arXiv subjects

Sergii Parchenko

Publications and source records attributed to Sergii Parchenko.

At least 19 recordsLinked to original sources

arXiv2025

Collective Magnetic Excitations in a Photo-excited Electron-doped Cuprate Superconductor

Elucidating the microscopic behavior of cuprates under ultrafast photoexcitation offers critical insights into their highly correlated out-of-equilibrium states. Although quasiparticle dynamics have been investigated extensively, the behavior of collective magnetic excitations remains comparatively unexplored. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu $L_3$-edge to track the collective magnetic excitations (paramagnons) in an optimally electron-doped cuprate driven out-of-equilibrium by a femtosecond pump laser pulse. Upon pumping, we observed an anti-Stokes signal associated with paramagnon generation, which modifies the paramagnon dispersion near the zone center, although the bandwidth remained unchanged. Moreover, the spectral weight exhibits a momentum-dependent variation across the Brillouin zone. The light-driven boost of the paramagnon population and the resulting spectral-weight transfer could provide new leverage to manipulate the properties of cuprates.

cond-mat.mtrl-sci↗

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 $19.71 \pm 0.7~\mu\mathrm{m}$ 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 $340~\mu\mathrm{s}$, 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

Anomalous spin dynamics after dual optical excitation

Ultrashort optical pulses are a cornerstone for manipulating electronic and magnetic states in materials on a femtosecond timescale. Conventional models assume that optical excitation primarily modifies the occupation of the electron energy levels without long-lasting altering of the coupling of individual electrons in certain processes. Here, we demonstrate that optical excitation with two femtosecond pulses that come from different directions fundamentally transforms the electron dynamics in copper, affecting the efficiency of angular momentum transfer between electrons and the lattice. Using time-resolved magneto-optical Kerr effect measurements, we reveal a ~2.5. increase in spin imbalance decay time following inverse Faraday effect excitation under dual-pump conditions compared to single-pulse excitation. This observation challenges the prevailing paradigm of ultrafast light-matter interactions, showing that dual optical excitation can transiently modify electron dynamics beyond simple changes in the energy levels occupancy. Our findings open new avenues for controlling quantum states through a dual pump approach, with implications for ultrafast spintronics and the design of novel light-driven states.

cond-mat.mtrl-sci↗

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↗

arXiv2025

Ultrafast decoupling of polarization and strain in ferroelectric BaTiO$_3$

A fundamental understanding of the interplay between lattice structure, polarization and electrons is pivotal to the optical control of ferroelectrics. The interaction between light and matter enables the remote and wireless control of the ferroelectric polarization on the picosecond timescale, while inducing strain, i.e., lattice deformation. At equilibrium, the ferroelectric polarization is proportional to the strain, and is typically assumed to be so also out of equilibrium. Decoupling the polarization from the strain would remove the constraint of sample design and provide an effective knob to manipulate the polarization by light. Here, upon an above-bandgap laser excitation of the prototypical ferroelectric BaTiO$_3$, we induce and measure an ultrafast decoupling between polarization and strain that begins within 350 fs, by softening Ti-O bonds via charge transfer, and lasts for several tens of picoseconds. We show that the ferroelectric polarization out of equilibrium is mainly determined by photoexcited electrons, instead of the strain. This excited state could serve as a starting point to achieve stable and reversible polarization switching via THz light. Our results demonstrate a light-induced transient and reversible control of the ferroelectric polarization and offer a pathway to control by light both electric and magnetic degrees of freedom in multiferroics.

cond-mat.mtrl-sci↗

arXiv2024

Magnetic resonance frequency of two-sublattice ferrimagnet with magnetic compensation temperature

Ferrimagnetic materials with a compensation temperature have recently attracted interest because of their unique combination of ferromagnetic and antiferromagnetic properties. However, their magnetization dynamics near the compensation temperature are complex and cannot be fully explained by conventional ferromagnetic resonance (FMR) or exchange resonance modes. Therefore, practical models are necessary to capture these dynamics accurately. In this study, we derived the analytical solutions for the magnetic resonance frequencies of compensated ferrimagnets over all temperature ranges, considering both the in-plane and out-of-plane orientations of the magnetization. Our solutions successfully reproduce the experimental data obtained from time-resolved magneto-optical Faraday rotation and Brillouin light scattering measurements for the in-plane and out-of-plane cases, respectively. This reproduction is achieved by incorporating the exchange stiffness and temperature dependence of the magnetic anisotropy into the free energy density. Additionally, at temperatures sufficiently far from the compensation temperature, our analytical solutions converge with the conventional FMR and exchange resonance models.

