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1
Petrović, Vladimir 1978. "Toward pure electronic spectroscopy". Thesis, Massachusetts Institute of Technology, 2008. http://hdl.handle.net/1721.1/46647.
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Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2009.Vita.
Includes bibliographical references.
In this thesis is summarized the progress toward completing our understanding of the Rydberg system of CaF and developing Pure Electronic Spectroscopy. The Rydberg system of CaF possesses a paradigmatic character due to its strongly polar ion-core. The first characterization of the Stark effect in a Rydberg system of this nature is presented here, and a diagnostic application of the Stark effect for making assignments of N+ and f quantum numbers has been demonstrated. In addition, a general method, which relies on polarization diagnostics and is applicable not only to studies of Rydberg states, for making unambiguous rotational assignments in the absence of rotational combination differences, has been described for the case of unresolved doublet states. New information, obtained using the Stark effect and polarization diagnostics, has furthered our knowledge of the partially core-penetrating character of nominally core-nonpenetrating states. In order to systematically obtain the same information that is contained in a Stark effect spectrum, but with less difficulty, we are developing experimental methods to record same-n* Rydberg-Rydberg transitions directly, using Time Domain THz and Chirped-Pulse Microwave Spectroscopies. In both of these methods, the spectrum is recorded in the time domain, which results in reliable relative transition intensities. We show that the relative transition intensities in a Rydberg-Rydberg spectrum provide information that permits separation of different interaction mechanisms between the Rydberg electron and the ion-core.
by Vladimir Petrović.
Ph.D.
2
Yang, Min-Chieh. "Electronic spectroscopy of transient molecules /". The Ohio State University, 1998. http://rave.ohiolink.edu/etdc/view?acc_num=osu1487949508372826.
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Bonifas, Andrew Paul. "Spectroscopy, Fabrication, and Electronic Characterization of Molecular Electronic Devices". The Ohio State University, 2011. http://rave.ohiolink.edu/etdc/view?acc_num=osu1305653420.
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Al, Sawi A. N. "Study of the electronic structure of InSb by electron spectroscopy". Thesis, University of Liverpool, 2017. http://livrepository.liverpool.ac.uk/3007631/.
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Ye, Jianjun. "Electronic spectroscopy of transition metal monohalides". Click to view the E-thesis via HKUTO, 2007. http://sunzi.lib.hku.hk/hkuto/record/B38990167.
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陳文端 i Man-tuen Chan. "Electronic spectroscopy of OH and ZrN". Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 1997. http://hub.hku.hk/bib/B31235578.
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Qian, Yue, i 钱玥. "Electronic spectroscopy of transition metal dimer". Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 2013. http://hub.hku.hk/bib/B50899971.
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This thesis reports laser spectroscopic studies of gas-phase transition metal dimers using laser ablation/reaction with free jet expansion and laser-induced fluorescence (LIF) spectroscopy technique. Themolecules studied in this work are palladium dimer (Pd2) and vanadium dimer (V2). Many compounds formed from these transition metals are important and functional catalysts in chemical reactions. Therefore, it is of great significance to start from the fundamental level to understand the properties and characteristics of the metal bonding and also the behavior of these metals when reacting with other chemicals.
The electronic transitions of Pd2and V2in the visible region were studied. Gas-phase Pd2and V2moleculeswereproduced by laser ablation of palladium and vanadium metal rod, respectively. For the Pd2molecule, eleven vibrational bands were recorded and analyzed, and have been assigned to the 〖[17.1]〗^3 □_g□ X^3 □_u^+ transition system. The bond length and vibrational frequency of the ground X^3 □_u^+ state were determined to be 2.47 Å and 211.38 cm-1, respectively. This is the first experimental investigation of the electronic transitions of Pd2.For the V2molecule,six vibrational bands were observed and assigned to a new 〖[19.6] 〗^3 □_u^□□ X^3 □_g^□ transition system. Molecular constants for the 〖[19.6] 〗^3 □_u^□ excited state were obtained from high-resolution LIF spectra. The electronic structure of the Pd2andV2molecules was discussed in detail using molecular orbital energy level diagrams, which is important for understanding the nature of chemical bonding in these dimers. Comparison of the transition metal dimers studied in this work with other dimers is also presented.published_or_final_version
Chemistry
Master
Master of Philosophy
8
Wattanavichean, N. "Raman spectroscopy of molecular electronic junctions". Thesis, University of Liverpool, 2017. http://livrepository.liverpool.ac.uk/3006908/.
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Molecular Electronics uses molecules sandwiched between two metals as a model system to create tailored solutions for applications such as energy harvesting and sensing. Electrons tunnelling across such a junction are a↵ected by the properties of the molecule itself as well as the interaction between metal and molecule. In particular, charge transport is known to couple to molecular vibrations, which can act both to dissipate energy as well as increase conductance. This thesis therefore applies in-situ vibrational spectroscopies, surface-enhanced Raman scattering and vibrational sum frequency generation, to investigate molecular junctions. As a model system, 4-mercaptopyridine sandwiched between a gold surface and an elec- trochemically deposited second metal layer is used. Four aspects are studied in detail in this thesis. Chapter 3 presents a detailed study of surface enhanced Raman spectra of 4-mercaptopyridine on gold. All experimental vibrational modes are assigned and related to the symmetry of the adsorbed molecule with the help of density functional calculations. In particular, the e↵ect of hydrogen bonding on the ring breathing modes of adsorbed mercaptopyridine is revealed for the first time. In chapter 4, surface-enhanced Raman spectroscopy is used to identify a spectroscopic signature of a successfully formed metal-molecule-metal junction after electrochemical deposition of a tran- sition metal layer. Chapter 5 then addresses the use of surface-enhanced Raman spectroscopy to identify charge transfer states of 4-mercaptopyridine by changing bias potential and excitation wavelength. A charge transfer state is found for protonated 4-mercaptopyridine at about 1.7 eV above the Fermi level, while the corresponding state for unprotonated 4-mercaptopyridine must lie at least 0.8 eV higher. Chapter 6 then explores the use of ultrafast vibrational sum frequency generation. The pyridine ring stretching modes are detected and metallisation of the 4-mercaptopyridine layer is seen to decrease the local order of the molecular layer. The influence of the mercaptopyridine charge transfer state can be seen in ultrafast pump - sum frequency probe spectroscopy of the gold substrate. This opens the prospect of investigating coupling between molecular vibrations and charge transfer in these junctions on a timescale of a picosecond or less.
