Ultrafast Soft X-ray Absorption Spectroscopy of Molecular Systems in the Water Window with Table-top High-order Harmonic Sources PDF Download
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Author: Carlo Kleine
Publisher:
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Languages : en
Pages : 0
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Englische Version: The invention of the laser made coherent light sources widely available. Technical advances in pulse power und pulse duration allow the study of linear and nonlinear interactions of light and matter and ultrashort time scales. The highest nonlinear frequency up-converting process, High-order harmonics generation, is today the standard for up to attosecond short table-top sources. This method has been recently applied for ultrafast spectroscopy in the soft x-ray water window. In this thesis, a table-top high-order harmonics setup is presented and used for pump-probe spectroscopy in the water window. A home-built soft x-ray absorption spectrometer enables the so far best resolution and detected flux at nitrogen K-edge. The setup is utilized to study ionization dynamics of diatomic nitrogen on femtosecond time scales and the subsequent picosecond plasma dynamics. In the realm of air lasing, where lasing in nitrogen ions formed by strong field ionization is studied new insides are provided, narrowing down possible theoretical interpretations. The low absorption cross section of water between the carbon and oxygen K-edges known as the water window, enables to investigate molecules and ions in aqueous solution. The first steady-state soft x-ray spectra are presented for ions and molecular systems in aqueous solution recorded with a table-top laser based setup. Furthermore, the approach is also applied for transient absorption spectra. Additional data from beamtimes at large scale facilities allow for a comparison of the approaches. Finally, spectroscopic results taken at BESSY II are presented. The structure and local environment of excess protons in water is studied for more than two centuries and are still controversially discussed. [...].
Author: Carlo Kleine
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Book Description
Englische Version: The invention of the laser made coherent light sources widely available. Technical advances in pulse power und pulse duration allow the study of linear and nonlinear interactions of light and matter and ultrashort time scales. The highest nonlinear frequency up-converting process, High-order harmonics generation, is today the standard for up to attosecond short table-top sources. This method has been recently applied for ultrafast spectroscopy in the soft x-ray water window. In this thesis, a table-top high-order harmonics setup is presented and used for pump-probe spectroscopy in the water window. A home-built soft x-ray absorption spectrometer enables the so far best resolution and detected flux at nitrogen K-edge. The setup is utilized to study ionization dynamics of diatomic nitrogen on femtosecond time scales and the subsequent picosecond plasma dynamics. In the realm of air lasing, where lasing in nitrogen ions formed by strong field ionization is studied new insides are provided, narrowing down possible theoretical interpretations. The low absorption cross section of water between the carbon and oxygen K-edges known as the water window, enables to investigate molecules and ions in aqueous solution. The first steady-state soft x-ray spectra are presented for ions and molecular systems in aqueous solution recorded with a table-top laser based setup. Furthermore, the approach is also applied for transient absorption spectra. Additional data from beamtimes at large scale facilities allow for a comparison of the approaches. Finally, spectroscopic results taken at BESSY II are presented. The structure and local environment of excess protons in water is studied for more than two centuries and are still controversially discussed. [...].
Author: Cédric Schmidt
Publisher: Springer Nature
ISBN: 3030678385
Category : Science
Languages : en
Pages : 119
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Book Description
This work studies the relaxation dynamics of molecules in both the gas and liquid phases after strong field ionization, using transient absorption in the soft X-rays. In particular, the thesis presents the first realization of time-resolved X-ray absorption spectroscopy in the spectral water window with a laser-based HHG source. These remarkable experiments were not only performed for isolated molecules, but also in liquids, for which the spectral coverage of the K-edges of C, N, and O are of primary importance for investigating biological molecules. The technique relies on the generation of high-order harmonics to further probe the electronic structure of molecules. Using the atomic selectivity of high energies and the temporal coherence of laser technology, we demonstrate the observation of the first stages of chemical transformation of matter in the gas and liquid phases.
