In this study, we employ classical molecular dynamics (MD) simulations to investigate the crystallisation kinetics of supercooled liquid palladium and relate the results to time-resolved X-ray diffraction measurements on rapidly quenched Pd thin films. Crystal nucleation and growth rates are determined over the temperature range 700–1150 K (0.38–0.65 T_m) by analysing the evolution of the microstructure during the liquid-to-crystal transition. The self-diffusion coefficient of Pd, obtained from the atomic mean-squared displacement, follows Arrhenius behaviour over the investigated temperature range, with an activation energy of 467(6) meV/atom, consistent with available data for supercooled liquid metals. The steady-state homogeneous nucleation rate exhibits a maximum of approximately 4 × 10^35 m^-3 s^-1 near 0.5 T_m. Crystal growth occurs at velocities of the order of metres per second, with a temperature dependence consistent with diffusion-limited Wilson-Frenkel kinetics rather than the collision-limited regime. Based on multiple statistically independent simulations, a time-temperature-transformation (TTT) diagram for crystallisation onset is constructed. The TTT curve exhibits a nose near 0.5 T_m and 100 ps, corresponding to a critical cooling rate for vitrification on the order of 10^13 K s^-1. The simulations reproduce the crystallisation onset time and temperature observed in time-resolved X-ray diffraction experiments on optically molten Pd thin films quenched at 5 × 10^11 K s^-1. These results indicate that homogeneous, rather than heterogeneous, nucleation governs the achievable supercooling in the experimentally studied films.

We report time-resolved diffuse extreme ultraviolet (EUV) scattering measurements of optically excited acoustic waves in thin Ti/SiN bilayers in transmission geometry. Following femtosecond optical excitation, the EUV diffuse scattering signal yields circular fringe patterns evolving as a function of the time delay between the optical pump and EUV probe pulses. We demonstrate that these patterns originate from multiple guided acoustic modes (Lamb waves) with wavelengths in the range 60–400 nm. By comparing the experimental frequency–wavevector maps with calculated dispersion curves, we show that diffuse scattering signal from Lamb waves is enhanced at discrete frequencies corresponding to longitudinal thickness resonances of the membrane. This observation indicates that Lamb waves with high in-plane wavevectors originate from the scattering of longitudinal thickness resonances by surface roughness. Our findings establish time-resolved diffuse EUV scattering as an efficient tool for probing nanoscale Lamb waves, applicable to the characterization of elastic properties of thin membranes.

The laser-induced fabrication of nanostructures with feature sizes below the optical diffraction limit is possible for almost any material for arbitrary sample geometries and dimensions by exploiting nonlinear excitations or optical near-field interactions. This overview highlights historical milestones, explains the underlying physical processes and associated challenges, and discusses current and future trends in the field of ultrafast laser nanostructuring.

Nanoscale miniaturization has revolutionized the field of spintronics by enabling exponential growth in areal bit density. A similar leap is also expected in device speeds through successfully harnessing femtosecond magnetization dynamics. However, combining this with the miniaturization of realistic devices is challenging. To address this, we studied the effect of dimensional confinement on the femtosecond demagnetization of Fe. By gradually increasing the level of confinement while keeping excitation conditions constant, we found that Fe layers thinner than 10 nm exhibit enlarged demagnetization amplitudes, reaching a ∼75% increase at 2 nm. By combining ultrafast experiments sensitive to the spins, the charge carriers, and the phonons, we establish that this finite-size effect is magnetic in origin and is not phonon-driven. With the support of ab-initio calculations and atomistic spin dynamics simulations, we identify the enhancement effect as due to local weakening of spin order at the Fe's interface, which becomes significant upon increased confinement.

In this study, we employ classical molecular dynamics (MD) simulations to investigate the crystallisation kinetics of supercooled liquid palladium and relate the results to time-resolved X-ray diffraction measurements on rapidly quenched Pd thin films. Crystal nucleation and growth rates are determined over the temperature range 700–1150 K (0.38–0.65 Tm) by analysing the evolution of the microstructure during the liquid-to-crystal transition. The self-diffusion coefficient of Pd, obtained from the atomic mean-squared displacement, follows Arrhenius behaviour over the investigated temperature range, with an activation energy of 467(6) meV/atom, consistent with available data for supercooled liquid metals. The steady-state homogeneous nucleation rate exhibits a maximum of approximately 4×10^35 m^-3 s^-1 near 0.5 Tm. Crystal growth occurs at velocities of the order of meters per second, with a temperature dependence consistent with diffusion-limited Wilson–Frenkel kinetics rather than the collision-limited regime. Based on multiple statistically independent simulations, a time–temperature–transformation (TTT) diagram for crystallisation onset is constructed. The TTT curve exhibits a nose near 0.5 Tm and 100 ps, corresponding to a critical cooling rate for vitrification on the order of 10^13 K/s. The simulations reproduce the crystallisation onset time and temperature observed in time-resolved X-ray diffraction experiments on optically molten Pd thin films quenched at 5×10^11 K/s. These results indicate that homogeneous, rather than heterogeneous, nucleation governs the achievable supercooling in the experimentally studied films.