9
Chan, Man-tuen. "Electronic spectroscopy of OH and ZrN /". Hong Kong : University of Hong Kong, 1997. http://sunzi.lib.hku.hk/hkuto/record.jsp?B18736361.
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Gopalakrishnan, Sandhya. "Electronic spectroscopy of the alkoxy radicals". Columbus, OH : Ohio State University, 2003. http://rave.ohiolink.edu/etdc/view?acc%5Fnum=osu1051024461.
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Thesis (Ph. D.)--Ohio State University, 2003.Title from first page of PDF file. Document formatted into pages; contains xxiv, 173 p.: ill. (some co.). Includes abstract and vita. Advisor: Terry A. Miller, Dept. of Chemistry. Includes bibliographical references (p. 171-173).
11
Ji, Tao. "Inelastic electron tunneling spectroscopy in molecular electronic devices from first-principles". Thesis, McGill University, 2011. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=96883.
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In this thesis, we present the first-principle calculations of inelastic electron tunneling spectroscopy(IETS) in single molecular break junctions. In a two-probe electrode-molecule-electrode setup, density functional theory(DFT) is used for the construction of the Hamiltonian and the Keldysh non-equilibrium Green's function(NEGF) technique will be employed for determining the electron density in non-equilibrium system conditions. Total energy functional, atomic forces and Hessian matrix can be obtained in the DFT-NEGF formalism and self-consistent Born approximation(SCBA) is used to integrate the molecular vibrations (phonons) into the framework once the phonon spectra and eigenvectors are calculated from the dynamic matrix. Geometry optimization schemes will also be discussed as an indispensable part of the formalism as the equilibrium condition is crucial to correctly calculate the phonon properties of the system.To overcome the numerical difficulties, especially the large computational time demand of the electron-phonon coupling problem, we develop a numerical approximation for the electron self-energy due to phonons and the error is controlled within numerical precision. Besides, a direct IETS second order I-V derivative expression is derived to reduce the error of numerical differentiation under reasonable assumptions. These two approximations greatly reduce the computation requirement and make the calculation feasible within current numerical capability.As the application of the DFT-NEGF-SCBA formalism, we calculate the IETS of the gold-octanedithiol(ODT) molecular junction. The I-V curve, conductance and IETS from ab-inito calculations are compared directly to experiments. A microscopic understanding of the electron-phonon coupling mechanism in the molecular tunneling junctions is explained in this example. In addition, comparisons of the hydrogen-dissociative and hydrogen-non-dissociative ODT junctions as well as the different charge transfer behaviors are presented to show the effects of thiol formation in the ODT molecular junction.Dans cette thèse, nous présentons des calculs ab initio de la spectroscopie à effet tunnel par électron inélastique (IETS)appliqués à des jonctions moléculaires. Dans le cadre d'une configuration électrode-molécule-électrode,la théorie de la fonctionnelle de la densité (DFT) est utilisée pour construire l'hamiltonien et les fonctions de Green hors-équilibres(NEGF) sont employées pour déterminer la densité électroniquedans des conditions hors-équilibre. Le cadrede la DFT-NEGF nous permet de calculer des quantités telles que la fonctionnelle d'énergie totale,les forces atomiques ainsi que la matrice de Hessian. L'approximationauto-consistante de Born (SCBA) est employée afin d'intégrer les vibrations moléculaires (phonons) dans le formalisme DFT-NEGF,une fois que le spectre des phonons et les vecteurs propres ont été calculés à partir de la matrice dynamique. Des méthodes d'optimisations géométriques sont aussi discutées en tant que part indispensable du formalisme,étant donné que la condition d'équilibre mécanique est essentielle afin de calculer correctement les propriétés des phonons du système.Afin de surmonter les difficultés numériques, particulièrement concernant la grande demandecomputationnelle requise pour le calcul du couplage électron-phonon, nous développons une approximation numérique pour la self-énergie associée aux phonons. De plus, en employant quelques hypothèses raisonables, nous dérivons une expression pour l'IETS calculée à partir de laseconde dérivée de la courbe I-V dans le butde réduire l'erreur associée à la différentiation numérique. L'utilisation de ces deux approximations diminuent grandement les exigences computationnelles et rendent les calculs possibles avec les capacités numériques actuelles.Comme application du formalisme DFT-NEGF-SCBA, nous calculons l'IETS de la jonction moléculaire or-octanedithiol(ODT)-or. La courbe I-V, la conductance et l'IETS obtenues par calculs ab initio sontdirectement comparées aux données expérimentales. Une compréhension microscopique du couplage électron-phonon pour une jonction moléculaire à effet tunnel est élaborée dans cet exemple. De plus, des comparaisons entre les jonctions ODT à hydrogène dissociatif et à hydrogène non-dissociatif ainsi queles différents comportements de transfert de charges sont présentés afin de montrer les effets de la formation du thiol dans la jonction moléculaire ODT.
12
Kemp, Jeremy. "Electron spectroscopy and electronic structure of first row transition metal oxides". Thesis, University of Oxford, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.257736.
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Dunkelberger, Adam David. "Time-resolved electronic spectroscopy of 2,2'-bisindene". Connect to resource, 2007. http://hdl.handle.net/1811/28440.
