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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.
In this thesis I summarize my contribution to the research field of ultrafast structural dynamics in condensend matter. It consists of 17 publications that cover the complex interplay between electron, magnon, and phonon subsystems in solid materials and the resulting lattice dynamics after ultrafast photoexcitation. The investigation of such dynamics is necessary for the physical understanding of the processes in materials that might become important in the future as functional materials for technological applications, for example in data storage applications, information processing, sensors, or energy harvesting. In this work I present ultrafast x-ray diffraction (UXRD) experiments based on the optical pump - x-ray probe technique revealing the time-resolved lattice strain. To study these dynamics the samples (mainly thin film heterostructures) are excited by femtosecond near-infrared or visible light pulses. The induced strain dynamics caused by stresses of the excited subsystems are measured in a pump-probe scheme with x-ray ...
The recent developement of high power lasers, delivering femtosecond pulses of 20 2 intensities up to 10 W/cm , has led to the discovery of new phenomena in laser interactions with matter. At these enormous laser intensities, atoms, and molecules are exposed to extreme conditions and new phenomena occur, such as the very rapid multi photon ionization of atomic systems, the emission by these systems of very high order harmonics of the exciting laser light, the Coulomb explosion of molecules, and the acceleration of electrons close to the velocity of light. These phenomena generate new behaviour of bulk matter in intense laser fields, with great potential for wide ranging applications which include the study of ultra-fast processes, the development of high-frequency lasers, and the investigation of the properties of plasmas and condensed matter under extreme conditions of temperature and pressure. In particular, the concept of the "fast ignitor" approach to inertial confinement fusion (ICF) has been proposed, which is based on the separation of the compression and the ignition phases in laser-driven ICF. The aim of this course on "Atom, Solids and Plasmas in Super-Intense Laser fields" was to bring together senior researchers and students in atomic and molecular physics, laser physics, condensed matter and plasma physics, in order to review recent developments in high-intensity laser-matter interactions. The course was held at the Ettore Majorana International Centre for Scientific Culture in Erice from July 8 to July 14,2000.
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
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.
This book presents the latest advances in ultrafast science, including ultrafast laser and measurement technology, and studies of ultrafast phenomena. It summarizes the results presented at the 12th Ultrafast Phenomena Conference and reviews the state of the art of this important and rapidly advancing field.
Ultrafast Phenomena XVI presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultrafast technology has a profound impact in a wide range of applications, amongst them biomedical imaging, chemical dynamics, frequency standards, material processing, and ultrahigh speed communications. This book summarizes the results presented at the 16th International Conference on Ultrafast Phenomena and provides an up-to-date view of this important and rapidly advancing field.
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.