arXiv subjects

Natalia Gerasimova

Publications and source records attributed to Natalia Gerasimova.

14 recordsLinked to original sources

arXiv2026

Attosecond soft X-ray pulses generated by chirp-dispersed manipulation in an XFEL reveal nonlinear core-electron dynamics in neon

Free-electron lasers have demonstrated their capability of generating intense attosecond X-ray pulses, which are the key to studying electron dynamics at their natural time scale and in specifically targeted electronic states, but come at the expanse of complicated generation schemes and stochastic pulse shapes. Here, we demonstrate a novel and simple operation concept based on the manipulation of the electron-bunch chirp-dispersion and working with the full 4.5 MHz repetition rate at the European XFEL in Germany. With a high-fidelity single-shot temporal characterisation, we detect X-ray pulses with durations of down to 200 attoseconds and peak powers reaching into the terawatt regime at ~1 keV photon energy. As a direct application, we present simultaneous measurements of nonlinear X-ray-matter interaction via time-resolved electron spectroscopy. Using the derived temporal pulse information and restricting the durations to a regime where individual X-ray pulses are shorter than the single-core-hole life time in neon atoms, we reveal an otherwise hidden peak-intensity dependence in the nonlinear dynamics of double-core-hole formation. Our results open the field of attosecond science to the investigation of electronic processes not only in the ground state but also in systems driven far off their equilibrium. They shed light on highly transient intermediate steps in complex electronic dynamics and thus promise to help build the conceptual bridge between fundamental physical processes and chemical photo-reactions.

physics.optics↗

arXiv2026

Femtosecond spin-state switching dynamics of spin-crossover molecules condensed in thin films

The photoinduced switching of Fe(II)-based spin-crossover complexes from singlet to quintet takes place at ultrafast time scales. This a priori spin-forbidden transition triggered numerous time-resolved experiments of solvated samples to elucidate the mechanism at play. The involved intermediate states remain uncertain. We apply ultrafast x-ray spectroscopy in molecular films as a method sensitive to spin, electronic, and nuclear degrees of freedom. Combining the progress in molecule synthesis and film growth with the opportunities at x-ray free-electron lasers, we analyze the transient evolution of the Fe L3 fine structure at room temperature. Our measurements and calculations indicate the involvement of an Fe triplet intermediate state. The high-spin state saturates at half of the available molecules, limited by molecule-molecule interaction within the film.

cond-mat.mes-hall↗

arXiv2025

High frame rate RIXS spectroscopy using a JUNGFRAU detector with an iLGAD sensor

Resonant inelastic X-ray scattering (RIXS) is a powerful photon-in, photon-out spectroscopy technique for probing electronic, magnetic, and lattice excitations in matter. Time-resolved RIXS extends this capability through a stroboscopic optical pump-probe scheme to characterize the time evolution of the photoexcitation and subsequent relaxation dynamics of a sample. This technique is, however, extremely photon-hungry, requiring high-repetition-rate and intense X-ray facilities. The Heisenberg RIXS (hRIXS) spectrometer at the Spectroscopy and Coherent Scattering (SCS) instrument of the European X-ray Free-Electron Laser (EuXFEL) is designed to exploit high-repetition-rates, while maintaining optimal time and energy resolution. In this work, we demonstrate the successful deployment of a JUNGFRAU detector equipped with an inverse Low Gain Avalanche Diode (iLGAD) sensor for time-resolved RIXS studies in the soft X-ray range, using the hRIXS spectrometer. A spatial resolution of $19.71 \pm 0.7~μ\mathrm{m}$ and a resolving power exceeding 10,000 were achieved at an unprecedented frame rate of 47 kHz. Intra-train resolved data measured with a high FEL peak fluence of $1.8~\mathrm{mJ/cm^{2}}$ for a 928.5 eV ph photon energy and 1.1 MHz repetition rate from cupric oxide (CuO) revealed a decrease in the emitted signal by ~10% over a time interval of $340~μ\mathrm{s}$, indicating FEL-induced effects that require monitoring when conducting high-repetition-rate experiments. These results establish the JUNGFRAU-iLGAD as a promising detector to harvest the full potential of the hRIXS spectrometer, and validate its suitability for soft X-ray applications.

physics.ins-det↗

arXiv2025

Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering

Strong electronic correlation can lead to insulating behavior and to the opening of large optical gaps, even in materials with partly filled valence shells. Although the non-equilibrium optical response encodes both local (quasi atomic) and collective (long range) responses, optical spectroscopy is usually more sensitive to the latter. Resonant x-ray techniques are better suited to investigate the quasi-atomic properties of correlated solids. Using time-resolved resonant inelastic x-ray scattering (RIXS), here we study the ultrafast non-equilibrium processes in NiO following photo-excitation by ultraviolet photons with energy exceeding the optical gap. We observe the creation of charge-transfer excitons that decay with a time constant of about 2\,ps, while itinerant photo-doping persists for tens of picoseconds. Following our discovery, which establishes time-resolved high-resolution RIXS as a powerful tool for the study of transient phenomena in condensed matter, the possible presence of charge-transfer excitons will need to be considered when interpreting optical pump-probe experiments on correlated quantum materials.