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Thesis (Honors)--Ohio State University, 2007.Title from first page of PDF file. Document formatted into pages: contains 35 p.; also includes graphics. Includes bibliographical references (p.35). Available online via Ohio State University's Knowledge Bank.
14
Brocke, Thomas. "Electronic Raman spectroscopy on semiconductor quantum dots". Göttingen Cuvillier, 2007.
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Dickinson, John Andrew. "Electronic spectroscopy and conformations of aromatic systems". Thesis, University of Oxford, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.363668.
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Pang, Hon-fung, i 彭漢鋒. "Electronic spectroscopy of iridium containing diatomic molecules". Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 2012. http://hub.hku.hk/bib/B47164220.
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This thesis reports the study of molecular and electronic structure of iridium containing diatomic molecules using the technique of laser ablation/reaction with free jet expansion and laser induced fluorescence (LIF) spectroscopy. The iridium containing diatomic molecules studied in this research are iridium phosphide (IrP), iridium boride (IrB) and iridium oxide (IrO). These molecules were produced by the reaction of Ir atoms ablated by a pulsed neodymium-doped yttrium aluminium garnet (Nd:YAG) laser and 1% PH3, 0.5% B2H6 and 6% N2O gases to produce IrP, IrB and IrO molecules respectively. Pulsed tunable lasers: a dye laser and an optical parametric oscillator (OPO) laser system were used to cover the spectral region between 390 and 650 nm in obtaining electronic transitions of the iridium containing diatomic molecules.
The recorded electronic spectra of IrP, IrB and IrO molecules yields information on the bond length and electronic structures. For the IrP molecule, five electronic transitions, namely the [21.2] 3Σ+ – X1Σ+, [21.7]1Σ+ – X1Σ+, [23.6] 0+ – X1Σ+, [23.7] 0+ – X1Σ+ and [23.9] 0+ – X1Σ+ transitions, have been recorded and analyzed. The bond length, r0, and the ΔG1/2 of the ground state of 193IrP molecule was determined to be 1.9928? and 569.77 cm-1 respectively. For the IrB molecule, four new electronic transition systems, namely the [18.8]3Δ3 – X3Δ3, [21.1]3Φ4 – X3Δ3, [22.8]3Φ3 – X3Δ3 and [22.4]1Φ3 – a1Δ2 transitions, were observed and analyzed rotationally. The bond lengths, r0, of the upper states of 193IrB were determined to be within 1.72 and 1.80?. For the IrO molecule, five electronic transitions from two different lower states were recorded and analyzed, namely the [17.6] 2.5 – X2Δ5/2, [17.8] 2.5 – X2Δ5/2, [21.5] 2.5 – X2Δ5/2, [22.0] 2.5 – X2Δ5/2 and [21.9] 3.5 – Ω = 3.5 transitions. The ground state of IrO has been confirmed to be 25/2. The bond length, r0, and the ΔG1/2 of the ground state of 193IrO molecule was determined to be 1.726 A and 900.00 cm-1 respectively. For all the transitions observed, rotationally-resolved transition lines were fit to theoretical models to obtain molecular constants for both the upper and lower electronic states. Typical molecular transition linewidths obtained was larger than 0.1cm-1, which is likely to be due to unresolved hyperfine structure in the rotational lines. In addition, the observation of isotopic spectrum confirmed the assignment of vibrational quantum number. Molecular and electronic structures of these iridium containing diatomic molecules were discussed using a simple molecular orbital theory.published_or_final_version
Chemistry
Doctoral
Doctor of Philosophy
17
Elliott, Nicola Louise. "High resolution electronic spectroscopy of transient species". Thesis, University of Bristol, 2007. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.443268.
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Elks, John Marcus Francis. "High resolution electronic spectroscopy of transient species". Thesis, University of Bristol, 2001. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.390790.
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Zhang, Xu Ph D. Massachusetts Institute of Technology. "Two-dimensional crystals : spectroscopy and electronic applications". Thesis, Massachusetts Institute of Technology, 2017. http://hdl.handle.net/1721.1/112036.
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Thesis: Ph. D., Massachusetts Institute of Technology, Department of Electrical Engineering and Computer Science, 2017.Cataloged from PDF version of thesis.
Includes bibliographical references (pages 159-177).
The success in creating atomically thin and mechanically robust two-dimensional (2D) crystals, starting with graphene, has unveiled new possibilities for next generation of ultrafast and ubiquitous electronics. One critical distinction between 2D crystals and 3D crystals is that 2D crystals are all-surface materials. Therefore, it is essential to understand how 2D materials interact with their environments and how this interaction impacts their electronic properties. From a practical perspective, it also provides us with a unique tool to tailor the electronic properties of 2D materials through surface functionalization. In the first half of this thesis, a suite of X-ray techniques is used to investigate how the surface functionalizing dopants will impact the electronic and chemical states of graphene. Based on this study, we develop an effective and non-invasive doping method for graphene through plasma-based chlorination. In order to make system-level 2D electronics successful, a flexible and ubiquitous energy harvesting solution is indispensable. Therefore, the second part of this thesis is dedicated to the development of a MoS₂ 2H-1T phase heterojunction-based GHz flexible rectifier as an enabling component for wireless energy harvester. It is the first flexible rectifier operating up to the X-band and it covers most of the unlicensed industrial, scientific and medical (ISM) radio band, including the Wi-Fi channels. By integrating this rectifier with an antenna, the MoS₂-enabled rectenna successfully demonstrates direct energy harvesting of electromagnetic (EM) radiation in the Wi-Fi band and lights up a commercial light-emitting diode (LED) with zero external bias (battery-free). Moreover, our MoS₂ rectifier also realizes successful frequency conversion as a mixer beyond 10 GHz on flexible substrates. This work provides a universal energy harvesting building block that can be integrated with various wearable electronic systems and paves the way towards using the existing Wi-Fi infrastructure as an energy hotspot for wireless charging.
by Xu Zhang.
