Electronic Structure, Intermolecular Interactions and Electron Emission Dynamics Via Anion Photoelectron Imaging PDF Download
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Author: Emily Rose Grumbling
Publisher:
ISBN:
Category :
Languages : en
Pages : 514
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Book Description
This dissertation explores the use of anion photoelectron imaging to interrogate electronic dynamics in small chemical systems with an emphasis on photoelectron angular distributions. Experimental ion generation, mass selection, laser photodetachment and photoelectron imaging were performed in a negative-ion photoelectron imaging spectrometer described in detail. Results for photodetachment from the simplest anion, H & ndash;, are used to illustrate fundamental principles of quantum mechanics and provide basic insight into the physics behind photoelectron imaging from a pedagogical perspective. This perspective is expanded by introducing imaging results for additional, representative atomic and small molecular anions, (O & ndash;, NH2 & ndash;and N3 & ndash;) obtained at multiple photon energies to address the energy-dependence of photoelectron angular distributions both conceptually and semi & ndash;quantitatively in terms of interfering partial photoelectron waves. The effect of solvation on several of these species, (H & ndash;, O & ndash;, and NH2 & ndash;) is addressed in photoelectron imaging of several series of cluster anions. The 532 and 355 nm energy spectra for H & ndash;(NH3)nand NH2 & ndash;(NH3)n(n= 0-5) reveal that these species are accurately described as the core anion solute stabilized electrostatically bynloosely coordinated NH3molecules. The photoelectron angular distributions for solvated H & ndash;deviate strongly from those predicted for unsolvated H & ndash;as the electron kinetic energy approaches zero, indicating a shift in the partial-wave balance consistent with both solvation-induced perturbation (and symmetry-breaking) of the H & ndash;parent orbital and photoelectron-solvent scattering. The photoelectron energy spectra obtained for the cluster series [O(N2O)n] & ndash;and [NO(N2O)n] & ndash;indicate the presence of multiple structural isomers of the anion cores, the former displaying sharp core-switching atn= 4, the latter isomer coexistence over the entire range studied. The photoelectron angular distributions for detachment from the O & ndash;(N2O)nand NO & ndash;(N2O)nisomers deviate strongly from those expected for bare O & ndash;and NO & ndash;, respectively, in the region of an anionic shape resonance of N2O, suggesting resonant photoelectron-solvent scattering. Partial-wave models for two-centered photoelectron interference in photodetachment from dissociating I2 & ndash;is presented and discussed in the context of previous results. New time-resolved photoelectron imaging results for I2super & ndash;, for both parallel and perpendicular pump and probe beam polarizations, are presented and briefly discussed. Finally, new ideas and directions are proposed.
Author: Emily Rose Grumbling
Publisher:
ISBN:
Category :
Languages : en
Pages : 514
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Book Description
This dissertation explores the use of anion photoelectron imaging to interrogate electronic dynamics in small chemical systems with an emphasis on photoelectron angular distributions. Experimental ion generation, mass selection, laser photodetachment and photoelectron imaging were performed in a negative-ion photoelectron imaging spectrometer described in detail. Results for photodetachment from the simplest anion, H & ndash;, are used to illustrate fundamental principles of quantum mechanics and provide basic insight into the physics behind photoelectron imaging from a pedagogical perspective. This perspective is expanded by introducing imaging results for additional, representative atomic and small molecular anions, (O & ndash;, NH2 & ndash;and N3 & ndash;) obtained at multiple photon energies to address the energy-dependence of photoelectron angular distributions both conceptually and semi & ndash;quantitatively in terms of interfering partial photoelectron waves. The effect of solvation on several of these species, (H & ndash;, O & ndash;, and NH2 & ndash;) is addressed in photoelectron imaging of several series of cluster anions. The 532 and 355 nm energy spectra for H & ndash;(NH3)nand NH2 & ndash;(NH3)n(n= 0-5) reveal that these species are accurately described as the core anion solute stabilized electrostatically bynloosely coordinated NH3molecules. The photoelectron angular distributions for solvated H & ndash;deviate strongly from those predicted for unsolvated H & ndash;as the electron kinetic energy approaches zero, indicating a shift in the partial-wave balance consistent with both solvation-induced perturbation (and symmetry-breaking) of the H & ndash;parent orbital and photoelectron-solvent scattering. The photoelectron energy spectra obtained for the cluster series [O(N2O)n] & ndash;and [NO(N2O)n] & ndash;indicate the presence of multiple structural isomers of the anion cores, the former displaying sharp core-switching atn= 4, the latter isomer coexistence over the entire range studied. The photoelectron angular distributions for detachment from the O & ndash;(N2O)nand NO & ndash;(N2O)nisomers deviate strongly from those expected for bare O & ndash;and NO & ndash;, respectively, in the region of an anionic shape resonance of N2O, suggesting resonant photoelectron-solvent scattering. Partial-wave models for two-centered photoelectron interference in photodetachment from dissociating I2 & ndash;is presented and discussed in the context of previous results. New time-resolved photoelectron imaging results for I2super & ndash;, for both parallel and perpendicular pump and probe beam polarizations, are presented and briefly discussed. Finally, new ideas and directions are proposed.