Laser ablation is a process that bears both fundamental physics interest and has wide industrial applications. For decades, the lack of probes on the relevant time and length scales has prevented access to the highly nonequilibrium phase decomposition processes triggered by laser excitation. In this study, a close integration of time-resolved probing by intense femtosecond X-ray pulses with large-scale atomistic modeling has yielded unique insights into the ablation dynamics of thin gold films irradiated by femtosecond laser pulses. The emergence and growth of nanoscale density heterogeneities in the expanding ablation plume, predicted in the simulations, are mapped to the rapid evolution of distinct small angle diffraction features. This mapping enables identification of the characteristic signatures of different phase decomposition processes occurring simultaneously in the plume, which are driven by photomechanical and thermodynamic driving forces. Beyond the specific insights into the ablation phenomenon, this study demonstrates the power of joint X-ray probing and atomistic modeling of material dynamics under extreme conditions of thermal and mechanical nonequilibrium.

Material processing with femtosecond lasers has attracted enormous attention because of its potential for technology and industrial applications. In parallel, time-resolved x-ray diffraction has been successfully used to study ultrafast structural distortion dynamics in semiconductor thin films or surface layers. However, real-world processing applications mostly are concerned with bulk materials, which prevents the use of x-ray surface based techniques. For processing applications, a fast and depth-sensitive probe is needed. To address this, we present a novel technique based on ultrafast x-ray dynamical diffraction (UDD) capable of imaging transient strain distributions inside bulk crystals upon laser excitation. This pump-probe technique provides a complete picture of thetemporal evolution of ultrafast distorted lattice depth profiles. We demonstrate the potential of UDD by studying a thin Si single crystal upon single pulse femtosecond optical excitation. Our study reveals that below the melting threshold strong lattice distortions not only longitudinal, but also transversal to the propagation of the strain wave appear on picosecond time scales along the single crystal. The observation of this transversal deformation after laser excitation contradicts previous work that were not able to observed it, what could be related to the high sensitivity of dynamical diffraction with respect to the lattice distortions. The speed of propagation of this ultrafast transversal strain deformation is observed to be slower to the longitudinal sound speed for Si as described in the bibliography.

The primary distinction between solid and liquid phases is mechanical rigidity, with liquids having a disordered atomic structure that allows flow. While melting is a common phase transition, its microscopic mechanisms still remain unclear. This study uses molecular dynamics simulations to investigate ultrafast melting in polycrystalline palladium, focusing on the relationship between atomic dynamics quantified by the root-mean-squared displacement (RMSD) and local structural disorder characterized by the deviation from centrosymmetry. In the crystal bulk, melting is preceded by a gradual rise in the RMSD and local disorder. As the Lindemann limit for the RMSD is approached, the increasing concentration of lattice defects is manifested by a discontinuous rise in disorder. On melting, the rise is followed by a rapid increase in displacement, indicative of atomic flow. In contrast, the grain boundaries undergo melting through a continuous increase of both the displacement and the disorder, resembling a glass transition on heating.

Glass-forming liquids exhibit structural relaxation behaviors, reflecting underlying atomic rearrangements on a wide range of timescales and playing a crucial role in determining material properties. However, the relaxation processes on the atomic scale are not well-understood due to the experimental difficulties in directly characterizing the evolving correlations of atomic-scale order in disordered systems. Here, we harness the coherence and ultrashort pulse characteristics of an x-ray free electron laser to directly probe atomic-scale ultrafast relaxation dynamics in the model system Ge15Te85. We demonstrate an analysis strategy for determining the intermediate scattering function by extracting the contrast decay of summed scattering patterns from two rapidly successive, nearly identical femtosecond x-ray pulses generated by a split-delay system. The result indicates a full decorrelation of atomic-scale order on the sub-picosecond timescale, supporting the argument for a high-fluidity fragile state of liquid Ge15Te85 above its dynamic crossover temperature. The demonstrated strategy opens an avenue for experimental studies of relaxation dynamics in liquids, glasses, and other highly disordered systems.

In this work, we describe an X-ray pump/X-ray probe delay line with limited view tomographic capability, called X-ray Tomographic-dElay-Line (XTEL). This optical system is designed for studying pico- to nanosecond dynamics of mesoscale materials processes at existing X-ray light sources. The XTEL was built in a 1-beam configuration and was tested on the Macromolecular Femtosecond Crystallography (MFX) instrument at the Linac Coherent Light Source (LCLS). The relative intensity of the probe vs. pump beam was measured to be 0.4% ± 0.1% and the instrument pointing was stable to within the rocking curve width of the crystal optics over multiple days. We also show the conceptual design for an XTEL-like optic with delays in the picosecond range, enabling the study of diffusion in the warm dense matter regime.

