Ultrafast X-ray Sources Research Articles

On the feasibility of time-resolved X-ray powder diffraction of macromolecules using laser-driven ultrafast X-ray sources.

With the emergence of ultrafast X-ray sources, interest in following fast processes in small molecules and macromolecules has increased. Most of the current research into ultrafast structural dynamics of macromolecules uses X-ray free-electron lasers. In parallel, small-scale laboratory-based laser-driven ultrafast X-ray sources are emerging. Continuous development of these sources is underway, and as a result many exciting applications are being reported. However, because of their low flux, such sources are not commonly used to study the structural dynamics of macromolecules. This article examines the feasibility of time-resolved powder diffraction of macromolecular microcrystals using a laboratory-scale laser-driven ultrafast X-ray source.

Stimulated X-ray emission spectroscopy.

We describe an emerging hard X-ray spectroscopy technique, stimulated X-ray emission spectroscopy (S-XES). S-XES has the potential to characterize the electronic structure of 3d transition metal complexes with spectral information currently not reachable and might lead to the development of new ultrafast X-ray sources with properties beyond the stateoftheart. S-XES has become possible with the emergence of X-ray free-electron lasers (XFELs) that provide intense femtosecond X-ray pulses that can be employed to generate a population inversion of core-hole excited states resulting in stimulated X-ray emission. We describe the instrumentation, the various types of S-XES, the potential applications, the experimental challenges, and the feasibility of applying S-XES to characterize dilute systems, including the Mn4Ca cluster in the oxygen evolving complex of photosystem II.

Nanosecond pulse X-ray emission source based on ultrafast laser modulation

<sec>In response to the growing demand for miniaturized ultrafast pulsed X-ray sources in the fields of fundamental science and space applications, we design and develop an ultrafast pulsed X-ray generator based on a laser-modulated light source and a photoelectric cathode. This innovative technology addresses the limitations commonly encountered in traditional X-ray emission devices, such as low repetition rate, insufficient time stability, and suboptimal pulse characteristics.</sec><sec>Our effort is to study and develop the ultrafast modulation control module for the pulsed X-ray generator. This effort results in achieving high levels of time accuracy and stability in ultrafast time-varying photon signals. Moreover, we successfully generate nanosecond pulsed X-rays by using a laser-controlled light source.</sec><sec>Theoretically, we establish a comprehensive time response model for the pulsed X-ray generator in response to short pulses. This includes a thorough analysis of the time characteristics of the emitted pulsed X-rays in the time domain. Experimentally, we conduct a series of tests related to various time-related parameters of the laser-controlled light source. Additionally, we design and implemente an experimental test system for assessing the time characteristics of pulsed X-rays, by using an ultrafast scintillation detector.</sec><sec>The experimental results clearly demonstrate that our pulsed X-ray generator achieves impressive capabilities, including high repetition rates (12.5 MHz), ultrafast pulses (4 ns), and exceptional time stability (400 ps) in X-ray emission. These results closely align with our established theoretical model. Compared with traditional modulation techniques, our system exhibits significant improvement in pulse time parameters, thereby greatly expanding its potential applications.</sec><sec>This research provides a valuable insight into achieving ultra-high time stability and ultrafast pulsed X-ray emission sources. These advances will further enhance the capabilities of X-ray technology for scientific research and space applications.</sec>

Toward ultrafast soft x-ray spectroscopy of organic photovoltaic devices.

Novel ultrafast x-ray sources based on high harmonic generation and at x-ray free electron lasers are opening up new opportunities to resolve complex ultrafast processes in condensed phase systems with exceptional temporal resolution and atomic site specificity. In this perspective, we present techniques for resolving charge localization, transfer, and separation processes in organic semiconductors and organic photovoltaic devices with time-resolved soft x-ray spectroscopy. We review recent results in ultrafast soft x-ray spectroscopy of these systems and discuss routes to overcome the technical challenges in performing time-resolved x-ray experiments on photosensitive materials with poor thermal conductivity and low pump intensity thresholds for nonlinear effects.

Oxide- and Silicate-Water Interfaces and Their Roles in Technology and the Environment.

Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic- and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by "anomalies" or "non-idealities" such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surface-sensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide- and silicate-water interfaces. This critical review discusses how science progresses from understanding ideal solid-water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. We anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.