cond-mat.str-el↗

arXiv2024

Analysis of long-lived effects in high-repetition-rate stroboscopic transient X-ray absorption experiments on thin films

Time-resolved X-ray absorption spectroscopy (tr-XAS) has been shown to be a versatile measurement technique for investigating non-equilibrium dynamics. Novel X-ray free electron laser (XFEL) facilities like the European XFEL offer increased repetition rates for stroboscopic XAS experiments through a burst operation mode, which enables measurements with up to 4.5 MHz. These higher repetition rates lead to higher data acquisition rates but can also introduce long-lived excitations that persist and thus build up during each burst. Here, we report on such long-lived effects in Ni and NiO thin film samples that were measured at the European XFEL. We disentangle the long-lived excitations from the initial pump-induced change and perform a detailed modelling-based analysis of how they modify transient X-ray spectra. As a result, we link the long-lived effects in Ni to a local temperature increase, as well as the effects in NiO to excited charge carrier trapping through polaron formation. In addition, we present possible correction methods, as well as discuss ways in which the effects of these long-lived excitations could be minimized for future time-resolved X-ray absorption spectroscopy measurements.

cond-mat.mtrl-sci↗

arXiv2024

The Heisenberg-RIXS instrument at the European XFEL

Resonant Inelastic X-ray Scattering (RIXS) is an ideal X-ray spectroscopy method to push the combination of energy and time resolutions to the Fourier transform ultimate limit, because it is unaffected by the core-hole lifetime energy broadening. And in pump-probe experiments the interaction time is made very short by the same core-hole lifetime. RIXS is very photon hungry so it takes great advantage from high repetition rate pulsed X-ray sources like the European XFEL. The hRIXS instrument is designed for RIXS experiments in the soft X-ray range with energy resolution approaching the Fourier and the Heisenberg limits. It is based on a spherical grating with variable line spacing (VLS) and a position-sensitive 2D detector. Initially, two gratings are installed to adequately cover the whole photon energy range. With optimized spot size on the sample and small pixel detector the energy resolution can be better than 40 meV at any photon energy below 1000 eV. At the SCS instrument of the European XFEL the spectrometer can be easily positioned thanks to air-pads on a high-quality floor, allowing the scattering angle to be continuously adjusted over the 65-145 deg range. It can be coupled to two different sample interaction chamber, one for liquid jets and one for solids, each equipped at the state-of-the-art and compatible for optical laser pumping in collinear geometry. The measured performances, in terms of energy resolution and count rate on the detector, closely match design expectations. hRIXS is open to public users since the summer of 2022.

cond-mat.str-el↗

arXiv2023

Transient non-collinear magnetic state for all-optical magnetization switching

Resonant absorption of a photon by bound electrons in a solid can promote an electron to another orbital state or transfer it to a neighboring atomic site. Such a transition in a magnetically ordered material could affect the magnetic order. While this process is an obvious road map for optical control of magnetization, experimental demonstration of such a process remains challenging. Exciting a significant fraction of magnetic ions requires a very intense incoming light beam, as orbital resonances are often weak compared to above-band-gap excitations. In the latter case, a sizeable reduction of the magnetization occurs as the absorbed energy increases the spin temperature, masking the non-thermal optical effects. Here, using ultrafast x-ray spectroscopy, we were able to resolve changes in the magnetization state induced by resonant absorption of infrared photons in Co-doped yttrium iron garnet, with negligible thermal effects. We found that the optical excitation of the Co ions affects the two distinct magnetic Fe sublattices differently, resulting in a transient non-collinear magnetic state. The present results indicate that the all-optical magnetization switching most likely occurs due to the creation of a transient, non-collinear magnetic state followed by coherent spin rotations of the Fe moments.

cond-mat.mtrl-sci↗

arXiv2023

Photon shot-noise limited transient absorption soft X-ray spectroscopy at the European XFEL

Femtosecond transient soft X-ray Absorption Spectroscopy (XAS) is a very promising technique that can be employed at X-ray Free Electron Lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here we present a dedicated setup for soft X-rays available at the Spectroscopy & Coherent Scattering (SCS) instrument at the European X-ray Free Electron Laser (EuXFEL). It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot-by-shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, the DSSC imaging detector, which is capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst, is employed and allows approaching the photon shot-noise limit. We review the setup and its capabilities, as well as the online and offline analysis tools provided to users.

