l’origine de l’efficacité quantique d’isomérisation. Nous avons pu déterminer cette efficacité quantique pour les deux formes stables du rétinal ainsi que leur dynamique d’isomérisation dans les mêmes conditions expérimentales.La génération de charge dans des couches actives pour le photovoltaique organique est étudiée dans un système composé d’un mélange de PCBM et d’un donneur organique dérivé du colorant BODIPY. L’influence de la nanostructuration de la couche active sur la génération de charge est étudiée. La génération de charge est limitée dans ce système par la recombinaison des charges générées et par la diffusion des excition aux interfaces donneur-accepteur. Ces observations indiquent que l’amélioration de la nanostructuration de la couche active peut permettre d’augmenter les rendements de photo-génération de chargeFemtosecond transient spectroscopies are used to investigate photonic energy conversion inorganic systems. These techniques allow to observe the ground and excited states of themolecules at the timescale of the photoreactions. It is used to understand the inter- andintramolecular energy and charge transfers leading to the desired photochemical process.The natural photoswiching retinal protein Anabaena sensory Rhodopsin is studied to understand the key parameters ruling the isomerisation quantum yield. We could determine the isomerisation quantum yield of both stable forms and their dynamics in the very same experimental conditions.Charge generation is investigated in small molecule bulk heterojunction active layers for organic solar cells made of PCBM and a BODIPY dye-derivative donor. The influence of the active layer morphology on charge generation is studied. The charge generation is limited by charge recombination but also by exciton diffusion to the donor-acceptor interface. The active layer morphology has to be improved to achieve more efficient organic solar cells with these materials
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Louot, Christophe. "Sources de supercontinuum pour la microspectroscopie Raman cohérente large-bande." Thesis, Limoges, 2018. http://www.theses.fr/2018LIMO0015/document.
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La microspectroscopie Raman cohérente (CARS) est une méthode d'analyse optique sans marqueur qui permet d'identifier des liaisons moléculaires dans un milieu d'intérêt (échantillon) pour permettre de déterminer la composition chimique de ce milieu. Elle nécessite l'excitation concomitante de l'échantillon par deux ondes spectralement décalées (onde pompe et onde Stokes) afin de faire entrer en résonance les liaisons à détecter. Pour la détection de plusieurs liaisons simultanément (microspectroscopie Raman cohérente large-bande ou Multiplex-CARS), la source Stokes monochromatique est remplacée par une source laser large-bande (supercontinuum). Les travaux effectués dans le cadre de cette thèse visent à proposer de nouvelles sources de supercontinuum émettant des faisceaux optimisés en termes d'élargissement spectral et de densité spectrale de puissance pour la microspectroscopie Multiplex-CARS. Pour ce faire, les moyens de développer des continuums spectraux performants ont été explorés dans trois fibres optiques différentes: une fibre microstructurées air/silice monomode à gros cœur dopé à l'ytterbium permettant une réamplification du signal tout au long de sa propagation ; une fibre monomode conventionnelle en régime de dispersion normale pour obtenir un élargissement spectral par saturation du gain Raman ; une fibre multimode dans laquelle le faisceau spectralement élargi par saturation du gain Raman à très forte puissance subit également un auto-nettoyage spatial par effet Kerr tout au long de sa propagation, produisant en sortie un faisceau de forte brillance dont le profil d’intensité est semblable à celui du mode fondamental. Une étude spectrotemporelle complète est présentée pour ces trois sourcesCoherent Raman microspectroscopy (CARS) is an optical method used to identify molecular bonds in a sample in order to analyze and determine its complete composition. It requires the simultaneous excitation of the sample by two waves (the pump wave and the Stokes wave) in order to induce resonant vibration of the bond to be detected. For multiple bonds analysis (broadband coherent Raman microspectroscopy our Multiplex-CARS), the monochromatic Stokes wave must be replaced by a broadband beam (supercontinuum). The aim of this thesis was to design supercontinuum sources optimized for Multiplex-CARS application, in particular in terms of spectral bandwidth and spectral power density. Supercontinuum generation was investigated in three different optical fibers: (i) a microstructured single mode fiber with a large Yb doped core in which the input beam was re-amplified all along its propagation; (ii) a conventional singlemode fiber pumped in the normal dispersion regime in which spectral broadening was achieved by means of Raman gain saturation; (iii) a conventional graded-index multimode fiber in which the beam spectrally broadened by Raman gain saturation at very high power also experienced spatial self-cleaning by Kerr effect, resulting in a high brillance output beam with an,intensity profile close to that of the fundamental mode. A complete spectrotemporal study is achieved for each of these three sources
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Derbazi, Maqboula. "Étude des caractéristiques Raman et optique non-linéaire des bronzes de tungstène quadratiques (A6M2M’8O30)." Thesis, Reims, 2013. http://www.theses.fr/2013REIMS041.