Ultrafast X-Ray Probes of Elementary Molecular Events

Elementary events that determine photochemical outcomes and molecular functionalities happen on the femtosecond and subfemtosecond timescales. Among the most ubiquitous events are the nonadiabatic dynamics taking place at conical intersections. These facilitate ultrafast, nonradiative transitions between electronic states in molecules that can outcompete slower relaxation mechanisms such as fluorescence. The rise of ultrafast X-ray sources, which provide intense light pulses with ever-shorter durations and larger observation bandwidths, has fundamentally revolutionized our spectroscopic capabilities to detect conical intersections. Recent theoretical studies have demonstrated an entirely new signature emerging once a molecule traverses a conical intersection, giving detailed insights into the coupled nuclear and electronic motions that underlie, facilitate, and ultimately determine the ultrafast molecular dynamics. Following a summary of current sources and experiments, we survey these techniques and provide a unified overview of their capabilities. We discuss their potential to dramatically increase our understanding of ultrafast photochemistry.

Impact of Solvent-Solute Hydrogen Bonding on Ultrafast Electron Transfer in a Trimetallic Iron-Ruthenium Complex

Transition metal complexes (TMCs) are widely used as light absorbers and catalysts for photochemical energy conversion processes such as photocatalytic reactions in liquid environments. Of particular interest are TMCs which incorporate multiple bridged metal centres because they represent a step towards more complex supramolecular assemblies that can ultimately enable control of the charge flow in solution-based photo-redox processes. However, the development of design guidelines for such molecular assemblies is impeded by an incomplete understanding of the coupling between their electronic and nuclear dynamics, including the interplay of TMCs with their liquid environment upon photoexcitation. Probing the involved processes requires high spatial sensitivity towards electronic motion and the ability to capture atomic motion on ultrafast timescales – a combination which is not readily available for optical transient spectroscopic techniques.X-ray free electron lasers (XFELs) have revolutionized the field of ultrafast science in recent years. XFELs generate tuneable and extremely bright X-ray pulses with a typical pulse duration of <30 fs, which are well-suited as an element-specific probe of ultrafast electronic and atomic motion in molecules and materials.1,2 Applied to TMCs, XFEL probes are sensitive to the local electronic structure in such molecular systems as well as to intra- and inter-molecular structural reorganization at an atomic level.3 In this talk, I will present work on the interaction of a linear trimetallic cyanide-bridged iron-ruthenium complex (FeRuFe) with its solvent environment, carried out using the LCLS XFEL facility at SLAC National Accelerator Laboratory. The focus of this study lies on elucidating how photoinduced intramolecular electron transfer processes in FeRuFe are affected by hydrogen bonding interactions between its cyanide ligands and the surrounding solvent molecules. In water, such solvent-solute hydrogen bonding interactions are stronger for Fe(II) than Fe(III), leading to substantial changes in solute-solvent interactions upon photoinduced electron transfer between metal centres.The experiment is performed in a pump-probe geometry on a liquid jet, where a visible/near-infrared pump induces a metal-to-metal charge transfer (MMCT) between Ru and Fe which is followed by an ultrafast back-electron transfer (BET). The excited state dynamics are monitored using hard X-ray pulses as a function of time delay between the laser pump and the X-ray probe pulses. To resolve and correlate electronic and structural dynamics upon MMCT excitation, we simultaneously perform ultrafast Fe Kβ X-ray emission spectroscopy (XES) and X-ray solution scattering (XSS) measurements, where XES is sensitive to the oxidation and spin state of the Fe centres and XSS provides information on atomic motion in solute and solvent, as demonstrated in previous work on a similar system.4 To evaluate the effect of solute-solvent hydrogen bonding interactions on the electron transfer dynamics, we perform measurements in a series of solvents with different hydrogen bonding properties, including water, methanol, and acetonitrile. We find that the BET increases as a function of decreasing hydrogen bonding ability of the solvent, and that distinct signatures of solvation dynamics are present in the scattering data. The resulting molecular level understanding of solvent reorganization coupled to electron transfer demonstrates that the strength and type of solute-solvent interactions are a central factor in determining the outcome of photoinduced charge transfer processes in TMCs.References Bergmann, U. et al. Using X-ray free-electron lasers for spectroscopy of molecular catalysts and metalloenzymes. Nat. Rev. Phys. 3, 264–282 (2021).Schoenlein, R. et al. Recent advances in ultrafast X-ray sources. Philos. Trans. R. Soc. Math. Phys. Eng. Sci. 377, 20180384 (2019).Gaffney, K. J. Capturing photochemical and photophysical transformations in iron complexes with ultrafast X-ray spectroscopy and scattering. Chem. Sci. 12, 8010–8025 (2021).Biasin, E. et al. Direct observation of coherent femtosecond solvent reorganization coupled to intramolecular electron transfer. Nat. Chem. 13, 343–349 (2021).