cond-mat.mtrl-sci↗

arXiv2024

Demagnetization dynamics after noncollinear dual optical excitation

We explore the impact of optical excitation using two interfering ultrashort optical pulses on ultrafast magnetization dynamics. Our investigation focuses on Pt/Co/Pt multilayers and TbCo alloy samples, employing a dual pump approach. We observe significant variations in the dynamics of magnetization suppression and subsequent recovery when triggered with two optical pulses of the same polarization-essentially meeting conditions for interference. Conversely, dynamics triggered with cross-polarized pump beams exhibit expected similarity to that triggered with a single pulse. Delving into the underlying physical processes contributing to laser-induced demagnetization and recovery dynamics, we find that our current understanding cannot elucidate the observed trends. Consequently, we propose that optical excitation with interfering light possesses not previously acknowledged capacity to induce long-lasting alterations in the dynamics of angular momentum.

physics.optics↗

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

Optically Induced Ferromagnetic Order in a Ferrimagnet

The parallel or antiparallel arrangement of electron spins plays a pivotal role in determining the properties of a physical system. To meet the demands for innovative technological solutions, extensive efforts have been dedicated to exploring effective methods for controlling and manipulating this arrangement [1]. Among various techniques, ultrashort laser pulses have emerged as an exceptionally efficient tool to influence magnetic order. Ultrafast suppression of the magnetic order [2,3], all-optical magnetization switching [4, 5, 6, 7], and light-induced magnetic phase transitions [8] are just a few notable examples. However, the transient nature of light-induced changes in the magnetic state has been a significant limitation, hindering their practical implementation. In this study, we demonstrate that infrared ultrashort laser pulses can induce a ferromagnetic arrangement of magnetic moments in an amorphous TbCo alloy, a material that exhibits ferrimagnetism under equilibrium conditions. Strikingly, the observed changes in the magnetic properties persist for significantly longer durations than any previously reported findings. Our results reveal that ultrashort optical pulses can generate materials with identical chemical composition and structural state but entirely distinct magnetic arrangements, leading to unique magnetic properties. This breakthrough discovery marks a new era in light-driven control of matter, offering the exciting potential to create materials with properties that were once considered unattainable.

cond-mat.mtrl-sci↗

arXiv2023

Plasmon-enhanced optical control of magnetism at the nanoscale via the inverse Faraday effect

The relationship between magnetization and light has been the subject of intensive research for the past century, focusing on the impact of magnetic moments on light polarization. Conversely, the manipulation of magnetism through polarized light is being investigated to achieve all-optical control of magnetism in spintronics. While remarkable discoveries such as single pulse all-optical switching of the magnetization in thin films and sub-micrometer structures have been reported, the demonstration of local optical control of magnetism at the nanoscale has remained elusive. Here, we show that exciting gold nanodiscs with circularly polarized femtosecond laser pulses leads to the generation of sizeable local magnetic fields that enable ultrafast local control of the magnetization of an adjacent magnetic film. In addition, we find that the highest magnetic fields are generated when exciting the sample at a wavelength larger than that of the actual plasmonic resonance of the gold nanodiscs, so avoiding undesired heating effects due to absorption. Our study paves the way for light-driven control in nanoscale spintronic devices and provides important insights into the generation of magnetic fields in plasmonic nanostructures.

physics.optics↗

arXiv2023

Magnetization precession after non-collinear dual optical excitation

We investigate the impact of non-collinear dual optical excitation on the magnetization precession in a permalloy thin film using two ultrashort laser pulses. By analyzing the magnetization dynamics using time-resolved magneto-optical methods, we find that the excitation with two ultrashort optical pulses introduces a long-lasting modification of the electron system seen as a sizable decrease of the precession frequency and significant increase (about 25%) of the decay time. Our results reveal that the observed effect strongly depends on the respective polarization of the two excitation pulses and the time delay between two optical pulses. Our findings indicate the occurrence of a new nonlinear opto-spin effect during photoexcitation with two interfering optical pulses which can potentially be observed in various materials and at different photon wavelengths.

cond-mat.mtrl-sci↗

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↗

arXiv2022

Giant magnetic anisotropy in the atomically thin van der Waals antiferromagnet FePS3

Van der Waals (vdW) magnets are an ideal platform for tailoring two-dimensional (2D) magnetism with immense potential for spintronics applications and are intensively investigated. However, little is known about the microscopic origin of magnetic order in these antiferromagnetic systems. We used X-ray photoemission electron microscopy to address the electronic and magnetic properties of the vdW antiferromagnet FePS3 down to the monolayer. Our experiments reveal a giant out-of-plane magnetic anisotropy of 22 meV per Fe ion, accompanied by unquenched magnetic orbital moments. Moreover, our calculations suggest that the Ising magnetism in FePS3 is a visible manifestation of spin-orbit entanglement of the Fe 3d electron system.

cond-mat.mes-hall↗

arXiv2022

Direct observation of a dynamical glass transition in a nanomagnetic artificial Hopfield network

