Ultrafast Photoinduced Phase Transitions in Complex Materials Probed by Time-resolved Resonant Soft X-ray Diffraction

Ultrafast Photoinduced Phase Transitions in Complex Materials Probed by Time-resolved Resonant Soft X-ray Diffraction

Author:

Publisher:

Published: 2014

Total Pages: 110

ISBN-13:

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In processing and data storage mainly ferromagnetic (FM) materials are being used. Approaching physical limits, new concepts have to be found for faster, smaller switches, for higher data densities and more energy efficiency. Some of the discussed new concepts involve the material classes of correlated oxides and materials with antiferromagnetic coupling. Their applicability depends critically on their switching behavior, i.e., how fast and how energy efficient material properties can be manipulated. This thesis presents investigations of ultrafast non-equilibrium phase transitions on such new materials. In transition metal oxides (TMOs) the coupling of different degrees of freedom and resulting low energy excitation spectrum often result in spectacular changes of macroscopic properties (colossal magneto resistance, superconductivity, metal-to-insulator transitions) often accompanied by nanoscale order of spins, charges, orbital occupation and by lattice distortions, which make these material attractive. Magnetite served as a prototype for functional TMOs showing a metal-to-insulator-transition (MIT) at T = 123 K. By probing the charge and orbital order as well as the structure after an optical excitation we found that the electronic order and the structural distortion, characteristics of the insulating phase in thermal equilibrium, are destroyed within the experimental resolution of 300 fs. The MIT itself occurs on a 1.5 ps timescale. It shows that MITs in functional materials are several thousand times faster than switching processes in semiconductors. Recently ferrimagnetic and antiferromagnetic (AFM) materials have become interesting. It was shown in ferrimagnetic GdFeCo, that the transfer of angular momentum between two opposed FM subsystems with different time constants leads to a switching of the magnetization after laser pulse excitation. In addition it was theoretically predicted that demagnetization dynamics in AFM should occur faster than in FM materials as no net angular momentum has to be transferred out of the spin system. We investigated two different AFM materials in order to learn more about their ultrafast dynamics. In Ho, a metallic AFM below T ≈ 130 K, we found that the AFM Ho can not only be faster but also ten times more energy efficiently destroyed as order in FM comparable metals. In EuTe, an AFM semiconductor below T ≈ 10 K, we compared the loss of magnetization and laser-induced structural distortion in one and the same experiment. Our experiment shows that they are effectively disentangled. An exception is an ultrafast release of lattice dynamics, which we assign to the release of magnetostriction. The results presented here were obtained with time-resolved resonant soft x-ray diffraction at the Femtoslicing source of the Helmholtz-Zentrum Berlin and at the free-electron laser in Stanford (LCLS). In addition the development and setup of a new UHV-diffractometer for these experiments will be reported


Photoinduced Phase Transitions

Photoinduced Phase Transitions

Author: Keiichiro Nasu

Publisher: World Scientific

Published: 2004-09-09

Total Pages: 354

ISBN-13: 9814483192

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A new class of insulating solids was recently discovered. When irradiated by a few visible photons, these solids give rise to a macroscopic excited domain that has new structural and electronic orders quite different from the starting ground state. This occurrence is called “photoinduced phase transition”, and this multi-authored book reviews recent theoretical and experimental studies of this new phenomenon.Why and how do photoexcited few electrons finally result in an excited domain with a macroscopic size? How is the resultant photoinduced phase different from the ordinary thermal-induced phase? This review volume answers those essential questions.This book has been selected for coverage in:• CC / Physical, Chemical & Earth Sciences• Index to Scientific Book Contents® (ISBC)


Emergent States in Photoinduced Charge-Density-Wave Transitions

Emergent States in Photoinduced Charge-Density-Wave Transitions

Author: Alfred Zong

Publisher: Springer Nature

Published: 2021-09-17

Total Pages: 234

ISBN-13: 3030817512

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This book advances understanding of light-induced phase transitions and nonequilibrium orders that occur in a broken-symmetry system. Upon excitation with an intense laser pulse, materials can undergo a nonthermal transition through pathways different from those in equilibrium. The mechanism underlying these photoinduced phase transitions has long been researched, but many details in this ultrafast, non-adiabatic regime still remain to be clarified. The work in this book reveals new insights into this phenomena via investigation of photoinduced melting and recovery of charge density waves (CDWs). Using several time-resolved diffraction and spectroscopic techniques, the author shows that the light-induced melting of a CDW is characterized by dynamical slowing-down, while the restoration of the symmetry-breaking order features two distinct timescales: A fast recovery of the CDW amplitude is followed by a slower re-establishment of phase coherence, the latter of which is dictated by the presence of topological defects in the CDW. Furthermore, after the suppression of the original CDW by photoexcitation, a different, competing CDW transiently emerges, illustrating how a hidden order in equilibrium can be unleashed by a laser pulse. These insights into CDW systems may be carried over to other broken-symmetry states, such as superconductivity and magnetic ordering, bringing us one step closer towards manipulating phases of matter using a laser pulse.