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Des recherches très importantes ont été dédiées à l'étude des composés ferroélectriques de type bronze de tungstène quadratique (TTB). Cette thèse concerne la synthèse et la caractérisation de 7 matériaux TTB de formule générale A6M2M'8O30 (A = Sr2+, Ba2+ ou Pb2+, M = Ti4+, Zr4+ ou HF4+; M' = Nb5+ ou Ta5+). Ces composés cristallins de grande taille ∼100 nm ont été synthétisés sous forme de poudre. Les moyennes expérimentales : diffractions des rayons X, spectroscopie Raman, la microscopie électronique MEB et MET, l'optique non linéaire ONL, ont permis d'établir des relations étroites entre structure et propriétés physiques. Les susceptibilités optiques non linéaires de 2eme et 3eme ordres, χ(2), χ(3) de chaque composés ont été déterminées et les valeurs résultantes du χ(3) ne montrent pas les mêmes caractéristiques que χ(2), car le signal de THG est moins dépendant de structure que SHG qui requiert un milieu non-centrosymétrique. Le décalage fréquentiel (Δσ) des modes de vibrations entre les structures à base de strontium(Sr) et celles à base de Barium(Ba) a été constaté afin d'identifier les signatures propres de ces composés. L'interprétation de ces poudres n'était pas facile car les pics sont très délicats. Nos mesures expérimentales montrent clairement que les positions des pics peuvent être modifiées par le changement cationique au sein des matériaux, plus la maille cristalline est rigide, plus on a des pics plus discernables. La différence est nettement visible là ou l'émission est autour de 808 cm-1 pour la structure (Sr), alors que pour le (Br) elle est autour de 780cm-1. Nous attribuons ce Δσ (28cm-1) à la transition de groupe de symétrie spatiale de Pba2 vers P4bm. L'ensemble des résultats décrits dans ce travail ont montrés la grande variété des paramètres sur lesquels il est possible d'agir afin d'optimiser les compositions en vue d'une application spécifiqueRecently, very significant research has been devoted to the study of ferroelectric compounds of tetragonal tungsten bronze (TTB). This thesis deals with the synthesis and characterization of 7 TTB's material with general formula A6M2M'8O30 (A = Sr2+, Ba2+ or Pb2+, M = Ti4+, Zr4+ or HF4+, M '= Nb5+ or Ta5+). These crystalline compounds of large size ~ 100 nm were synthesized in powder form. The experimental Technics: X-ray diffraction, Raman spectroscopy, scanning electron microscopy SEM and TEM and nonlinear optics NLO, allowed us to establish close relationships between structure and physical properties. The nonlinear 2nd and 3rd order optical susceptibility χ(2), χ(3) of all compounds were determined and the resulting values of χ(3) did not show the same characteristics as measures of χ(2) because the THG signal is less dependent on the structure where SHG signal requires a non-centro-symmetric medium. The frequency shift between the vibration modes of structures containing strontium (Sr) and those based on Barium (Ba) has been detailed to identify signatures of these specific compounds. The interpretation of these powders wasn't that easy as these peaks are very delicate but our experimental results clearly show that the positions of the peaks can be modified by the change in cation materials, as long as the crystal lattice is more rigid, more we get discernible Raman modes. This difference is clearly visible where the emission is around 808 cm-1 for the structure Sr, whereas the Br it is centered around 780cm-1. We attribute these Δσ (28cm-1) to the transition of spatial symmetry group from Pba2 to P4bm. Results showed the wide variety of settings in which it is possible to act in order to optimize the compositions for a specific application
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Abd, Alrahman Chadi. "Spectroscopie Laser avec des cavités résonantes de haute finesse couplées à un peigne de fréquences : ML-CEAS et vernier effet techniques. Applications à la mesure in situ de molécules réactives dans les domaines UV et visible." Thesis, Grenoble, 2012. http://www.theses.fr/2012GRENY095/document.
