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Andrei Benediktovitch

Publications and source records attributed to Andrei Benediktovitch.

17 recordsLinked to original sources

Generation of high-fluence and high-intensity hard x-ray attosecond pulses at European XFEL

By combining hard x-ray attosecond pulses from the European XFEL with total-reflection focusing x-ray optics, we generated nanofocused hard x-ray attosecond pulses with intensities and fluences comparable to the highest values attained in the hard x-ray regime. A peak intensity on the order of 10$^{20}$ W/cm$^2$ is confirmed through the observation of saturation in amplified spontaneous emission from copper atoms. These x-ray pulses enable new scientific opportunities, including the exploration of higher-order nonlinear light--matter interactions, damage-free structure determination, and coherent control of atoms and molecules.

physics.optics↗

X-ray Coherent Attosecond Pulse Pair Spectroscopy

X-ray free electron laser (XFEL) experiments using self-amplified spontaneous emission (SASE) pulses typically achieve temporal resolutions of order several femtoseconds, as the pulse duration puts a practical limit to pump-probe or probe-probe schemes. Even with the emerging capabilities to generate pulses with attosecond durations with new single-spike SASE schemes, direct access to attosecond electron dynamics remains an experimental challenge. Here we show how X-ray coherent attosecond pulse-pair spectroscopy (X-CAPPS) provides a powerful new approach to access the ultrashort time-delay window. Coherent attosecond pulse pairs with time delays varying from ~500 as to ~5 fs are generated with Cu K$α_1$ stimulated X-ray emission from a gain medium pumped by intense SASE XFEL pulses. These pulse pairs are analyzed with two subsequent Bragg crystal spectrometers, and the resulting interference spectrum is captured on two sequential 2D image detectors encoding their time separation, relative amplitudes, and phases with high precision. X-CAPPS requires no split-and-delay X-ray optics, nor XFEL pulse modifications, making it broadly implementable across existing facilities. This technique enables the investigation of attosecond processes with $\mathring{A}$ngström resolution, providing a new tool for probing ultrafast dynamics across a wide range of atomic, molecular, and solid systems.

physics.optics↗

Theory of x-ray scattering from optically pumped excitons in atomically thin semiconductors

We propose a framework to explore the internal charge distribution of mesoscopic quasiparticles by inelastic x-ray scattering, while also accounting for the conventional scattering from electrons. Specifically, we investigate a new contribution of intrinsic and optically pumped excitons (bound electron-hole pairs) to the x-ray scattering spectrum of transition metal dichalcogenides (TMDCs). The optical excitation leads to the creation of Wannier exciton populations, adding new quasi-elastic processes beyond the conventional electronic features to the x-ray scattering spectra. Differential spectra (with and without optical pumping) can be used to isolate and identify the internal charge distribution of the optically pumped excitons in the scattering response, potentially offering insights into many-body interactions and quasi-particle dynamics in 2D systems.

cond-mat.mes-hall↗

Spin waves excited by hard x-ray transient gratings

Recent progress in ultrafast x-ray sources helped establish x-rays as an important tool for probing lattice and magnetic dynamics initiated by femtosecond optical pulses. Here, we explore the potential of ultrashort hard x-ray pulses for driving magnetic dynamics. We use a transient grating technique in which a spatially periodic x-ray excitation pattern gives rise to material excitations at a well-defined wave vector, whose dynamics are monitored via diffraction of an optical probe pulse. The excitation of a ferrimagnetic gadolinium bismuth iron garnet film placed in an external tilted magnetic field by x-rays at the Gd L3 edge results in both magnetic and non-magnetic transient gratings whose contributions to the diffracted signal are separated by polarization analysis. We observe the magnetization precession at both longitudinal acoustic and spin wave frequencies. An analysis with the Landau-Lifshitz-Gilbert equation indicates that the magnetization precession is driven by strain resulting from thermal expansion induced by absorbed x-rays. The results establish x-ray transient gratings as a tool for driving coherent phonons and magnons, with the potential of accessing wave vectors across the entire Brillouin zone.