Spin glasses, generally defined as disordered systems with randomized competing interactions, are a widely investigated complex system. Theoretical models describing spin glasses are broadly used in other complex systems, such as those describing brain function, error-correcting codes, or stock-market dynamics. This wide interest in spin glasses provides strong motivation to generate an artificial spin glass within the framework of artificial spin ice systems. Here, we present the experimental realization of an artificial spin glass consisting of dipolar coupled single-domain Ising-type nanomagnets arranged onto an interaction network that replicates the aspects of a Hopfield neural network. Using cryogenic x-ray photoemission electron microscopy (XPEEM), we performed temperature-dependent imaging of thermally driven moment fluctuations within these networks and observed characteristic features of a two-dimensional Ising spin glass. Specifically, the temperature dependence of the spin glass correlation function follows a power law trend predicted from theoretical models on two-dimensional spin glasses. Furthermore, we observe clear signatures of the hard to observe rugged spin glass free energy in the form of sub-aging, out of equilibrium autocorrelations and a transition from stable to unstable dynamics.

cond-mat.dis-nn↗

arXiv2022

Photoinduced structural dynamics of multiferroic TbMnO$_3$

We use time-resolved hard x-ray diffraction to investigate the structural dynamics of the multiferroic insulator TbMnO$_3$ in the low temperature antiferromagnetic and ferroelectrically ordered phase. The lattice response following photoexcitation at 1.55 eV is detected by measuring the (0 2 4) and (1 3 -5) Bragg reflections. A 0.02% tensile strain, normal to the surface, is seen to arise within 20 - 30 ps. The magnitude of this transient strain is over an order of magnitude lower than that predicted from laser-induced heating, which we attribute to a bottleneck in the energy transfer between the electronic and lattice subsystems. The timescale for the transient expansion is consistent with that of previously reported demagnetization dynamics. We discuss a possible relationship between structural and demagnetization dynamics in TbMnO$_3$, in which photoinduced atomic motion modulates the exchange interaction, leading to a destruction of the magnetic order in the system.

cond-mat.str-el↗

arXiv2020

Structurally assisted melting of excitonic correlations in 1T-TiSe2

The simultaneous condensation of electronic and structural degrees of freedom gives rise to new states of matter, including superconductivity and charge-density-wave formation. When exciting such a condensed system, it is commonly assumed that the ultrafast laser pulse disturbs primarily the electronic order, which in turn destabilizes the atomic structure. Contrary to this conception, we show here that structural destabilization of few atoms causes melting of the macroscopic ordered charge-density wave in 1T-TiSe2. Using ultrafast pump-probe non-resonant and resonant X-ray diffraction, we observe full suppression of the Se 4p orbital order and the atomic structure at excitation energies more than one order of magnitude below the suggested excitonic binding energy. Complete melting of the charge-density wave occurs 4-5 times faster than expected from a purely electronic charge-screening process, strongly suggesting a structurally assisted breakup of excitonic correlations. Our experimental data clarifies several questions on the intricate coupling between structural and electronic order in stabilizing the charge-density-wave in 1T-TiSe2. The results further show that electron-phonon-coupling can lead to different, energy dependent phase-transition pathways in condensed matter systems, opening new possibilities in the conception of non-equilibrium phenomena at the ultrafast scale.

cond-mat.str-el↗

arXiv2020

Correlation between electronic and structural orders in 1T-TiSe2

The correlation between electronic and crystal structures of 1T-TiSe2 in the charge density wave (CDW) state is studied by x-ray diffraction. Three families of reflections are used to probe atomic displacements and the orbital asymmetry in Se. Two distinct onset temperatures are found, TCDW and a lower T* indicative for an onset of Se out-of-plane atomic displacements. T* coincides with a DC resistivity maximum and the onset of the proposed gyrotropic electronic structure. However, no indication for chirality is found. The relation between the atomic displacements and the transport properties is discussed in terms of Ti 3d and Se 4p states that only weakly couple to the CDW order.

cond-mat.str-el↗

arXiv2020

Ultrafast electron localization in a correlated metal

Ultrafast electron delocalization induced by a fs laser pulse is a well-known process and is the initial step for important applications such as fragmentation of molecules or laser ablation in solids. It is well understood that an intense fs laser pulse can remove several electrons from an atom within its pulse duration. [1] However, the speed of electron localization out of an electron gas, the capture of an electron by ion, is unknown. Here, we demonstrate that electronic localization out of the conduction band can occur within only a few hundred femtoseconds. This ultrafast electron localization into 4f states has been directly quantified by transient x-ray absorption spectroscopy following photo-excitation of a Eu based correlated metal with a fs laser pulse. Our x-ray experiments show that the driving force for this process is either an ultrafast reduction of the energy of the 4f states, a change of their bandwidth or an increase of the hybridization between the 4f and the 3d states. The observed ultrafast electron localization process raises further basic questions for our understanding of electron correlations and their coupling to the lattice.

cond-mat.str-el↗