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La communauté de la chimie atmosphérique souffre d'un manque de mesures rapides, fiables résolues spatialement et temporellement pour un large éventail de molécules réactives (radicaux tels que NO2, OH, BrO, IO, etc). En raison de leur forte réactivité, ces molécules contrôlent largement la durée de vie et la concentration de nombreuses espèces clés dans l'atmosphère, et peuvent avoir un impact important sur le climat. Les concentrations de ces radicaux sont extrêmement faibles (ppbv ou moins) et très variable dans le temps et dans l'espace, ce qui impose un véritable défi lors de la détection. Dans la première partie de cette thèse, un spectromètre UV robuste, compacte et transportable est développé, exploitant la technique ML-CEAS pour mesurer à des niveaux très faibles (pptv et même en dessous) des molécules réactives d'importance atmosphérique, en particulier, les radicaux d'oxyde d'halogènes, afin de répondre aux besoins émergents. La technique ML-CEAS est basée sur le couplage d'un laser femtoseconde à blocage de modes à une cavité optique de haute finesse, qui agit comme un piège à photons pour augmenter l'interaction entre la lumière et l'échantillon de gaz intracavité. Cela permet d'améliorer fortement la sensibilité d'absorption. La limite de détection obtenue pour le radical IO est de 20 ppqv pour un temps d'acquisition de 5 minutes, ce qui est un résultat impressionnant. Dans la deuxième partie de cette thèse, une nouvelle technique spectroscopique est développée appelée effet Vernier, qui est également basé sur l'interaction entre un laser femtoseconde à blocage de mode et une cavité optique de haute finesse. Cette technique fournit une sensibilité de détection similaire à la technique ML-CEAS, mais l'avantage est que le nombre des éléments spectraux est donné par la finesse de la cavité optique et donc peut atteindre plusieurs dizaines de milliers. De plus, cette configuration simplifie le montage expérimental par la suppression du spectrographe qui est remplacé par une simple photodiode. Le temps d'acquisition d'un spectre peut être aussi réduit à moins d' 1 msThe atmospheric chemistry community suffers a lack of fast, reliable and space resolved measurements for a wide set of reactive molecules (e.g. radicals such as OH, NO3, BrO, IO, etc). Due to their high reactivity, these molecules largely control the lifetime and concentration of numerous key atmospheric species, and may have an important impact on the climate. The concentrations of such radicals are extremely low (ppbv or less) and highly variable in time and space, which imposes a real challenge during the detection. In the first part of this thesis, a compact, robust and transportable UV spectrometer is developed, exploiting the Mode-Locked Cavity Enhanced Absorption Spectroscopy (ML-CEAS) technique to measure pptv and sub-pptv levels of atmospherically important reactive molecules, in particular, halogen oxide radicals, to respond to the emerging needs. The ML-CEAS technique is based on coupling a Mode-Locked femtosecond laser to a high finesse optical cavity, which acts as a photon trap to increase the interaction between the light and the intracavity gas sample, which highly enhances the absorption sensitivity. The detection limit obtained for the IO radical is 20 ppqv (part per quadrillion), which is an impressive result. In the second part of this thesis, a new spectroscopic technique is developed, called Vernier effect, which is also based on the interaction between a mode-locked femtosecond laser with a high finesse optical cavity. This technique provides detection sensitivity similar to that of ML-CEAS technique, but the advantage is that the number of the spectral elements is given by the cavity finesse, so it can reach ten thousands, as well as this technique has a simple setup, where the spectrograph is replaced by a photodiode. Additionally, the time required to measure one output absorption spectrum can be less than 1 ms
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Wetzel, Benjamin. "Etudes expérimentales et numériques des instabilités non-linéaires et des vagues scélérates optiques." Phd thesis, Université de Franche-Comté, 2012. http://tel.archives-ouvertes.fr/tel-01002680.
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Ces travaux de thèse rapportent l'étude des instabilités non-linéaires et des évènements extrêmesse développant lors de la propagation guidée d'un champ électromagnétique au sein de fibresoptiques. Après un succinct rappel des divers processus linéaires et non-linéaires menant à lagénération de super continuum optique, nous montrons que le spectre de celui-ci peut présenterde larges fluctuations, incluant la formation d'événements extrêmes, dont les propriétés statistiqueset l'analogie avec les vagues scélérates hydrodynamiques sont abordées en détail. Nous présentonsune preuve de principe de l'application de ces fluctuations spectrales à la génération de nombres etde marches aléatoires et identifions le phénomène d'instabilité de modulation, ayant lieu lors de laphase initiale d'expansion spectrale du super continuum, comme principale contribution à la formationd'événements extrêmes. Ce mécanisme est étudié numériquement et analytiquement, en considérantune catégorie de solutions exactes de l'équation de Schrödinger non-linéaire présentant descaractéristiques de localisations singulières. Les résultats obtenus sont vérifiés expérimentalement,notamment grâce à un système de caractérisation spectrale en temps réel et à l'utilisation conjointede métriques statistiques innovantes (ex : cartographie de corrélations spectrales). L'excellent accordentre simulations et expériences a permis de valider les prédictions théoriques et d'accéder àune meilleure compréhension des dynamiques complexes inhérentes à la propagation non-linéaired'impulsions optiques.