physics.optics↗

Attosecond Inner-Shell Lasing at Angstrom Wavelengths

Since the invention of the laser nonlinear effects such as filamentation, Rabi-cycling and collective emission have been explored in the optical regime leading to a wide range of scientific and industrial applications. X-ray free electron lasers (XFELs) have led to the extension of many optical techniques to X-rays for their advantages of angstrom scale spatial resolution and elemental specificity. One such example is XFEL driven population inversion of 1s core hole states resulting in inner-shell K$α$ (2p to 1s) X-ray lasing in elements ranging from neon to copper, which has been utilized for nonlinear spectroscopy and development of next generation X-ray laser sources. Here we show that strong lasing effects, similar to those observed in the optical regime, can occur at 1.5 to 2.1 angstrom wavelengths during high intensity (> ${10^{19}}$ W/cm${^{2}}$) XFEL driven inner-shell lasing and superfluorescence of copper and manganese. Depending on the temporal substructure of the XFEL pump pulses(containing ${~10^{6}}$ - ${10^{8}}$ photons) i, the resulting inner-shell X-ray laser pulses can exhibit strong spatial inhomogeneities as well as spectral splitting, inhomogeneities and broadening. Through 3D Maxwell Bloch theory we show that the observed spatial inhomogeneities result from X-ray filamentation, and that the spectral splitting and broadening is driven by Rabi cycling with sub-femtosecond periods. Our simulations indicate that these X-ray pulses can have pulse lengths of less than 100 attoseconds and coherence properties that open the door for quantum X-ray optics applications.

physics.optics↗

Experimentally constrained wave function method

In this work, we extend the x-ray constrained wavefunction fitting approach, a key method in quantum crystallography for charge density reconstruction, to incorporate experimental observables beyond x-ray diffraction. Unlike traditional quantum crystallography methods, which are typically limited to molecules in their ground states, our approach integrates excited states. This advancement will enable simultaneous fitting of x-ray diffraction data alongside optical and x-ray spectroscopic data. We introduce a comprehensive theoretical framework that allows for the inclusion of any experimental observable as a constraint in wavefunction reconstruction. Furthermore, we provide detailed derivations and instructions for implementation of this method using two electronicstructure methods: a generalized Hartree-Fock method for excited states and the Coupled Cluster Equation-of-motion method.

quant-ph↗

Stochastic modeling of superfluorescence in compact systems

We propose an approach based on stochastic differential equations to describe superfluorescence in compact ensembles of multi-level emitters in the presence of various incoherent processes. This approach has a numerical complexity that does not depend on the number of emitters. The stochastic differential equations are derived directly from the quantum master equation. In this study, we present a series of numerical examples, comparing our solution to exact calculations and discussing the limits of applicability. For many relevant cases, the proposed stochastic differential equations provide accurate results and correctly capture quantum many-body correlation effects.

quant-ph↗

Stochastic modeling of x-ray superfluorescence

An approach to modeling the dynamics of x-ray amplified spontaneous emission and superfluorescence -- the phenomenon of collective x-ray emission initiated by intense pulses of X-ray Free Electron Lasers -- is developed based on stochastic partial differential equations. The equations are derived from first principles, and the relevant approximations, derivation steps, and extensions specific to stimulated x-ray emission are presented. The resulting equations take the form of three-dimensional generalized Maxwell-Bloch equations augmented with noise terms for both field and atomic variables. The derived noise terms possess specific correlation properties that enable the correct reconstruction of spontaneous emission. Consequently, the developed theoretical formalism is universally suitable for describing all stages of stimulated x-ray emission: spontaneous emission, amplified spontaneous emission, and superfluorescence. We present numerical examples that illustrate various properties of the emitted field, including spatio-temporal coherence, spectral-angular and polarization characteristics. We anticipate that the proposed theoretical framework will establish a robust foundation for interpreting measurements in stimulated x-ray emission spectroscopy, modeling x-ray laser oscillators, and describing other experiments leveraging x-ray superfluorescence.