Long range terahertz driven electron acceleration using phase shifters

Terahertz radiation (THz)-based electron acceleration has the potential as a technology for driving the next-generation, compact ultrafast and ultrabright electron and x-ray sources. Dephasing is one of the key problems that prevent long THz–electron interaction lengths in the sub- to few-MeV range, where electron velocities vary significantly during high-field acceleration. Here, we present a phase-shifter design with double vacuum channels to alternate the phase velocity that effectively extends the THz–electron interaction length in THz-powered dielectrically loaded waveguides. The electrons are swept multiple-times back and forth through the accelerating phase of the THz wave to undergo continuous acceleration along the entire interaction. In addition, the double vacuum channel design enables increases in both the phase and group velocities of the THz wave, which leads to an adaptive synchronous acceleration with extended interaction length. This method paves the way for the practical implementation of THz-powered devices for high-energy ultrafast electron sources.

Ultrafast magnetic scattering on ferrimagnets enabled by a bright Yb-based soft x-ray source

Development of ultrafast table-top x-ray sources that can map various spin, orbital, and electronic configurations and reordering processes on their natural time and length scales is an essential topic for modern condensed matter physics as well as ultrafast science. In this work, we demonstrate spatiotemporally resolved resonant magnetic scattering (XRMS) to probe the inner-shell 4d electrons of a rare-earth (RE) composite ferrimagnetic system using a bright &gt; 200 e V soft x-ray high harmonic generation (HHG) source, which is relevant for future energy-efficient, high-speed spintronic applications. The XRMS is enabled by direct driving of the HHG process with power-scalable, high-energy Yb laser technology. The optimally phase-matched broadband plateau of the HHG offers a record photon flux ( &gt; 2 × 1 0 9 p h o t o n s / s / 1 % bandwidth) with excellent spatial coherence and covers the entire resonant energy range of RE’s N 4 , 5 edges. We verify the underlying physics of our x-ray generation strategy through the analysis of microscopic and macroscopic processes. Using a CoTb alloy as a prototypical ferrimagnetic system, we retrieve the spin dynamics, and resolve a fast demagnetization time of 500 ± 126 f s , concomitant with an expansion of the domain periodicity, corresponding to a domain wall velocity of ∼ 750 m / s . The results confirm that, far from cross-contamination of low-energy absorption edges in multi-element systems, the highly localized states of 4 d electrons associated with the N 4 , 5 edges can provide high-quality core-level magnetic information on par with what can be obtained at the M edges, which is currently accessible only at large-scale x-ray facilities. The analysis also indicates the rich material-, composition-, and probing-energy-dependent driving mechanism of RE-associated multicomponent systems. Considering the rapid emergence of high-power Yb lasers combined with novel nonlinear compression technology, this work indicates potential for next-generation high-performance soft x-ray HHG-based sources in future extremely photon-hungry applications on the table-top scale, such as probing electronic motion in biologically relevant molecules in their physiological environment (liquid phase), and advanced coherent imaging of nano-engineered devices with 5 ∼ 8 n m resolution.

Multi-Lane Mirror for Broadband Applications of the Betatron X-ray Source

A new generation of small-scale ultrafast X-ray sources is rapidly emerging. Laser-driven betatron radiation represents an important class of such ultrafast X-ray sources. With the sources driving towards maturity, many important applications in material and biological sciences are expected to be carried out. While the last decade mainly focused on the optimization of the source properties, the development of such sources into user-oriented beamlines in order to explore the potential applications has recently taken off and is expected to grow rapidly. An important aspect in the realization of such beamlines will be the implementation of proper X-ray optics. Here, we present the design of a multi-lane X-ray mirror as a versatile focusing device covering a wide spectral range of betatron X-rays. The expected photon flux in the focal plane of such optics was also estimated through geometrical simulations.

Using the photoinduced L 3 resonance shift in Fe and Ni as time reference for ultrafast experiments at low flux soft x-ray sources.

