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O. Yu. Gorobtsov

Publications and source records attributed to O. Yu. Gorobtsov.

9 recordsLinked to original sources

Memory in strain-tuned insulator-metal-insulator sequence of transitions after photoexcitation in the Mott material V2O3

Memory effects during metal-insulator transitions in quantum materials reveal complex physics and potential for novel electronics mimicking biological neural systems. Nonetheless, understanding of memory and nonlinearity in sequential non-equilibrium transitions remains elusive as the full chain of transitions can involve features lasting anywhere from femtoseconds to microseconds. Here, we extend time-resolved x-ray Bragg diffraction to the dynamic range of timescales spanning 9 orders of magnitude to fully trace the pathways of photoexcited insulator-metal transition and the following relaxation through non-equilibrium metal-insulator transitions in epitaxial films of V2O3, a promising Mott material. We find 5 orders of magnitude variation in metal-insulator transition time, from nanoseconds to hundreds of microseconds, depending on pre-excitation phase state. We provide a theoretical explanation and simulations based on strain feedback to domain nucleation. The lingering transition is stretched in time by memory of spatial and energy heterogeneity and, contrary to known memory effects in vanadium oxides commonly described by power laws, follows an extremely (factor below 0.2) stretched exponential. The induced dramatic slowdown in the light-driven highly correlated system signifies unusually high heterogeneity of transition barriers similar to biological systems, and demonstrates importance of non-local correlations of structure in evolution of transitional phases in quantum materials.

cond-mat.mtrl-sci

Spontaneous supercrystal formation during a strain-engineered metal-insulator transition

Mott metal-insulator transitions possess electronic, magnetic, and structural degrees of freedom promising next generation energy-efficient electronics. We report a previously unknown, hierarchically ordered state during a Mott transition and demonstrate correlated switching of functional electronic properties. We elucidate in-situ formation of an intrinsic supercrystal in a Ca2RuO4 thin film. Machine learning-assisted X-ray nanodiffraction together with electron microscopy reveal multi-scale periodic domain formation at and below the film transition temperature (TFilm ~ 200-250 K) and a separate anisotropic spatial structure at and above TFilm. Local resistivity measurements imply an intrinsic coupling of the supercrystal orientation to the material's anisotropic conductivity. Our findings add an additional degree of complexity to the physical understanding of Mott transitions, opening opportunities for designing materials with tunable electronic properties.

cond-mat.mtrl-sci

Interaction and transformation of metastable defects in intercalation materials

Non-equilibrium defects often dictate macroscopic functional properties of materials. In intercalation hosts, widely used in rechargeable batteries, high-dimensional defects largely define reversibility and kinetics1,2,3,4. However, transient defects briefly appearing during ionic transport have been challenging to capture, limiting the understanding of their life cycle and impact. Here, we overcome this challenge and track operando the interaction and impact of metastable defects within NaxNi1-xMnyO2 intercalation hosts in a charging sodium-ion battery. Three-dimensional coherent X-ray imaging3,4,5 reveals transformation and self-healing of a metastable domain boundary, glissile dislocation loop, and stacking fault. A local strain gradient suggests a quantifiable difference in ion diffusion, coincident with the macroscopic change in diffusion coefficient. Analysis of the unexpected4,6 defect anisotropy highlights the importance of mesostructure, suggesting a possible control approach and disputing the rigidity of the framework layers. The shared nature of oxygen framework layers makes our results applicable to a wide range of intercalation materials.

cond-mat.mtrl-sci

Seeded x-ray free-electron laser generating radiation with laser statistical properties

The invention of optical lasers led to a revolution in the field of optics and even to the creation of completely new fields of research such as quantum optics. The reason was their unique statistical and coherence properties. The newly emerging, short-wavelength free-electron lasers (FELs) are sources of very bright coherent extreme-ultraviolet (XUV) and x-ray radiation with pulse durations on the order of femtoseconds, and are presently considered to be laser sources at these energies. Most existing FELs are highly spatially coherent but in spite of their name, they behave statistically as chaotic sources. Here, we demonstrate experimentally, by combining Hanbury Brown and Twiss (HBT) interferometry with spectral measurements that the seeded XUV FERMI FEL-2 source does indeed behave statistically as a laser. The first steps have been taken towards exploiting the first-order coherence of FELs, and the present work opens the way to quantum optics experiments that strongly rely on high-order statistical properties of the radiation.

physics.optics

Diffraction based Hanbury Brown and Twiss interferometry performed at a hard x-ray free-electron laser