Author: Shigemasa Suga
Publisher: Springer Nature
ISBN: 3030640736
Category : Science
Languages : en
Pages : 511
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Book Description
This book presents photoelectron spectroscopy as a valuable method for studying the electronic structures of various solid materials in the bulk state, on surfaces, and at buried interfaces. This second edition introduces the advanced technique of high-resolution and high-efficiency spin- and momentum-resolved photoelectron spectroscopy using a novel momentum microscope, enabling high-precision measurements down to a length scale of some tens of nanometers. The book also deals with fundamental concepts and approaches to applying this and other complementary techniques, such as inverse photoemission, photoelectron diffraction, scanning tunneling spectroscopy, as well as photon spectroscopy based on (soft) x-ray absorption and resonance inelastic (soft) x-ray scattering. This book is the ideal tool to expand readers’ understanding of this marvelously versatile experimental method, as well as the electronic structures of metals and insulators.
Author: Etienne Garand
Publisher:
ISBN:
Category :
Languages : en
Pages : 528
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Book Description
The anion slow photoelectron velocity-map imaging (SEVI) technique, a high resolution (̃1 cm-1) variant of anion photoelectron spectroscopy, is applied to the study of open-shell anions and neutral species. First, SEVI is used to study the CnH (n=5-9), C2nN (n=1-3), CnO (n=2-3) and CnS (n=2-3) heteroatom doped carbon clusters. The SEVI spectra are assigned with the help of electronic structure calculations and Franck-Condon simulations. Precise electron affinities, term energies and vibrational frequencies are determined for these species. These studies also yield evidence of vibronic coupling in the ground states of C6H, C8H, C9H and CCS. Futhermore, it is found that the ground states of the C5H-;, C7H-;, C7H-;, C4N-; and C6N-; anions are linear triplet sigma states, contrary to previous theoretical studies that reported bent structures. In addition, the strong vibronic coupling between the very close-lying 2A1 and 2B2 states of the HCO2 and DCO2 radicals is studied using SEVI. The complex photodetachment spectra are simulated and assigned using a quasidiabatic Hamiltonian approach. The strong vibronic coupling is highlighted by the observation of several nominally forbidden transitions. The SEVI technique is also applied to the study of the weakly bound ArO and KrO van der Waals complexes. The interaction potential and spin-orbit splitting of the neutral and anion states are determined and compared with high-level electronic structure calculations. Finally, the SEVI spectra of the ClH2-; and ClD2-; anions are used to characterized the electronic and nuclear coupling in the pre-reactive region of the Cl(2P)+H2 reaction and to understand the reactivity of the excited spin-orbit state of chlorine. The SEVI spectra are compared to simulations with and without non-adiabatic couplings between the Cl spin-orbit states. The non-adiabatic effects are found to be small but their inclusion improves agreement with experiment. The second part of this work concerns the structure of ionic clusters which is studied with infrared multiple photon dissociation (IRMPD) spectroscopy. The stepwise solvation of the bicarbonate anion is probed by acquiring the IRPMD spectra of HCO3-(H2O)1-10 clusters in the gas-phase. Electronic structure calculations have been performed on the n=1-8 clusters to identify the structure of the low-lying isomers and to assign the observed spectral features. It is found that the water molecules preferably bind to the negatively charged CO2 moiety of the HCO3 & hibar; anion. A binding motif consisting of a four-membered ring with each water forming a single H-bond with the CO2 moiety is found for clusters with n=4 or larger. In addition, the structure of the small (SiO)3-5+ clusters have been studied with IRPMD and electronic structure calculations. The onset for the formation of the first Si-Si bond is observed for the n=5 cluster.