Theory and Applications of Time-resolved Spectroscopies

Theory and Applications of Time-resolved Spectroscopies

Author: Yuan Chen (Researcher on material dynamics)

Publisher:

Published: 2020

Total Pages:

ISBN-13:

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Time-resolved spectroscopies of materials provide a wealth of information on material dynamics, and have been a focus of study for decades. With increasing energy and time resolution, time-resolved spectroscopies have been able to detect quasiparticle dynamics, details of electron transport, and ultrafast phase transitions. More recently, as a novel technique, time-resolved resonant inelastic x-ray scattering (trRIXS) is developed and used to investigate spin and charge orders in strongly correlated materials. In this dissertation, I will review the theories of equilibrium and nonequilibrium spectroscopies, with an emphasis on the development of trRIXS theory. Numerical simulation of trRIXS is performed on a single-band tight binding model under the high frequency limit and low frequency limit, revealing Floquet physics and real-time charge oscillation respectively. I will also give examples of applications of time-resolved spectroscopies, especially trRIXS: detecting photoinduced chiral edge states in a graphene nanoribbon and investigating charge excitations in a pumped Mott insulator. Specifically, for the graphene nanoribbon, trRIXS has the potential to selectively probe certain edge states at given energies, providing a conclusive answer to the existence of photoinduced chiral edge states. Finally I will discuss some technical aspects in my implementation of trRIXS code for noninteracting systems. I hope this dissertation can deepen the understanding of pump-probe spectroscopies, especially the novel trRIXS, and provide resources to help design future experiments.


Photoinduced Phase Transitions Studied by Femtosecond Single-shot Spectroscopy

Photoinduced Phase Transitions Studied by Femtosecond Single-shot Spectroscopy

Author: Taeho Shin

Publisher:

Published: 2010

Total Pages: 228

ISBN-13:

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Single-shot femtosecond spectroscopy has been developed and employed for the study of phase transitions of solid-state materials. Using two crossed echelons, a two dimensional spatial delay gradient was generated across a single probe pulse profile. This novel scheme enables us to monitor irreversible change in solids by acquiring many time-resolved data points with a single laser pulse. With the integration with a non-collinear optical parametric amplifier (NOPA) and a conventional pump-probe instrument, ultrafast dynamics of coherent lattice vibrations and photo-induced phase transitions were examined in two different systems. Ultrafast dynamics such as coherent lattice vibrations and bond softening were investigated for Bi thin films and bulk single crystals. Depending on the thickness, transient reflectivity was changed significantly. The variations are ascribed to different electronic structures possibly originating from quantum confinement. Bond softening exhibits a strong thickness dependence due to hot carrier dynamics as well as to the different electronic structures. At high pump fluences, no phonon oscillations were observed suggesting a phase transition to liquid or to a higher symmetry crystalline phase (reverse Peierls distortion). Together with thermal modeling, double pump measurements reveal nonthermal melting occurring in bulk and thin Bi films. A higher threshold fluence for nonthermal melting is observed in bulk bismuth as compared to thin films, suggesting ultrafast carrier dynamics such as ballistic transport. In addition to nonthermal effects, thermal effects such as inelastic electron-phonon scattering and nonradiative recombination play a crucial role in melting and cooling at later times after nonthermal melting takes place. A quasi one-dimensional platinum iodide complex showed strong oscillations in reflectivity which are attributed to oscillatory motions of wave packets on a selftrapped exciton (STE) potential surface., As optical excitation increased, electron transfer from Pt 2+ to an adjacent Pt4+ occurred over a wider range of lattice sites and weakened the oscillations. Above a certain pump fluence, oscillations disappeared completely indicating that the mixed valence, charge density wave state changed to monovalent, Mott-Hubbard phase. The reverse phase transition, i.e., from the MottHubbard phase to the charge density wave state began within 3 ps of the optical pump.


Time-resolved Diffraction

Time-resolved Diffraction

Author: J. R Helliwell

Publisher: Oxford University Press

Published: 1997-12-18

Total Pages: 446

ISBN-13: 9780198500322

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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.


Imaging Light with Photoelectrons on the Nano-Femto Scale

Imaging Light with Photoelectrons on the Nano-Femto Scale

Author: Yanan Dai

Publisher: Springer Nature

Published: 2020-09-03

Total Pages: 124

ISBN-13: 3030528367

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This thesis presents significant advances in the imaging and theory of the ultrafast dynamics of surface plasmon polariton fields. The author details construction of a sub-10 femtosecond and sub-10 nanometer spatiotemporal resolution ultrafast photoemission microscope which is subsequently used for the discovery of topological meron and skyrmion-like plasmonic quasiparticles. In particular, this enabled the creation of movies of the surface plasmon polariton fields evolving on sub-optical wavelength scales at around 0.1 femtosecond per image frame undergoing vortex phase evolution. The key insight that the transverse spin of surface plasmon polaritons undergoes a texturing into meron or skyrmion-like topological quasiparticles (defined by the geometric charge of the preparation) follows. In addition, this thesis develops an analytical theory of these new topological quasiparticles, opening new avenues of research, while the ultrafast microscopy techniques established within will also be broadly applicable to studies of nanoscale optical excitations in electronic materials.