physics.ins-det↗

arXiv2022

Electron Dynamics at High-Energy Densities in Nickel from Non-linear Resonant X-ray Absorption Spectra

The pulse intensity from X-ray free-electron lasers (FELs) can create extreme excitation densities in solids, entering the regime of non-linear X-ray-matter interactions. We show L3-edge absorption spectra of metallic nickel thin films with fluences entering a regime where several X-ray photons are incident per absorption cross-section. Main features of the observed non-linear spectral changes are described with a predictive rate model for electron population dynamics during the pulse, utilizing a fixed density of states and tabulated ground-state properties.

cond-mat.mtrl-sci↗

arXiv2022

The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni

The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. The interplay between the respective terms of the Hamiltonian is of fundamental interest, since it produces most, if not all, of the exotic phenomena observed in the solid state. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be caused by electron repopulation and correlation-induced modifications of the electronic structure, respectively. Importantly, the theoretical description of this experimental result hence requires to take the local Coulomb interaction into account, revealing a temporal interplay between band formation, exchange interaction, and Coulomb repulsion.

cond-mat.mtrl-sci↗

arXiv2021

Symmetry-dependent ultrafast manipulation of nanoscale magnetic domains

Symmetry is a powerful concept in physics, but its applicability to far-from-equilibrium states is still being understood. Recent attention has focused on how far-from-equilibrium states lead to spontaneous symmetry breaking. Conversely, ultrafast optical pumping can be used to drastically change the energy landscape and quench the magnetic order parameter in magnetic systems. Here, we find a distinct symmetry-dependent ultrafast behaviour by use of ultrafast x-ray scattering from magnetic patterns with varying degrees of isotropic and anisotropic symmetry. After pumping with an optical laser, the scattered intensity reveals a radial shift exclusive to the isotropic component and exhibits a faster recovery time from quenching for the anisotropic component. These features arise even when both symmetry components are concurrently measured, suggesting a correspondence between the excitation and the magnetic order symmetry. Our results underline the importance of symmetry as a critical variable to manipulate the magnetic order in the ultrafast regime.

cond-mat.mes-hall↗

arXiv2021

High spatial coherence and short pulse duration revealed by the Hanbury Brown and Twiss interferometry at the European XFEL

Second-order intensity interferometry was employed to study the spatial and temporal properties of the European X-ray Free-Electron Laser (EuXFEL). Measurements were performed at the soft X-ray SASE3 undulator beamline at a photon energy of 1.2 keV in the Self-Amplified Spontaneous Emission (SASE) mode. Two high-power regimes of the SASE3 undulator settings, i.e. linear and quadratic tapering at saturation, were studied in detail and compared with the linear gain regime. The statistical analysis showed an exceptionally high degree of spatial coherence up to 90% for the linear undulator tapering. Analysis of the measured data in spectral and spatial domains provided an average pulse duration of about 10 fs in our measurements. The obtained results will be valuable for the experiments requiring and exploiting short pulse duration and utilizing high coherence properties of the EuXFEL.

physics.optics↗

arXiv2018

ROSA: Reconstruction of Spectrogram Autocorrelation for Self-Amplified Spontaneous Emission Free-Electron Lasers

In recent years X-ray Free Electron Lasers (XFELs) proved to be unmatched sources of ultrashort pulses of spatially coherent quasimonochromatic X-ray radiation. Diagnostics of XFEL emission properties, in particular pulse duration, spectrum and temporal profile is extremely important in order to analyze the experimental results. In this paper we propose a cost-effective method to examine these properties of Self-Amplified Spontaneous Emission (SASE) pulses. It only requires an ensemble of measured SASE spectra and provides the temporal autocorrelation of the ensemble-averaged Wigner distribution of SASE FEL pulses.

physics.optics↗

arXiv2013

The monochromator beamline at FLASH: performance, capabilities and upgrade plans

The monochromator beamline at the FLASH facility at DESY is the worldwide first XUV monochromator beamline operational on a free electron laser (FEL)source. Being a single-user machine, FLASH demands a high flexibility of the instrumentation to fulfil the needs of diverse experiments performed by a multidisciplinary user community. Thus, the beamline has not only been used for high-resolution spectroscopy that it was originally designed for, but also for pump-probe experiments controlling the temporal-spectral properties at moderate resolution, and as a filter for high harmonics of the FEL at very low resolution. The present performance and capabilities of the beamline are discussed with emphasis on particularities arising from the nature of the FEL source, and current developments are presented aiming to enhance its capabilities for accommodating a wide variety of experiments.

physics.acc-ph↗