We study the optical-pump induced ultrafast transient change of x-ray absorption at L3 absorption resonances of the transition metals Ni and Fe in the Fe0.5Ni0.5 alloy. We find the effect for both elements to occur simultaneously on a femtosecond timescale. This effect may hence be used as a handy cross correlation scheme, providing a time-zero reference for ultrafast optical-pump soft x-ray-probe measurement. The method benefits from a relatively simple experimental setup as the sample itself acts as time-reference tool. In particular, this technique works with low flux ultrafast soft x-ray sources. The measurements are compared to the cross correlation method introduced in an earlier publication.

Kilohertz Macromolecular Crystallography Using an EIGER Detector at Low X-ray Fluxes

Time-resolved in-house macromolecular crystallography is primarily limited by the capabilities of the in-house X-ray sources. These sources can only provide a time-averaged structure of the macromolecules. A significant effort has been made in the development of in-house laser-driven ultrafast X-ray sources, with one of the goals as realizing the visualization of the structural dynamics of macromolecules at a very short timescale within the laboratory-scale infrastructure. Most of such in-house ultrafast X-ray sources are operated at high repetition rates and usually deliver very low flux. Therefore, the necessity of a detector that can operate at the repetition rate of the laser and perform extremely well under low flux conditions is essential. Here, we present experimental results demonstrating the usability of the hybrid-pixel detectors, such as Eiger X 1M, and provide experimental proof that they can be successfully operated to collect macromolecular crystallographic data up to a detector frame rate of 3 kHz from synchrotron sources. Our results also show that the data reduction and structural analysis are successful at such high frame rates and fluxes as low as 108 photons/s, which is comparable to the values expected from a typical laser-driven X-ray source.

High-flux x-ray photon emission by a superluminal hybrid electromagnetic mode of intense laser in a plasma waveguide

The feasibility of several novel ultrafast x-ray sources has been demonstrated through the interaction between laser and a micro-structured target. However, the resulting photon flux is still deficient for some applications. Here, we proposed a new method to yield high-flux synchrotron radiation by adopting compact hollow plasma waveguide. We verified the method theoretically and numerically. Linearly polarized laser pulses propagating in the waveguide are mainly converted into the electromagnetic mode HE11 with a superluminal phase speed of 1.02c when the pulse is coupled with the waveguide. The mode fields lead to a strong oscillating force and short oscillation period for energetic electrons, which are accelerated via the longitudinal acceleration mechanism. Then, the short x-ray beam is generated with high yield of 1011–1012. The corresponding photon flux reaches 3.5 × 1021 photons s−1 · 0.1% bandwidth. The high-flux source can be even used for single shot ultrafast imaging or the ultrafast x-ray diffraction and absorption studies.

Recent advances in ultrafast X-ray sources.

Over more than a century, X-rays have transformed our understanding of the fundamental structure of matter and have been an indispensable tool for chemistry, physics, biology, materials science and related fields. Recent advances in ultrafast X-ray sources operating in the femtosecond to attosecond regimes have opened an important new frontier in X-ray science. These advances now enable: (i) sensitive probing of structural dynamics in matter on the fundamental timescales of atomic motion, (ii) element-specific probing of electronic structure and charge dynamics on fundamental timescales of electronic motion, and (iii) powerful new approaches for unravelling the coupling between electronic and atomic structural dynamics that underpin the properties and function of matter. Most notable is the recent realization of X-ray free-electron lasers (XFELs) with numerous new XFEL facilities in operation or under development worldwide. Advances in XFELs are complemented by advances in synchrotron-based and table-top laser-plasma X-ray sources now operating in the femtosecond regime, and laser-based high-order harmonic XUV sources operating in the attosecond regime. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.

Hard X-ray Generation from ZnO Nanowire Targets in a Non-Relativistic Regime of Laser-Solid Interactions

We present a detailed investigation of X-ray emission from both flat and nanowire zinc oxide targets irradiated by 60 fs 5 × 1016 W/cm2 intensity laser pulses at a 0.8 µm wavelength. It is shown that the fluence of the emitted hard X-ray radiation in the spectral range 150–800 keV is enhanced by at least one order of magnitude for nanowire targets compared to the emission from a flat surface, whereas the characteristic Kα line emission (8.64 keV) is insensitive to the target morphology. Furthermore, we provide evidence for a dramatic increase of the fast electron flux from the front side of the nanostructured targets. We suggest that targets with nanowire morphology may advance development of compact ultrafast X-ray sources with an enhanced flux of hard X-ray emission that could find wide applications in highenergy density (HED) physics.

Ultrafast X-Ray Spectroscopy of Conical Intersections.

Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level abinitio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S_{2}(ππ^{*}) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections.