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Vigouroux, Hélène. "Etude de vitrocéramiques optiques pour le doublement de fréquence." Phd thesis, Université Sciences et Technologies - Bordeaux I, 2012. http://tel.archives-ouvertes.fr/tel-00806577.
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Le développement des lasers de puissance engendre un intérêt pour la recherche de matériaux présentant des propriétés optiques non linéaires (ONL). Les matériaux vitreux sont de très bons candidats puisqu'ils peuvent être transparents et élaborés en grandes dimensions. La précipitation de particules non centro-symétrique dans un verre permet d'engendrer cette propriété en volume, et d'ingérer facilement ce matériau dans les dispositifs lasers. Dans ce contexte, cette thèse présente les résultats obtenus sur la précipitation de la phase LiNO3 dans la matrice vitreuse 35 Li2O- 25 Nb2O5- 40 SiO2. Le mécanisme de cristallisation de cette phase est étudié par analyse thermique, imagerie optique et électronique ainsi que par une analyse in-situ. Ces analyses mettent en évidence une cristallisation sphérolitique du niobate de lithium dans ce verre, conduisant à l'obtention de vitrocéramiques. Les propriétés optiques non linéaires d'ordre deux sont mesurés sur ces matériaux. Un signal original et isotrope de Génération de Second Harmonique a été mesuré. Une analyse multi-échelle permet une meilleure compréhension et une corrélation entre la structure des sphérolites et l'origine de la génération d'un tel signal. Le modèle développé suite à ces analyses permet d'entrevoir le développement de nouveaux matériaux micro-composites à propriétés ONL isotropes.
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Sebastian, Ananthu. "Noise dynamics in multi-Stokes Brillouin laser." Thesis, Rennes 1, 2020. http://www.theses.fr/2020REN1S068.
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La diffusion Brillouin stimulée (SBS) est un processus d'interaction cohérent, pour lequel la lumière est diffusée à partir des ondes acoustiques générées optiquement. Les lasers Brillouin suscitent un très grand intérêt pour leur capacité à produire des largeurs de raie ultra cohérentes. Cette thèse est consacrée à la compréhension des propriétés de bruit des lasers à fibre Brillouin en anneau, fonctionnant avec de multiples ordres de Stokes. Tout d'abord, nous présentons une technique basée sur la méthode de ringdown de la cavité, qui permet de caractériser le coefficient de gain Brillouin directement à partir du sondage de la cavité laser. Ses avantages sont d'obtenir des paramètres à partir d'une seule expérience avec de faibles puissances optiques (quelques 10 milliwatts) pour des cavités courtes (quelques mètres de long, ou cavités intégrées). Deuxièmement, il est démontré qu'une largeur de raie intrinsèque de quelques dizaines de mHz peut être facilement obtenue en cascadant deux lasers Brillouin non résonants (pour lesquels la pompe effectue un seul passage à l'intérieur de la cavité). Afin d'obtenir ces résultats, la stabilité à long terme a été améliorée en utilisant une boucle d'asservissement de type Pound Drever Hall, ce qui nous permet de comparer nos résultats analytiques et expérimentaux. Malheureusement, nous n'avons pas exploré les limites fondamentales de la réduction du bruit en raison du plancher de bruit de notre banc de mesure. Troisièmement, un des travaux majeurs de cette thèse est l'étude analytique et expérimentale des propriétés du bruit, y compris le bruit de fréquence et le bruit relatif d'intensité, d'un laser Brillouin résonant (pour lequel, les ondes de pompe et de Stokes sont résonantes à l'intérieur de la cavité). En particulier, les impacts du facteur de qualité de la cavité fibrée en anneau, le désaccord de gain Brillouin ont été évalués très précisément sur les caractéristiques du RIN du laser telles que la réduction de l'amplitude du bruit et la fréquence de relaxation. Nous soulignons le fait que de nombreuses caractéristiques du bruit de fréquence sont liées aux propriétés du RIN par un couplage entre l'intensité et la phase. Nous montrons que le processus en cascade modifie la dynamique du laser Brillouin par rapport à celle d'un laser Brillouin monomode avec une seule composante de Stokes de premier ordre. Nos résultats expérimentaux sont en excellent accord avec nos simulations, obtenues grâce à notre système non linéaire décrivant le fonctionnement d'un laser Brillouin multi-Stokes. Cette bonne concordance est principalement due à notre capacité : à obtenir des valeurs très précises des paramètres de la cavité et du coefficient de gain Brillouin en utilisant la technique CRDM ; à atteindre une stabilité à long terme (plusieurs dizaines d'heures) ; à contrôler finement le désaccord entre la résonance de Stokes du laser et