Author: Alison Virginia Davis
Publisher:
ISBN:
Category :
Languages : en
Pages : 362
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Book Description
Author: Mangalathayil Ali Abdu
Publisher: Springer Science & Business Media
ISBN: 9400703260
Category : Science
Languages : en
Pages : 479
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Book Description
This book is a multi-author treatise on the most outstanding research problems in the field of the aeronomy of the Earth’s atmosphere and ionosphere, encompassing the science covered by Division II of the International Association of Geomagnetism and Aeronomy (IAGA). It contains several review articles and detailed papers by leading scientists in the field. The book is organized in five parts: 1) Mesosphere-Lower Thermosphere Dynamics and Chemistry; 2) Vertical Coupling by Upward Propagating Waves; 3) Ionospheric Electrodynamics and Structuring; 4) Thermosphere- Ionosphere Coupling, Dynamics and Trends and 5) Ionosphere-Thermosphere Disturbances and Modeling. The book consolidates the progress achieved in the field in recent years and it serves as a useful reference for graduate students as well as experienced researchers.
Author: Joseph Woicik
Publisher: Springer
ISBN: 3319240439
Category : Science
Languages : en
Pages : 576
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Book Description
This book provides the first complete and up-to-date summary of the state of the art in HAXPES and motivates readers to harness its powerful capabilities in their own research. The chapters are written by experts. They include historical work, modern instrumentation, theory and applications. This book spans from physics to chemistry and materials science and engineering. In consideration of the rapid development of the technique, several chapters include highlights illustrating future opportunities as well.
Author: Wolfgang Domcke
Publisher: World Scientific
ISBN: 9814313440
Category : Science
Languages : en
Pages : 769
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Book Description
The concept of adiabatic electronic potential-energy surfaces, defined by the Born?Oppenheimer approximation, is fundamental to our thinking about chemical processes. Recent computational as well as experimental studies have produced ample evidence that the so-called conical intersections of electronic energy surfaces, predicted by von Neumann and Wigner in 1929, are the rule rather than the exception in polyatomic molecules. It is nowadays increasingly recognized that conical intersections play a key mechanistic role in chemical reaction dynamics. This volume provides an up-to-date overview of the multi-faceted research on the role of conical intersections in photochemistry and photobiology, including basic theoretical concepts, novel computational strategies as well as innovative experiments. The contents and discussions will be of value to advanced students and researchers in photochemistry, molecular spectroscopy and related areas.
Author: Robert Schunk
Publisher: Cambridge University Press
ISBN: 0521877067
Category : Science
Languages : en
Pages : 641
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Book Description
Describes the physical, plasma and chemical processes controlling ionospheres, upper atmospheres and exospheres, for researchers and graduates.
Author:
Publisher:
ISBN:
Category : Chemistry
Languages : en
Pages : 778
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Book Description
Author: Cheuk-yiu Ng
Publisher: World Scientific
ISBN: 9814494739
Category : Science
Languages : en
Pages : 684
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Book Description
Owing to the advances of vacuum ultraviolet and ultrafast lasers and third generation synchrotron sources, the research on photoionization, photoelectrons, and photodetachment has gained much vitality in recent years. These new light sources, together with ingenious experimental techniques, such as the coincidence imaging, molecular beam, pulsed field ionization photoelectron, mass-analyzed threshold ion, and pulsed field ion pair schemes, have allowed spectroscopic, dynamic, and energetic studies of gaseous species to a new level of detail and accuracy. Profitable applications of these methods to liquids are emerging.This invaluable two-volume review consists of twenty-two chapters, focusing on recent developments in photoionization and photodetachment studies of atoms; molecules, transient species, clusters, and liquids.