quant-ph↗

XLO-II, a high-repetition rate X-ray laser oscillator

In a recent paper we proposed to build an x-ray laser oscillator (XLO) in the 6-10 keV range providing intense, stable, transform-limited, x-ray pulses based on population inversion driven by an x-ray pulse train generated by an x-ray free-electron laser (XFEL) operated at a repetition rate of about 100 Hz. Here we present an analysis of recent experimental results on x-ray lasing with population inversion, damage caused by the pump on the lasing medium, and optical cavities, together with theoretical/numerical simulations. Our findings suggest that it is possible to build and operate a second-generation x-ray laser oscillator, XLO-II, operating at up to 125 kHz repetition rate. XLO-II will be pumped by 6-10 keV x-ray SASE pulses, generated by the new LCLS-II-HE XFEL now under construction at SLAC National Accelerator Laboratory, utilizing a CW superconducting linac and capable of running at 1 MHz repetition rate. XLO-II will generate transform-limited, coherent x-ray pulses with an average power in the tens of mW range. It will open new experimental capabilities, for instance in fields like imaging, interferometry, and quantum x-ray optics. The main characteristics of XLO-II and its main components, including the optical cavity, will be discussed.

physics.acc-ph↗

Quantum stochastic trajectories for particles and fields based on positive P-representation

In this work we introduce a phase-space description based on the positive P representation for bosonic fields interacting with a system of quantum emitters. The formalism is applicable to collective light-matter interactions and open quantum systems with decoherence. Conservation of particle numbers is considered, and a Jordan-Schwinger transformation enables the representation of multi-level quantum emitters. The evolution of the phase-space description of the combined system of emitters and field is formulated in terms of stochastic trajectories and we derive the rules of mapping from traditional quantum mechanics to this stochastic formalism. The resulting equations of motion encode deterministic, classical evolution with quantum effects incorporated by stochastic noise terms. The framework's equations and properties are provided without specifying the Hamiltonian, aiming for broad applicability in diverse research domains. A potential future application is the quantum mechanical description of collective spontaneous emission of an incoherently pumped ensemble of atoms.

quant-ph↗

Generation of Intense Phase-Stable Femtosecond Hard X-ray Pulse Pairs

Coherent nonlinear spectroscopies and imaging in the X-ray domain provide direct insight into the coupled motions of electrons and nuclei with resolution on the electronic length and time scale. The experimental realization of such techniques will strongly benefit from access to intense, coherent pairs of femtosecond X-ray pulses. We have observed phase-stable X-ray pulse pairs containing more thank 3 x 10e7 photons at 5.9 keV (2.1 Angstrom) with about 1 fs duration and 2-5 fs separation. The highly directional pulse pairs are manifested by interference fringes in the superfluorescent and seeded stimulated manganese K-alpha emission induced by an X-ray free-electron laser. The fringes constitute the time-frequency X-ray analogue of the Young double-slit interference allowing for frequency-domain X-ray measurements with attosecond time resolution.

physics.atom-ph↗

Towards novel probes for valence charges via X-ray optical wave mixing

We present a combined theoretical and experimental study of X-ray optical wave mixing. This class of nonlinear phenomena combines the strengths of spectroscopic techniques from the optical domain, with the high-resolution capabilities of X-rays. In particular, the spectroscopic sensitivity of these phenomena can be exploited to selectively probe valence dynamics. Specifically, we focus on the effect of X-ray parametric down-conversion. We present a theoretical description of the process, from which we deduce the observable nonlinear response of valence charges. Subsequently, we simulate scattering patterns for realistic conditions and identify characteristic signatures of the nonlinear conversion. For the observation of this signature, we present a dedicated experimental setup and results of a detailed investigation. However, we do not find evidence of the nonlinear effect. This finding stands in strong contradiction to previous claims of proof-of-principle demonstrations. Nevertheless, we are optimistic to employ related X-ray optical wave mixing processes on the basis of the methods presented here for probing valence dynamics in the future.