Development of sub-100 femtosecond timing and synchronization system.

The precise timing and synchronization system is an essential part for the ultra-fast electron and X-ray sources based on the photocathode injector where strict synchronization among RF, laser, and beams are required. In this paper, we present an integrated sub-100 femtosecond timing and synchronization system developed and demonstrated recently in Tsinghua University based on the collaboration with Lawrence Berkeley National Lab. The timing and synchronization system includes the fiber-based CW carrier phase reference distribution system for delivering stabilized RF phase reference to multiple receiver clients, the Low Level RF (LLRF) control system to monitor and generate the phase and amplitude controllable pulse RF signal, and the laser-RF synchronization system for high precision synchronization between optical and RF signals. Each subsystem is characterized by its blocking structure and is also expansible. A novel asymmetric calibration sideband signal method was proposed for eliminating the non-linear distortion in the optical synchronization process. According to offline and online tests, the system can deliver a stable signal to each client and suppress the drift and jitter of the RF signal for the accelerator and the laser oscillator to less than 100 fs RMS (∼0.1° in 2856 MHz frequency). Moreover, a demo system with a LLRF client and a laser-RF synchronization client is deployed and operated successfully at the Tsinghua Thomson scattering X-ray source. The beam-based jitter measurement experiments have been conducted to evaluate the overall performance of the system, and the jitter sources are discussed.

Attosecond X-ray Diffraction Triggered by Core or Valence Ionization of a Dipeptide.

With the advancement of intense ultrafast X-ray sources, it is now possible to create a molecular movie by following the electronic dynamics in real time and real space through time-resolved X-ray diffraction. Here we employ real-time time-dependent density functional theory (RT-TDDFT) to simulate the electronic dynamics after an impulse core or valence ionization in the glycine-phenylalanine (GF) dipeptide. The time-evolving dipole moment, the charge density, and the time-resolved X-ray diffraction signals are calculated. The charge oscillation is calculated for 7 fs for valence ionization and 500 as for core ionization. The charge oscillation time scale is comparable to that found in a phenylalanine monomer (4 fs) [ Science 2014 , 346 , 336 ] and is slightly longer because of the elongated glycine chain. Following valence ionization, the charge migration across the GF is mediated by the delocalized lone-pair orbitals of oxygen and nitrogen of the electron-rich amide group. The temporal Fourier transform of the dipole moment provides detailed information on the charge migration dynamics and the molecular orbitals involved. Heterodyne-detected attosecond X-ray diffraction signals provide the magnitude and phase of the scattering amplitude in momentum space and can thus be inverted to yield the charge density in real space.

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today’s ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources.

Transient structure of thin films based on one-dimensional chain model

Functional materials have received much attention in the development of scientific technology. Macroscopic function of material is usually linked to the microscopic properties. In order to understand the relationship between structure and function, it is necessary to observe transient structural change of material in real time. In the earlier experimental work femtosecond optical probes were used to measure associated modulation in optical properties like transmissivity or reflectivity and extract the information about structural dynamics through sophisticated theoretical modeling. Since the development of laser-based ultrafast X-ray sources, there has been extensive work on femtosecond X-ray diffraction measurements. The coupling of sensitive X-ray with time-resolved pump-probe technique provides a way to directly monitor the time-dependent lattice structural changes in condensed matter. Recent researches are devoted to the study of non-thermal melting and coherent acoustic photons. The classical continuous elastic equation can only provide a limited view of structural dynamics. So, simulation of structural dynamics at an atomic level and comparison of such simulation with time-resolved X-ray diffraction data are necessary.#br#In this paper, we use the one-dimensional chain model to study the effect of thermal stress on the lattice due to the inhomogeneity of temperature distribution after ultrafast laser heating. It is developed from the classic continuous elastic equation by considering a nanometer film as a chain of point mass connected by springs. The simulation can directly reveal the positon of each point mass (atom) as a function of time for a given temperature (stress) profile. The simulation results accord very well with experimental data obtained with femtosecond X-ray diffraction. Compared with simulation results, the ultrafast X-ray diffraction experimental results are not enough to distinguish the compression near the zero time, but the characteristic time (~123 ps) and broadening of the diffraction peak are clearly observed. The simulation and experimental study of the lattice structural response are of great help for understanding the direct relationship between the lattice responses caused by ultrafast laser excitation, the generation and propagation of strain, one-dimensional chain model has important applications in studying the recoverable ultrafast lattice dynamics of metals, semiconductors and other materials.