Ph. D.
20
Chan, Mau Hing. "Photothermal deflection spectroscopy of novel electronic materials". HKBU Institutional Repository, 1996. http://repository.hkbu.edu.hk/etd_ra/66.
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Culberson, Lori. "Molecular Electronic Structure via Photoelectron Imaging Spectroscopy". Diss., The University of Arizona, 2013. http://hdl.handle.net/10150/301677.
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This dissertation explores the use of photoelectron imaging spectrometry to probe the molecular electronic structure of various chemical systems, with an emphasis on photoelectron angular distributions. Experimental ion generation, mass selection, laser photodetachment, and photoelectron ion imaging were all done in a photoelectron imaging spectrometer described in detail. Results from simplistic systems, OH- and CH-, are used to illustrate the general and fundamental capabilities of imaging spectroscopy and angular distributions. This illustration is then expanded when both qualitative and quantitative analyses of photoelectron angular distributions are used to aid in the understanding of the electronic structure of several heterocyclic aromatic systems. First a qualitative analysis aids in the exploration of the electronic structure of thiophenide, C₄H₃S⁻, and furanide, C₄H₃O⁻. Ground and excited C₄H₃S and C₄H₃O radical states are observed, and bond dissociation energies are defined. Next, a new model used to qualitatively analyze photoelectron angular distributions resulting from mixed s - p hybrid states is presented and applied to detachment from pyridinide, C₅H₄N⁻; as a benchmark system. Before further exploring this model, the synthesis of several deuterated heterocyclic compounds is presented in order to determine the experimentally produced systems in our experimental setup. The electronic structure of the resultant molecules oxazolide, C₃H₂NO⁻, and thiazolide, C₃H₂NS⁻; are then investigated. Using this new qualitative model, the mixed s - p states model, to evaluate the angular distributions of the systems, the hybridization of the anion molecular orbitals is probed. Comparison of the photoelectron angular distributions that are modeled for each heterocyclic aromatic system yields several trends relating aromatic stabilization, molecular hybridization, and bond dissociation energies. A new qualitative model is then presented to evaluate photoelectron angular distributions resulting from mixed p - d states and applied to detachment from NO⁻. Finally, new ideas and directions are proposed.
22
Volpato, Andrea. "Innovative Strategies in Coherent Multidimensional Electronic Spectroscopy". Doctoral thesis, Università degli studi di Padova, 2017. http://hdl.handle.net/11577/3425369.
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Recent experimental evidences of long-lived quantum electronic coherences in photosynthetic systems have focused the attention on the possible role of quantum phenomena in enhancing biologically relevant functions and the performance of man-made energy devices.
Two-dimensional electronic spectroscopy (2DES) provided several compelling evidences that sparked the discussion, but we are far from achieving clear statements.
The technique is little more than a decade old and active research is progressing on setup development and data-analysis procedures.
A high-performance setup has been built and advanced calibration procedure and acquisition schemes have been designed, in order to tackle the challenges of current instrumental implementations.
Time-frequency decomposition techniques, borrowed from the signal-processing field, have been adapted and applied to the analysis of 2DES coherent oscillating signals. Moreover, a global analysis method based on the variable projection algorithm has been developed for robust and quantitative analysis of coherence signatures. The dynamics of the relevant beating components is resolved with unmatched clarity, supplying a valuable help in their interpretation.
An oligomeric porphyrin based model system has been investigated with the developed tools. Vibrational coherences with drastically different behaviors have been analyzed bringing out the role of the disorder in modulating the coherent dynamics.La recente osservazione di coerenze quantistiche elettroniche con lunga durata in sistemi fotosintetici ha stimolato l’interesse sul possibile ruolo dei fenomeni quantistici nel migliorare alcune funzioni di rilevanza biologica e nell'aumentare le prestazioni di dispositivi artificiali. Tale interesse è stato supportato da numerose evidenze sperimentali fornite dalla spettroscopia bidimensionale elettronica (2DES) ma la ricerca in questo ambito è ancora lontana dal raggiungere conclusioni definitive. La tecnica 2DES è nata da poco più di un decennio ed è ancora molto attiva la ricerca per lo sviluppo di un apparato strumentale ottimale e di efficienti metodi di elaborazione dati. Nell'ambito del progetto di dottorato, è stato costruito un setup sperimentale ad alte prestazioni accoppiato con avanzate procedure di calibrazione e di acquisizione dati, affrontando le sfide principali delle attuali implementazioni strumentali. Attingendo dal campo ingegneristico dell’elaborazione dei segnali, le tecniche di decomposizione tempo-frequenza sono state applicate allo studio di segnali oscillanti 2DES. Inoltre, un metodo di analisi globale basato sul variable projection algorithm è stato sviluppato, allo scopo di avere uno strumento robusto e quantitativo per lo studio dei responsi coerenti. La definizione della dinamica delle componenti oscillanti si è dimostrata un valido strumento per l’interpretazione del dato sperimentale. I metodi sviluppati sono stati utilizzati per l'analisi dei dati sperimentali ottenuti con un sistema modello costituito da un oligomero con catene laterali porfiriniche. Sono state analizzate coerenze vibrazionali con caratteristiche differenti evidenziando l’influenza del disordine nel modulare la risposta coerente.
23
Wright, Helen Elizabeth. "Studies of the electronic structure of metals and alloys by electron spectroscopy". Thesis, University of Liverpool, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.329397.
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Newell, Mark Alistair. "Physical and electronic structure of simple metal systems studied by electron spectroscopy". Thesis, University of Liverpool, 1992. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.333499.
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Rafferty, Brian Edward. "Probing electronic structure near the bandgap region using electron energy loss spectroscopy". Thesis, University of Cambridge, 1997. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.627334.