physics.optics↗

Self amplification of channeling radiation at Bragg diffraction conditions

X-ray radiation of relativistic electrons passing through the crystal lattice (in case of channeling radiation) requires electrons with energies just from tens up to hundreds MeV, but has a drawback: low number of emitted X-ray quanta. However, the brightness of such a source could be potentially increased if the current density of the electron bunch is high enough to initiate the self amplified spontaneous emission (SASE) process. The conditions at which this phenomenon could take place for the case of axial channeling are analyzed in the present paper within the first order perturbation theory. The transition from spontaneous to SASE regime is described, the requirements for bunch current parameters initiating SASE process are determined taking into account the periodic structure of the crystal medium. It is also shown that satisfying Bragg diffraction conditions could enhance self amplification. Numerical results for the case of axial channeling in Si, Ge and C crystals are presented as an example.

physics.acc-ph↗

Radiation of a Charge Moving in a Wire Structure

A theoretical approach for describing the electromagnetic radiation produced by prolonged electron bunch propagating in the lattice of metallic wires of finite length is presented. This approach is based on vibrator antenna theory and involves approximate solving of Hallen's integral equation. For a single wire, it is also supposed that a wire is sufficiently thin and charge motion is relativistic. For many-wire structures, the approximation similar to kinematic approach of parametric X-ray radiation (PXR) theory is additionally applied. The validity of the method is verified by numerical simulations with COMSOL Multiphysics. Possible applications of interaction between charged particle bunches and artificial wire structures are discussed.

physics.acc-ph↗

Quantum theory of superfluorescence based on two-point correlation functions

Irradiation of a medium by short intense pulses from x-ray / XUV free electron lasers can result in saturated photoionization of inner electronic shells. As a result an inversion of populations between core levels appears. The resulting fluorescent radiation can be amplified during its propagation through the inverted medium and results in intense, quasi transform-limited radiation bursts. While the optical counterpart of this phenomena, known as superfluorescence, was intensively investigated, a generalized treatment is needed in the x-ray / XUV domain, where the dynamics of pumping and evolution due to fast decay processes play a crucial role. To provide a general theoretical approach, we start from the fundamental, quantized minimal coupling Hamiltonian of light-matter interaction and after a series of approximations arrive at a closed system of equations for the two-point correlation function of atomic coherences and the two-time correlation function of the emitted field. The obtained formalism enables us to investigate collective spontaneous emission in various regimes. It is extended consistently to include incoherent processes that are relevant in the x-ray / XUV domain. These processes are introduced into the formalism by corresponding Lindblad superoperators. The connection to other approaches is discussed and numerical examples related to recent experiments are presented.

quant-ph↗

Bunches of misfit dislocations on the onset of relaxation of Si$_{0.4}$Ge$_{0.6}$/Si(001) epitaxial films revealed by high-resolution x-ray diffraction

The experimental x-ray diffraction patterns of a Si$_{0.4}$Ge$_{0.6}$/Si(001) epitaxial film with a low density of misfit dislocations are modeled by the Monte Carlo method. It is shown that an inhomogeneous distribution of 60$^\circ$ dislocations with dislocations arranged in bunches is needed to explain the experiment correctly. As a result of the dislocation bunching, the positions of the x-ray diffraction peaks do not correspond to the average dislocation density but reveal less than a half of the actual relaxation.

cond-mat.mtrl-sci↗

Linear Theory Analysis of Self-Amplified Parametric X-ray Radiation from High Current Density Electron Bunches

Linear theory of the parametric beam instability or the self-amplification of parametric x-ray radiation (PXR) from relativistic electrons in a crystal is considered taking into account finite emittance of the electron beam and absorption of the radiation. It is shown that these factors change essentially the estimation of threshold parameters of the electron bunches for the coherent X-ray generation. The boundary conditions for the linear theory of the effect is analyzed in details and it is shown that the grazing incidence diffraction geometry is optimal for the growth of instability. Numerical estimations of amplification and coherent photon yield in dependence on the electron current density are presented for the case of mm-thickness Si crystal and 100 MeV electrons. Possible improvements of the experimental scheme for optimization of the coherent radiation intensity are discussed.

physics.acc-ph↗