la fréquence du maximum de gain Brillouin. Nous démontrons expérimentalement pour la première fois que le bruit de fréquence est dégradé en présence d'une diffusion Brillouin anti-Stokes. Nous montrons également qu'un désaccord de gain de l'ordre de quelques centaines de kHz peut dégrader la réduction du bruit d'intensité ou également augmenter la largeur de raie par un couplage amplitude-phase. Toutes ces observations très fines nous permettent donc de fixer les limites fondamentales de tels systèmes laser comme : l'augmentation du bruit due aux ordres anti-Stokes ; le rôle du bruit de pompe et son interrelation possible avec la finesse de la cavité ; l'effet du désaccord inhérent aux ordres de Stokes plus élevés. Toutes ces conclusions sont les clés de la conception et de l'ingénierie de ces lasers à fibre Brillouin, qui suscitent actuellement beaucoup d'intérêt comme en témoignent les travaux en cours dans la communauté scientifique. Cette thèse de doctorat contribue à une meilleure compréhension des lasers Brillouin multi-StokesStimulated Brillouin Scattering (SBS) is a coherent interaction process in which light is scattered from optically generated acoustic waves. It is a powerful tool for microwave and optical signal processing, distributed sensing and spectroscopy. Brillouin lasers are attracting a lot of interest for their ability to produce ultra coherent linewidths. This thesis is devoted to the understanding of noise properties of Brillouin fiber ring lasers, operating with multiple Stokes orders. First, we present a technique based on the cavity ring-down method, which allows to characterize the Brillouin gain coefficient directly from probing the laser cavity. Its advantages are to obtain parameters from a single experiment with low optical powers (some 10 milliwatts) for short cavities (a few meters long, or integrated cavities). Secondly, it is shown that an intrinsic linewidth of a few tens of mHz can be easily obtained by cascading two non-resonant Brillouin lasers (for which the pump performs a single pass inside the cavity). In order to obtain these results, the long-term stability has been improved by using a Pound-Drever-Hall servo loop, which allows us to compare our analytical and experimental results. Unfortunately, we were unable to explore the fundamental limits of noise reduction due to the noise floor of our bench. Thirdly, one of the major works of this thesis is the theoretical and experimental study of the noise properties, including frequency noise and relative intensity noise, of a resonant Brillouin laser (for which pump and Stokes waves are resonant inside the cavity). In particular, the impacts of the fiber-ring-cavity quality factor, Brillouin gain detuning, are evaluated very precisely on the laser RIN features such as amplitude noise reduction and relaxation frequency. We emphasize the fact that many characteristics of the frequency noise are related to the RIN properties by a coupling between intensity and phase. We show that the cascade process modifies the dynamics of the Brillouin laser when compared to those of a single-mode Brillouin laser with a single first-order Stokes component. Our experimental results are in excellent agreement with our numerical simulations, obtained thanks to our non-linear system describing the operation of a multi-Stokes Brillouin laser. This good match is mainly due to our ability: to obtain very precise values of the cavity parameters and the Brillouin gain coefficient using the CRDM technique ; to achieve long-term stability (hours); to finely control the detuning between the laser Stokes resonance and the frequency of the Brillouin gain maximum. We demonstrate experimentally for the first time that frequency noise is degraded in the presence of anti-Stokes Brillouin scattering. We also show that a gain detuning of the order of a few hundred kHz can degrade the intensity noise reduction or also increase the linewidth by amplitude-phase coupling. All these very fine observations thus allow us to set the fundamental limits of such laser systems such as: the increase in noise due to anti-Stokes orders; the role of pump noise and its possible interrelation with cavity finesse; the effect of the detuning inherent to higher Stokes orders. All these conclusions are key to the design and engineering of these Brillouin fiber lasers, which are currently attracting a great deal of interest as evidenced by the work in progress in the scientific community. This PhD thesis contributes to a better understanding of multi-Stokes Brillouin lasers
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Liu, Yu-Mei, and 劉玉美. "Studies of Nonlinear Optics and Spectroscopy." Thesis, 1993. http://ndltd.ncl.edu.tw/handle/15263895012306776664.
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