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Roth, Friedrich. "Electronic structure of selected aromatic hydrocarbon systems investigated with electron energy-loss spectroscopy". Doctoral thesis, Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden, 2013. http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-106800.
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Organic materials with fascinating/intriguing electronic properties have been the driving force for many research activities in the past, and in particular for important progress in materials science covering both new functional materials as well as theoretical developments. In addition, charge transfer, i. e., the addition or removal of charges to or from molecules in organic solids is one route to modify and control their electronic properties. Recently, the discovery of superconductivity in several alkali metal intercalated hydrocarbon systems (picene, phenanthrene, coronene and 1,2;8,9-dibenzopentacene) with rather high transition temperatures has opened a new chapter in organic material science as well as solid-state physics.
The search for a microscopic understanding of the mechanism that drives materials superconducting always has initiated a large number of scientific activities, and there are numerous examples where these activities have provided major advancement. A basic foundation of this understanding is the knowledge of the electronic properties of the material under investigation.
In this context, this thesis reports first, very detailed insight into the electronic structure of both undoped as well as potassium doped picene, coronene and 1,2;8,9-dibenzopentacene using electron energy-loss spectroscopy (EELS) as main experimental method. Additionally, also photoemission spectroscopy experiments have been performed to investigate the occupied electronic density of states close to the chemical potential. In order to learn more about the electronic structure we have compared the results we obtained from EELS and photoemission spectroscopy with theoretical calculations based on Density functional theory (DFT) using the local-density approximation (LDA).
We identify the peculiar case of very close lying conduction bands that upon doping harbour the electrons that form the Cooper-pairs in the superconducting state. Moreover, the presented data display substantial changes in the electronic excitation spectrum upon doping, whereas in the doped case the appearance of one new peak (for picene) and several new peaks (for coronene and 1,2;8,9-dibenzopentacene) in the former optical gap is reported. By using a Kramers–Kronig analysis (KKA) it is possible to gain information about the nature of this doping introduced excitations. In particular, in case of picene, the new low energy feature can be assigned to a charge carrier plasmon. Interestingly, this plasmon disperses negatively upon increasing momentum transfer, which deviates significantly from the traditional picture of metals based on the homogeneous electron gas. The comparison with calculations of the loss function of potassium intercalated picene shows how this finding is the result of the competition between metallicity and electronic localization on the molecular units.
Furthermore, core level excitation measurements show the reduction of the lowest lying C 1s excitation feature, which clearly demonstrates that potassium intercalation leads to a filling of the conduction bands with electrons. Additionally, the measurements of potassium intercalated 1,2;8,9-dibenzopentacene clearly indicate the formation of particular doped phases with compositions K_xdibenzopentacene (x = 1, 2, 3), whereas the data suggest that K_1dibenzopentacene has an insulating ground state with an energy gap of about 0.9 eV, while K_2dibenzopentacene and K_3dibenzopentacene might well be metallic, because of the absent of an energy gap in the electronic excitation spectra.
Interestingly, a comparison of the photoemission as well as EELS spectra of undoped 1,2;8,9-dibenzopentacene and pentacene reveal that the electronic states close to the Fermi level and the electronic excitation spectra of the two materials are extremely similar, which is due to the fact, that the additional two benzene rings in 1,2;8,9-dibenzopentacene virtually do not contribute to the delocalized pi molecular orbitals close to the Fermi level. This close electronic similarity is in contrast to the behavior upon potassium doping, where evidence for a Mott state has been reported in the case of pentacene.
A comparison of the low energy excitation spectra of chrysene with picene (phenacenes) as well as tetracene with pentacene (acenes) crystals reveal a significant difference between the former and the latter two materials. While for the phenacenes (zigzag arrangement) the excitation onset is characterized by up to five weak excitation features with only small anisotropy and without visible Davydov splitting within the a*, b*-planes, the acene (linear arrangement) spectra are dominated by a large excitation close to the onset and a sizable Davydov splitting. The presented data show further that the spectral shape of the pentacene excitation spectrum provides clear evidence for a large admixture of molecular Frenkel-type excitons with charge-transfer excitations resulting in excited states with a significantly mixed character. This conclusion is in good agreement with recent advanced calculations which predicted a charge-transfer admixture to the lowest singlet excitation which is significantly dependent upon the length of the acene molecules. Moreover, also for picene and chrysene we observe differences which point towards an increased charge-transfer contribution to the singlet excitation spectrum in the former.
Finally, investigations of the electronic properties of undoped and potassium doped chrysene, a close relative of picene, show that the doping introduced changes are in a similar range such as observed in case of picene. Interestingly, due to the analogy between the observed changes in the electronic structure upon potassium doping between chrysene and picene and further similarity in the crystal structure we speculate that chrysene is a promising candidate for another aromatic hydrocabon superconductor.
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Menon, Nanda. "A study of electronic structure anisotropy by spatially resolved electron energy loss spectroscopy". Thesis, University of Cambridge, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.624123.
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Zhang, Guowei. "Electronic structure of quasicrystals studied by photoemission spectroscopy". Thesis, University of Ottawa (Canada), 1996. http://hdl.handle.net/10393/9559.