Author: Zhi-Heng Loh
Publisher:
ISBN:
Category :
Languages : en
Pages : 300
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Author: Yoann Pertot
Publisher:
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Category :
Languages : en
Pages :
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Author: García Iriepa Cristina
Publisher: Elsevier
ISBN: 0323972225
Category : Medical
Languages : en
Pages : 520
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Book Description
Theoretical and Computational Photochemistry: Fundamentals, Methods, Applications and Synergy with Experimental Approaches provides a comprehensive overview of photoactive systems and photochemical processes. After an introduction to photochemistry, the book discusses the key computational chemistry methods applied to the study of light-induced processes over the past decade, and further outlines recent research topics to which these methods have been applied. By discussing the synergy between experimental and computational data, the book highlights how theoretical studies could facilitate understanding experimental findings. This helpful guide is for both theoretical chemists and experimental photochemistry researchers interested in utilizing computational photochemistry methods for their own work. - Reviews the fundamentals of photochemistry, helping those new to the field in understanding key concepts - Provides detailed guidance and comparison of computational and theoretical methods, highlighting the suitability of each method for different case studies - Outlines current applications to encourage discussion of the synergy between experimental and computational data, and inspiring further application of these methods to other photochemical processes
Author: Roberto Marquardt
Publisher: Elsevier
ISBN: 0128172355
Category : Science
Languages : en
Pages : 376
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Book Description
Molecular Spectroscopy and Quantum Dynamics, an exciting new work edited by Professors Martin Quack and Roberto Marquardt, contains comprehensive information on the current state-of-the-art experimental and theoretical methods and techniques used to unravel ultra-fast phenomena in atoms, molecules and condensed matter, along with future perspectives on the field. - Contains new insights into the quantum dynamics and spectroscopy of electronic and nuclear motion - Presents the most recent developments in the detection and interpretation of ultra-fast phenomena - Includes a discussion of the importance of these phenomena for the understanding of chemical reaction dynamics and kinetics in relation to molecular spectra and structure
Author:
Publisher:
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Category :
Languages : en
Pages : 18
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Book Description
This research program explored time-resolved dynamics of molecular systems by femtosecond photoelectron spectroscopy using high order harmonics. Ultrafast soft x-ray laser pump/probe studies revealed changes in binding relations and atomic core level shifts in the molecules during chemical rearrangements by detecting the changes in photoelectron energies as a function of internuclear separation in dissociative states in real time. Harmonic pulses with photon energies up to 100 eV and femtosecond time resolution were produced with excellent efficiency and pulse-to-pulse stability. Valence and core photoelectron spectra were obtained on neutral atoms and molecules. Phase manipulation of high order harmonics was achieved. Photoelectron spectra and photoionization mass spectra of gas phase ionic liquids were obtained. Two color excitation spectra of bromine molecules were investigated, as well as Rydberg wave packet photoelectron angular distributions. Pump/probe experiments on the photodissociation of metal carbonyls, halogens, and aluminum halides were also under investigation.
Author: Joachim Stöhr
Publisher: Springer Science & Business Media
ISBN: 3662028530
Category : Science
Languages : en
Pages : 415
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Book Description
This is the first ever comprehensive treatment of NEXAFS spectroscopy. It is suitable for novice researchers as an introduction to the field, while experts will welcome the detailed description of state-of-the-art instrumentation and analysis techniques, along with the latest experimental and theoretical results.
Author: J. Gomes Ferreira
Publisher: Springer Science & Business Media
ISBN: 1461307317
Category : Science
Languages : en
Pages : 425
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Book Description
The fields of X-Ray Spectroscopy in Atomic and Solid State Physics have undergone spectacular growth, sometimes rather anarchic, during the past decade. The old mold of X-ray spectroscopy has been burst, and this ASI provided an in-depth exploration of theory and recently developed techniques; however, some work still needs to be done to create a new frame and reduce anarchy in the field. The purpose of this Institute was to gather atomic and solid state physicists working in theoretical and new experimental techniques recently developed. The lectures were concerned with, among others, the following fields: theory of X-ray near-edge structure, XPS and AES with conventional and synchrotron radiation sources, PIXE, EXAFS, SEXAFS, XRF, SXS, and molecular spectroscopy. The Institute considered in detail some of these experimental tech niques and the pertinent theoretical interpretations by selecting an important list of lectures which summarize the scientific contents of the ASI. The truly international character of this NATO ASI, its size, and the high quality of the lecturers contributed to make this school a very fruitful scientific meeting. Two to four general lectures were given each working day and three afternoons were reserved for presentation of current work in the form of posters. We think that these poster presentations reflect the current research work of the participants.
Author:
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Languages : en
Pages :
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Water has many anomalous thermodynamic and physical properties as a result of the intermolecular hydrogen-bonding (H-bonding). In this dissertation, several synchrotron x-ray techniques were used to investigate the structure of ice and liquid water, both neat, pure water, and in aqueous solutions. First, the effect of protons and hydroxide ions was explored using x-ray Raman Scattering (XRS) and small angle x-ray scattering (SAXS). Both excess protons and hydroxide ions induce strong H-bonds in water molecules in their vicinity. However, proton appears to have only a local effect while hydroxide induces more density fluctuations on the long length scale. Then the effect of ionic charge was explored using SAXS. It was observed that multivalent cations such as magnesium and aluminum ions form "quasi-lattice" in the solution due to the repulsive interactions between the hydrated cations. Higher-charged molecular anions such as sulfate and phosphate do not have such a pronounced effect due to the fundamental difference in cation and anion hydration mechanisms in water. Following the study of molecular anions, the perchlorate anion, a most structure-breaking anion, was studied in more depth using x-ray absorption spectroscopy (XAS) and SAXS. It was observed that perchlorate not only breaks H-bonds in water, but also interacts with water in the hydration shells of multivalent cations such that the "quasi-lattice" structure is significantly disrupted. Finally, temperature-dependent XAS of supercooled water was studied and the absorption cross section was compared with ice data to further understand the interpretation of XAS in this dissertation.