We present a table-top setup for femtosecond time-resolved x-ray diffraction based on a Cu Kα (8.05 keV) laser driven plasma x-ray source. Due to its modular design, it provides high accessibility to its individual components (e.g., x-ray optics and sample environment). The Kα-yield of the source is optimized using a pre-pulse scheme. A magnifying multilayer x-ray mirror with Montel–Helios geometry is used to collect the emitted radiation, resulting in a quasi-collimated flux of more than 105 Cu Kα photons/pulse impinging on the sample under investigation at a repetition rate of 10 Hz. A gas ionization chamber detector is placed right after the x-ray mirror and used for the normalization of the diffraction signals, enabling the measurement of relative signal changes of less than 1% even at the given low repetition rate. Time-resolved diffraction experiments on laser-excited epitaxial Bi films serve as an example to demonstrate the capabilities of the setup. The setup can also be used for Debye–Scherrer type measurements on poly-crystalline samples.

This keynote presentation addresses the advantages, recent developments, and perspectives of laser processing with ultrashort laser pulses. A special focus is laid on the tailored structuring of thin films as well as the manufacturing and probing of sub-diffraction surface nanostructures – an ongoing race to extreme scales. Current limitations are identified and an outlook to future scaling perspectives will be provided.

We have studied ultrafast structural transformations in sub-picosecond laser-excited metals - thin Fe and Pd layers. The temporal evolution of the samples' state was characterized using the x-ray diffraction technique at XFEL facility. The application of the ultrashort (fs) x-ray pulses allowed to direct probe the atomic structure of the sample with an unprecedentedly high temporal resolution of ~500 fs (relevant for the ultrafast rates of studied processes). The experimental results were compared with molecular dynamics simulations. The proposed experimental approach is matching the timescales of experimental and computational studies of structural transformations. It enabled new insight into the atomic-level mechanisms and kinetics of ultrafast phase transitions.

Glass forming liquids exhibit structural relaxation behaviors, reflecting underlying atomic rearrangements on a wide range of timescales. These behaviors play a crucial role in determining many material properties. However, the relaxation processes on the atomic scale are not well understood due to the experimental difficulties in directly characterizing the evolving correlations of atomic order in disordered systems. Here, taking the model system Ge15Te85, we demonstrate an experimental approach that probes the relaxation dynamics by scattering the coherent X-ray pulses with femtosecond duration produced by X-ray free electron lasers (XFELs). By collecting the summed speckle patterns from two rapidly successive, nearly identical X-ray pulses generated using a split-delay system, we can extract the contrast decay of speckle patterns originating from sample dynamics and observe the full decorrelation of local order on the sub-picosecond timescale. This provides the direct atomic-level evidence of fragile liquid behavior of Ge15Te85. Our results demonstrate the strategy for XFEL-based X-ray photon correlation spectroscopy (XPCS), attaining femtosecond temporal and atomic-scale spatial resolutions. This twelve orders of magnitude extension from the millisecond regime of synchrotron-based XPCS opens a new avenue of experimental studies of relaxation dynamics in liquids, glasses, and other highly disordered systems.

Irradiation of solid surfaces with high intensity, ultrashort laser pulses triggers a variety of secondary processes that can lead to the formation of transient and permanent structures over a large range of length scales from mm down to the nano‐range. One of the most prominent examples are LIPSS – Laser‐Induced Periodic Surface Structures. While LIPSS have been a scientific evergreen for of almost 60 years, experimental methods that combine ultrafast temporal with the required nm spatial resolution have become available only recently with the advent of short pulse, short wavelength free electron lasers. Here, the current status and future perspectives in this field are discussed by exploiting the unique possibilities of these 4th‐generation light sources to address by time‐domain experimental techniques the fundamental LIPSS‐question, namely why and how laser irradiation can initiate the transition of a “chaotic” (rough) surface from an aperiodic into a periodic structure.

Light-matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

The tailoring of spin-crossover films has made significant progress over the past decade, mostly motivated by the prospect in technological applications. In contrast to spin-crossover complexes in solution, the investigation of the ultrafast switching in spin-crossover films has remained scarce. Combining the progress in molecule synthesis and film growth with the opportunities at X-ray free-electron lasers, we study the photoinduced spin-state switching dynamics of a molecular film at room temperature. The subpicosecond switching from the S = 0 low-spin ground state to the S = 2 high-spin state is monitored by analyzing the transient evolution of the Fe L3 X-ray absorption edge fine structure, i.e. element-specifically at the switching center of the Fe(II) complex. Our measurements show the involvement of an intermediate state in the switching. At large excitation fluences, the fraction of high-spin molecules saturates at ≈50%, which is likely due to molecule-molecule interaction within the film.