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X-ray diffraction is an invaluable tool in the field of structural dynamics. In the work described in this thesis, time-resolved X-ray diffraction experiments were carried out to investigate ultrafast lattice dynamics. Ultrashort laser pulses were used to induce non-thermal melting and large-amplitude strain waves, and X-rays were used to probe these phenomena. Non-thermal melting was studied in indium antimonide (InSb). It was found that the inertial model, which states that the motion of the atoms is determined by their initial vibrational energy at the time of laser irradiation, accurately describes the process of non-thermal melting. It was demonstrated that the model is valid over a large range of temperatures, from 35 to 500 K, when taking the zero-point energy into account at low temperatures. It was also shown how the process of non-thermal melting can be used as a timing monitor to determine the relative timing of laser and X-ray beams in pump/probe experiments. It was shown how the use of an opto-acoustic transducer could reduce the duration of an Xray pulse. The transducer was made of a thin gold film deposited on the surface of bulk InSb. Upon heating the thin gold film with an ultrashort laser pulse, a strain wave was generated in the semiconductor. This resulted in a modulated phonon spectrum and X-ray reflectivity. It was shown that a 100 ps long X-ray pulse can be transformed to a 20 ps pulse with an 8% efficiency. A large-amplitude strain wave was generated in graphite using an ultrashort laser pulse to elucidate the potential role of strain in phase transitions. The temporal evolution of the strain wave was mapped, and the pressure deduced. It was found that it was possible to induce a pressure and temperature corresponding to the region in the carbon phase diagram in which diamond can form.
Volume 1 of this work presents theory and methods to study the structure of condensed matter on different time scales. The authors cover the structure analysis by X-ray diffraction methods from crystalline to amorphous materials, from static-relaxed averaged structures to short-lived electronically excited structures, including detailed descriptions of the time-resolved experimental methods. Complementary, an overview of the theoretical description of condensed matter by static and time-dependent density functional theory is given, starting from the fundamental quantities that can be obtained by these methods through to the recent challenges in the description of time dependent phenomena such as optical excitations. Contents Static structural analysis of condensed matter: from single-crystal to amorphous DFT calculations of solids in the ground state TDDFT, excitations, and spectroscopy Time-resolved structural analysis: probing condensed matter in motion Ultrafast science
Since the early 20th century, X-ray and electron scattering has provided a powerful means by which the location of atoms can be identified in gas-phase molecules and condensed matter with sub-atomic spatial resolution. Scattering techniques can also provide valuable observables of the fundamental properties of electrons in matter such as an electron’s spin and its energy. In recent years, significant technological developments in both X-ray and electron scattering have paved the way to time-resolved analogues capable of capturing real-time snapshots of transient structures undergoing a photochemical reaction. Structural Dynamics with X-ray and Electron Scattering is a two-part book that firstly introduces the fundamental background to scattering theory and photochemical phenomena of interest. The second part discusses the latest advances and research results from the application of ultrafast scattering techniques to imaging the structure and dynamics of gas-phase molecules and condensed matter. This book aims to provide a unifying platform for X-ray and electron scattering.
Recent technological advances in synchrotron and neutron sources, detectors, and computer hardware and software have made possible diffraction techniques which collect data at successive moments in time. This is the first book to bring together reviews and research articles covering the three branches of time-resolved diffraction--X-ray, electron, and neutron field. Time-Resolved Diffraction covers gases, liquids, amorphous solids, fibers, and crystals and does so in a multidisciplinary framework which includes examples from molecular biology and chemistry, as well as techniques from physics and materials science. The various time scales of data collection cover ten orders of magnitude, from the sub-pico domain to the kilosecond. Research scientists and graduate students will find this book the most complete compendium of work in this developing field.
ABSTRACT: Direct observation and understanding of atomic-level structural dynamics are important frontiers in scientific research and applications. Femtosecond electron diffraction (FED), a technique that combines time-resolved pump-probe and electron diffraction concepts, holds a great promise to reveal the dynamical processes of ultrafast phenomena in biology, chemistry and solid-state physics at the atomic time and length scales.
This work focuses on complementary crystallographic and spectroscopic areas of dynamic structural science, from papers presented at the 46th NATO sponsored course in Erice, Sicily 2013. These papers cover a range of material from background concepts to more advanced material and represent a fully inter-disciplinary collection of the latest ideas and results within the field. They will appeal to practising or novice crystallographers, both chemical and biological, who wish to learn more about modern spectroscopic methods and convergent advances and hence vice versa for experimental and computational spectroscopists. The chapters refer to the latest techniques, software and results and each chapter is fully referenced. The volume provides an excellent starting point for new comers in the emerging, multi-disciplinary area of time resolved science.
Nonlinear Optics, Quantum Optics, and Ultrafast Phenomena with X-Rays is an introduction to cutting-edge science that is beginning to emerge on state-of-the-art synchrotron radiation facilities and will come to flourish with the x-ray free-electron lasers currently being planned. It is intended for the use by scientists at synchrotron radiation facilities working with the combination of x-rays and lasers and those preparing for the science at x-ray free-electron lasers. In the past decade synchrotron radiation sources have experienced a tremendous increase in their brilliance and other figures of merit. This progress, driven strongly by the scientific applications, is still going on and may actually be accelerating with the advent of x-ray free-electron lasers. As a result, a confluence of x-ray and laser physics is taking place, due to the increasing importance of laser concepts, such as coherence and nonlinear optics to the x-ray community and the importance of x-ray optics to the laser-generation of ultrashort pulses of x-rays.
Volume 1 of this work presents theory and methods to study the structure of condensed matter on different time scales. The authors cover the structure analysis by X-ray diffraction methods from crystalline to amorphous materials, from static-relaxed averaged structures to short-lived electronically excited structures, including detailed descriptions of the time-resolved experimental methods. Complementary, an overview of the theoretical description of condensed matter by static and time-dependent density functional theory is given, starting from the fundamental quantities that can be obtained by these methods through to the recent challenges in the description of time dependent phenomena such as optical excitations. Contents Static structural analysis of condensed matter: from single-crystal to amorphous DFT calculations of solids in the ground state TDDFT, excitations, and spectroscopy Time-resolved structural analysis: probing condensed matter in motion Ultrafast science