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To investigate the electronic structure of the high-quality quasicrystals, photoemission spectroscopy measurements have been carried out using synchrotron radiation source in the photo-energy range 35-150 eV. The studied quasicrystals are icosahedral Al$\rm\sb{70}Pd\sb{20}Mn\sb ,\ Al\sb{65}Cu\sb{20}Os\sb ,$ and $\rm Al\sb{65}Cu\sb{20}Ru\sb ,$ and decagonal $\rm Al\sb{65}Co\sb Cu\sb{20}$ and $\rm Al\sb{70}Co\sb Ni\sb .$ Resonance photoemission near the transition from the shallow core levels to the d valence bands has been employed to show that the feature close to the Fermi level in the valence bands is predominantly due to the d electron states in the nearly-half-full subshells (Mn, Fe, Ru, Os). The feature farther from the Fermi level has been identified as being mainly due to the d electron states in the full d subshells (Pd, Cu). In some cases, the experimental partial densities of states have been obtained by taking advantage of the synchrotron-radiation-based photoemission technique and the large changes in the cross sections. The as-measured valence-band spectra were corrected for the experimental parameters and the background in order to make a meaningful comparison between the spectra. The high energy-resolution ultraviolet photoelectron spectroscopy measurements on icosahedral $\rm Al\sb{65}Cu\sb{20}Fe\sb{7.5}Ru\sb{7.5}$ prove that there is a pseudogap from the d electrons close to the Fermi level. The studied samples were characterized by the X-ray diffraction and the diffraction patterns were indexed based on several indexing schemes. A description of the indexing procedures is presented. The experimental results of this work are related to the theoretical predictions of a pseudogap and spikiness in the density of states. The unusual behavior of the resistivity of the quasicrystals is interpreted in terms of disorder and other relevant theories.
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Pooley, Simon Jonathan. "Electronic spectroscopy of some metal-containing free-radicals". Thesis, University of Leicester, 1998. http://hdl.handle.net/2381/30023.
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Laser-induced fluorescence (LIF) spectroscopy has been used to probe the properties of some metal-containing free-radicals. These radicals were formed using three different techniques; fragmentation through electric discharge, laser ablation and laser photolysis and were studied in a supersonic jet expansion. A dispersed fluorescence spectroscopic study of the zinc-monoethyl free radical was performed. From this work vibrational frequencies, particularly of the Zn-C stretching and the Zn-C-C bending modes, have determined for both the X˜ and A states. In addition several peaks in the excitation spectrum reported by Povey et al. (22500--24000 cm-1) have been assigned. Recently Professor T.A. Miller and co-workers at Ohio State University recorded rotationally-resolved LIF spectra of ZnC2H5 in the 22500--23100 cm-1 region. This study complemented the dispersed fluorescence work described above, so the author was asked to generate a model and interpret this spectra. A Hamiltonian model to simulate rotational structure of asymmetric top molecules which includes spin-rotation terms has been written by the author to form part of a spectral simulation program. This program was used to simulate the rotationally resolved LIF spectra of ZnC2H5 detailed above. Unfortunately a complete analysis has not been possible but values for the A, B and C rotational constants for many of the bands are presented here along with a analysis of the observed values of spin-rotation constants. Finally, LIF spectra of a new electronic transition of BaOH, the D˜2sum+ - X 2sum+ system has been observed. Also, the C˜ - X˜ system was reinvestigated. The C˜ - X˜ system is particularly interesting because it shows much more complexity than might be expected from previous studies. Vibrationally and partially rotationally resolved spectra are reported for both systems and the C˜ - X˜ region offers some evidence that the molecule may be bent in the excited state with a large spin-rotation interaction coupling.
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Bieske, Evan John, i n/a. "The Electronic Spectroscopy of Neutral and Ionic Clusters". Griffith University. School of Science, 1989. http://www4.gu.edu.au:8080/adt-root/public/adt-QGU20051109.112502.
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This thesis is concerned with weakly bound neutral and ionic clusters. Spectra of the region near the S1fS0 electronic origin of four neutral van der Waals molecules - aniline-argon, phenol-argon, chlorobenzene-argon and fluorobenzene-argon - were obtained using resonance enhanced multiphoton ionization (REMPI). These spectra indicate that Fermi resonances between van der Waals stretching and bending motions are important in these molecules. Effective Hamiltonians are constructed that describe well the low frequency vibrations. In order to better discuss the low frequency van der Waals motions of aromatics bound to one and two rare gas atoms a simple model for the vibrations is developed. The model enables expression of van der Waals frequencies in terms of fundamental molecular properties and enables facile comparison of effective force constants in a variety of van der Waals molecules. The model is successfully employed to explain van der Waals vibrational structure associated with the origin region of aniline-(argon)2 using van der Waals potential parameters derived from the aniline-(argon)1 spectrum. REMPI and emission spectra of larger clusters of aniline and argon are also reported and discussed. Using atom-atom potentials, equilibrium structures for aniline-(argon)n (n=l, 2, 3) are calculated. The calculations prove useful in the analysis of the spectra.The BfX transitions of the cation complexes fluorobenzene+-argon and chlorobenzene+-argon have been investigated. The cations were prepared by resonance enhanced multiphoton ionization of the neutral van der Waals molecules. A time delayed tunable dye laser was then used to dissociate the cations, loss of an argon atom being the dominant process. When the second laser was tuned to a cation resonance the dissociation cross section increased markedly, allowing characterization of BfX transition. The resulting spectra are presented and discussed.
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Lakin, Nicholas Mark. "Electronic and microwave spectroscopy of indium(I) hydroxide". Thesis, University of Oxford, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.259963.
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Ashworth, Stephen Hugh. "The high resolution electronic spectroscopy of nickel dichloride". Thesis, University of Oxford, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.302831.
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Wong, Lai Ally, i 王麗. "Electronic spectroscopy of cobalt monohalides and nitric oxide". Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 2003. http://hub.hku.hk/bib/B29468127.
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Tuttle, William Duncan. "Electronic and photoelectron spectroscopy of substituted benzene molecules". Thesis, University of Nottingham, 2018. http://eprints.nottingham.ac.uk/54244/.