We demonstrate experimentally Hanbury Brown and Twiss (HBT) interferometry at a hard X-ray Free Electron Laser (XFEL) on a sample diffraction patterns. This is different from the traditional approach when HBT interferometry requires direct beam measurements in absence of the sample. HBT analysis was carried out on the Bragg peaks from the colloidal crystals measured at Linac Coherent Light Source (LCLS). We observed high degree (80%) spatial coherence of the full beam and the pulse duration of the monochromatized beam on the order of 11 fs that is significantly shorter than expected from the electron bunch measurements.

physics.optics

Structural studies of the bond-orientational order and hexatic-smectic transition in liquid crystals of various compositions

We report on X-ray studies of freely suspended hexatic films of three different liquid crystal compounds. By applying angular X-ray cross-correlation analysis (XCCA) to the measured diffraction patterns the parameters of the bond-orientational (BO) order in the hexatic phase were directly determined. The temperature evolution of the BO order parameters was analyzed on the basis of the multicritical scaling theory (MCST). Our results confirmed the validity of the MCST in the whole temperature range of existence of the hexatic phase for all three compounds. The temperature dependence of the BO order parameters in the vicinity of the hexatic-smectic transition was fitted by a conventional power law with a critical exponent $β\approx0.1$ of extremely small value. We found that the temperature dependence of higher order harmonics of the BO order scales as the powers of the first harmonic, with exponent equal to harmonic number. This indicates a nonlinear coupling of the BO order parameters of different order. It is shown that compounds of various composition, possessing different phase sequences, display the same thermodynamic behavior in the hexatic phase and in the vicinity of the smectic-hexatic phase transition.

cond-mat.soft

Statistical properties of a free-electron laser revealed by the Hanbury Brown and Twiss interferometry

We present a comprehensive experimental analysis of statistical properties of the self-amplified spontaneous emission (SASE) free-electron laser (FEL) FLASH at DESY in Hamburg by means of Hanbury Brown and Twiss (HBT) interferometry. The experiments were performed at the FEL wavelengths of 5.5 nm, 13.4 nm, and 20.8 nm. We determined the 2-nd order intensity correlation function for all wavelengths and different operation conditions of FLASH. In all experiments a high degree of spatial coherence (above 50%) was obtained. Our analysis performed in spatial and spectral domains provided us with the independent measurements of an average pulse duration of the FEL that were below 60 fs. To explain complicated behaviour of the 2-nd order intensity correlation function we developed advanced theoretical model that includes the presence of multiple beams and external positional jitter of the FEL pulses. By this analysis we determined that in most experiments several beams were present in radiating field and in one of the experiments external positional jitter was about 25% of the beam size. We envision that methods developed in our study will be used widely for analysis and diagnostics of the FEL radiation.

physics.optics

Phase of the transmitted wave in the dynamical theory and quasi-kinematical approximation

Variation of the phase of the beam transmitted through a crystalline material as a function of the rocking angle is a well known dynamical effect in x-ray scattering. Unfortunately, it is not so easy to measure directly these phase variations in a conventional scattering experiment. It was recently suggested that the transmitted phase can be directly measured in ptychography experiments performed on nanocrystal samples. Results of such experiment for different crystal thickness, reflections and incoming photon energies, in principle, can be fully described in the frame of dynamical theory. However, dynamical theory does not provide a simple analytical expression for the further analysis. We develop here quasi-kinematical theory approach that allows to describe correctly the phase of the transmitted beam for the crystal thickness less than extinction length that is beyond applicability of the conventional kinematical theory.

cond-mat.mtrl-sci

Theoretical study of electronic damage in single particle imaging experiments at XFELs for pulse durations 0.1 - 10 fs

X-ray free-electron lasers (XFELs) may allow to employ the single particle imaging (SPI) method to determine the structure of macromolecules that do not form stable crystals. Ultrashort pulses of 10 fs and less allow to outrun complete disintegration by Coulomb explosion and minimize radiation damage due to nuclear motion, but electronic damage is still present. The major contribution to the electronic damage comes from the plasma generated in the sample that is strongly dependent on the amount of Auger ionization. Since the Auger process has a characteristic time scale on the order of femtoseconds, one may expect that its contribution will be significantly reduced for attosecond pulses. Here, we study the effect of electronic damage on the SPI at pulse durations from 0.1 fs to 10 fs and in a large range of XFEL fluences to determine optimal conditions for imaging of biological samples. We analyzed the contribution of different electronic excitation processes and found that at fluences higher than $10^{13}$-$10^{15}$ photons/$μ$m$^2$ (depending on the photon energy and pulse duration) the diffracted signal saturates and does not increase further. A significant gain in the signal is obtained by reducing the pulse duration from 10 fs to 1 fs. Pulses below 1 fs duration do not give a significant gain in the scattering signal in comparison with 1 fs pulses. We also study the limits imposed on SPI by Compton scattering.

physics.bio-ph