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Intramolecular vibrational redistribution (IVR) has long been investigated in para-fluorotoluene (pFT), with many comparisons made to para-difluorobenzene (pDFB). These comparisons have shown an increased IVR rate for pFT compared to pDFB at similar internal energies, and there are two factors which could influence this - the addition of the methyl group and the lowering of the symmetry of the molecule. This thesis looks to separate these two effects by introducing a comparison of pFT to para-chlorofluorobenzene, as well as an additional comparison of para-xylene (pXyl) to pDFB. Resonance-enhanced multiphoton ionisation (REMPI) spectra of these four molecules are presented, with zero-electron-kinetic-energy (ZEKE) photoelectron spectra recorded via many intermediate levels up to ~00+1200 cm-1 for both pFT and pXyl. These ZEKE spectra allow the assignment of many torsional, vibrational and vibration-torsion levels in these two molecules, with pXyl treated with the appropriate G72 molecular symmetry group for the first time. Several reassignments, as well as many new assignments, are presented for pFT and pXyl. Use of the REMPI and ZEKE techniques allows for the probing of any couplings between levels in the S1 state, as well as providing ground state cation information, and this is supplemented by comparison of REMPI activity between the four para-disubstituted benzene molecules. Proposed couplings, which appear to become more widespread at higher internal energies, are supported by density of states calculations, and a discussion of the influence of both the methyl group and the molecular symmetry on the couplings is presented.
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Robles, Eric San Jose. "Electronic spectroscopy of jet-cooled organometallic free radicals /". The Ohio State University, 1992. http://rave.ohiolink.edu/etdc/view?acc_num=osu1487776801323524.
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Toyota, Kazuo. "Electronic theory for spectroscopy and molecular force field". 京都大学 (Kyoto University), 2002. http://hdl.handle.net/2433/149820.
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Bieske, Evan John. "The Electronic Spectroscopy of Neutral and Ionic Clusters". Thesis, Griffith University, 1989. http://hdl.handle.net/10072/367202.
Pełny tekst źródłaStreszczenie:
This thesis is concerned with weakly bound neutral and ionic clusters. Spectra of the region near the S1fS0 electronic origin of four neutral van der Waals molecules - aniline-argon, phenol-argon, chlorobenzene-argon and fluorobenzene-argon - were obtained using resonance enhanced multiphoton ionization (REMPI). These spectra indicate that Fermi resonances between van der Waals stretching and bending motions are important in these molecules. Effective Hamiltonians are constructed that describe well the low frequency vibrations. In order to better discuss the low frequency van der Waals motions of aromatics bound to one and two rare gas atoms a simple model for the vibrations is developed. The model enables expression of van der Waals frequencies in terms of fundamental molecular properties and enables facile comparison of effective force constants in a variety of van der Waals molecules. The model is successfully employed to explain van der Waals vibrational structure associated with the origin region of aniline-(argon)2 using van der Waals potential parameters derived from the aniline-(argon)1 spectrum. REMPI and emission spectra of larger clusters of aniline and argon are also reported and discussed. Using atom-atom potentials, equilibrium structures for aniline-(argon)n (n=l, 2, 3) are calculated. The calculations prove useful in the analysis of the spectra.The BfX transitions of the cation complexes fluorobenzene+-argon and chlorobenzene+-argon have been investigated. The cations were prepared by resonance enhanced multiphoton ionization of the neutral van der Waals molecules. A time delayed tunable dye laser was then used to dissociate the cations, loss of an argon atom being the dominant process. When the second laser was tuned to a cation resonance the dissociation cross section increased markedly, allowing characterization of BfX transition. The resulting spectra are presented and discussed.Thesis (PhD Doctorate)
Doctor of Philosophy (PhD)
School of Science
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Valduga, De Almeida Camargo Franco. "Unravelling vibrational and electronic coherences via two-dimensional electronic spectroscopy of zinc-porphyrins". Thesis, University of East Anglia, 2017. https://ueaeprints.uea.ac.uk/63645/.
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Two-dimensional electronic spectroscopy (2D-ES) is a cutting edge experimental method to probe ultrafast phenomena such as energy transfer, chemical reactions, coherent wavepacket motion, etc. It is an extension of transient absorption methods which recovers the signal as a function of the excitation frequency, resolving signals that are overlapped in traditional techniques, and allowing simultaneous high spectral resolution in excitation frequency and high temporal resolution of the dynamics. 2D-ES studies of light-harvesting systems from photosynthetic organisms reported coherent wavepacket motion, attributed to electronic coherences between different exciton states. Vibrational and vibronic coherences can also be observed with 2D-ES, and it is thus important to study the specific signatures of each. In this thesis, we present an experimental setup that is well suited to recover coherent wavepacket motion and employ it to study vibrational coherences in a zinc-porphyrin monomer. A first experiment is analyzed with the traditional convention of using only the real part of the complex-valued 2D-ES signal, and interference between neighboring oscillatory features is revealed, explained and modeled. We also find that when the full complex-valued signal is analyzed, the most pronounced interference features disappear, and in this case an analysis based on double-sided Feynman diagrams suffices to describe all observations. We then report an experiment with a blue-shifted laser spectrum, which matches the molecular absorption in a way that is more commonly found in 2D-ES studies, and observe signatures that closely resemble the features expected for a purely electronic coherence, which we explain considering the laser spectrum for all three field-matter interactions. Finally, we demonstrate a 2D-ES experiment with a red-shifted spectrum which exclusively probes coherences in the ground state, complementing experiments with the blue-shifted spectrum. We argue that a combination of the two suffices for unambiguous interpretation of coherences in 2D-ES, lifting the need for an ultrabroadband laser.
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Dogbe, John Kofi. "Comparing cluster and slab model geometries from density functional theory calculations of si(100)-2x1 surfaces using low-energy electron diffraction". abstract and full text PDF (free order & download UNR users only), 2007. http://0-gateway.proquest.com.innopac.library.unr.edu/openurl?url_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:dissertation&res_dat=xri:pqdiss&rft_dat=xri:pqdiss:3258835.
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Pullen, Aletha Marie. "Spectroscopic characterization of carbon based molecular electronic junctions". Connect to this title online, 2004. http://rave.ohiolink.edu/etdc/view?acc%5Fnum=osu1099671322.
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Thesis (Ph. D.)--Ohio State University, 2004.Title from first page of PDF file. Document formatted into pages; contains xvii, 208 p.; also includes graphics (some col.). Includes bibliographical references (p. 189-208).
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Öberg, Henrik. "Electronic structure and spectroscopy calculations in fuel cell catalysis". Licentiate thesis, Stockholms universitet, Fysikum, 2011. http://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-58807.
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This thesis presents joint experimental and theoretical studies of surface phenomena at an electronic structure level in proton exchange membrane fuel cells (PEM-FC's). The fuel cell activity can be related to the oxygen reduction taking place at the cathodic surface through the oxygen reduction reaction (ORR). Under certain conditions the dissociative adsorption of O2 becomes the rate limiting reaction step and may therefore affect the overall fuel cell activity. Using core-level spectroscopy in terms of X-ray Photoemission Spectroscopy (XPS), the O2 dissociation barrier on Pt(111) has been determined and density functional theory (DFT) calculations reproduce the estimate well, using structure models that account for lateral adsorbate-adsorbate interactions, a finding that may have implications on the approach to calculate electronic structure properties of heterogeneous surface catalysis. Through a Brønsted-Evans-Polanyi (BEP) relation, the activation barrier for dissociation can be connected to the chemisorption energy of the atomic oxygen binding to the Pt surface. By affecting this energy, the activity of the fuel cell can be tuned; straining the Pt lattice weakens the O-Pt bond according to the Nørskov-Hammer d-band model which relates the adsorbate-substrate chemisorption energy to the position of the d-band center relative the Fermi level. X-ray Absorption (XAS) and Emission Spectroscopy (XES) have been used together with DFT to investigate the electronic structure effect in Pt due to strain, by depositing overlayers of Pt on Cu(111). The d-band model can to some extent be employed to describe the strain effect - but the discrepancies between the calculations and the experiments remain an open question at present. Furthermore, the oxidation of the Pt(111) surface have been studied using XPS and XAS. DFT calculations support the experimental picture and suggest an oxidation resulting in an α-PtO2 type of surface-oxide.
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Fougère, Scott Gregory. "The electronic structure and spectroscopy of rhodium diatomic molecules". Thesis, National Library of Canada = Bibliothèque nationale du Canada, 2000. http://www.collectionscanada.ca/obj/s4/f2/dsk1/tape3/PQDD_0018/NQ52760.pdf.
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Haberer-Gehrmann, Danny. "Electronic Properties of Functionalized Graphene Studied With Photoemission Spectroscopy". Doctoral thesis, Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden, 2012. http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-97417.
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Graphene, a two dimensional single layer of graphite, attracts a lot of attention of researchers around the globe due to its remarkable physical properties and application potential. The origin can thereby be found in the peculiar electronic structure since graphene is a zero gap semi-conductor with a linear energy dispersion in the vicinity of the Fermi level. Consequently, the charge carriers in graphene mimic massless Dirac Fermions which brings principles of quantum electrodynamics and exotic effects like Klein tunneling into a bench-top experiment. Modifying the electronic and/or crystal structure structure by functionalization might therefore as well lead to new tantalizing physical properties, novel compound materials based on graphene like graphane (fully hydrogenated graphene) or flourographene (fluorinated graphene), and ultimately new applications.
In this work, the influences on the electronic structure of graphene are investigated with photoemission spectroscopies after covalent functionalization by atomic hydrogen and ionic functionalization with potassium. Regarding hydrogenation, the formation of tunable bandgap is observed along with a full recovery of the electronic properties of graphene upon removing the hydrogen by thermal annealing. Using high resolution x-ray photoemission and molecular dynamics simulations, the formation of a C4H structure is predicted for substrate supported graphene at a saturation H-coverage of 25%, due to a preferential para- arrangement of hydrogen atoms. In fully electron doped, hydrogenated graphene the formation of dispersionless hydrogen impurity state is observed with angle-resolved photoemission spectroscopy. This flat state is extended over the whole Brillouin zone and according to calculations not localized. Potassium-doped graphene shows a similar doping level as its 3D parent component, the graphite intercalation compound KC8. Investigating the electron-phonon coupling in doped graphene, by direct derivation of the Eliashberg-function, shows an asymmetric coupling strength along the high-symmetry directions in the Brillouin Zone of graphene. In the K-M direction additional low energetic contributions could be identified which may originate from out-of-plane phonon modes. Regarding the electron-phonon-coupling strength of the high energy in-plane phonon modes a reasonable agreement with theoretical predictions is found.
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Hodges, Philip J. "Transition metal halides, studied by high-resolution electronic spectroscopy". Thesis, University of Oxford, 2006. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.433477.
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Moxey, S. R. "Electronic spectroscopy of unstable species in free jet expansions". Thesis, University of Oxford, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.233491.
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Musgrave, Adam. "Electronic spectroscopy of Van der Waals clusters and complexes". Thesis, University of Nottingham, 2007. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.445684.
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Bin, Hussein Mohd Zobir. "Electronic spectroscopy naphthols, 1,2,4,5-tetraflurorobenzene, fluorostyrenes and oxalyl fluoride". Thesis, University of Reading, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.329597.
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Fowles, Paul Stephen. "The electronic structure of metals studied by Auger spectroscopy". Thesis, University of Liverpool, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.279693.
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Pearson, Jonathan. "Electronic spectroscopy of the transient species HNO and SnF". Thesis, University of Bristol, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.319048.
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Chang, Bor-Chen. "Electronic spectroscopy of argon-hydroxyl and neon-hydroxyl complexes /". The Ohio State University, 1993. http://rave.ohiolink.edu/etdc/view?acc_num=osu1487844948074256.
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