arXiv subjects

O. G. Shpyrko

Publications and source records attributed to O. G. Shpyrko.

12 recordsLinked to original sources

arXiv2025

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↗

arXiv2024

Imaging ultrafast electronic domain fluctuations with X-ray speckle visibility

Speckle patterns manifesting from the interaction of coherent X-rays with matter offer a glimpse into the dynamics of nanoscale domains that underpin many emergent phenomena in quantum materials. While the dynamics of the average structure can be followed with time-resolved X-ray diffraction, the ultrafast evolution of local structures in nonequilibrium conditions have thus far eluded detection due to experimental limitations, such as insufficient X-ray coherent flux. Here we demonstrate a nonequilibrium speckle visibility experiment using a split-and-delay setup at an X-ray free-electron laser. Photoinduced electronic domain fluctuations of the magnetic model material Fe$_{3}$O$_{4}$ reveal changes of the trimeron network configuration due to charge dynamics that exhibit liquid-like fluctuations, analogous to a supercooled liquid phase. This suggests that ultrafast dynamics of electronic heterogeneities under optical stimuli are fundamentally different from thermally-driven ones.

cond-mat.str-el↗

arXiv2017

Nucleation of dislocations and their dynamics in layered oxides cathode materials during battery charging

Defects and their interactions in crystalline solids often underpin material properties and functionality as they are decisive for stability, result in enhanced diffusion, and act as a reservoir of vacancies. Recently, lithium-rich layered oxides have emerged among the leading candidates for the next-generation energy storage cathode material, delivering 50 % excess capacity over commercially used compounds. Oxygen-redox reactions are believed to be responsible for the excess capacity, however, voltage fading has prevented commercialization of these new materials. Despite extensive research the understanding of the mechanisms underpinning oxygen-redox reactions and voltage fade remain incomplete. Here, using operando three-dimensional Bragg coherent diffractive imaging, we directly observe nucleation of a mobile dislocation network in nanoparticles of lithium-rich layered oxide material. Surprisingly, we find that dislocations form more readily in the lithium-rich layered oxide material as compared with a conventional layered oxide material, suggesting a link between the defects and the anomalously high capacity in lithium-rich layered oxides. The formation of a network of partial dislocations dramatically alters the local lithium environment and contributes to the voltage fade. Based on our findings we design and demonstrate a method to recover the original high voltage functionality. Our findings reveal that the voltage fade in lithium-rich layered oxides is reversible and call for new paradigms for improved design of oxygen-redox active materials.

cond-mat.mtrl-sci↗

arXiv2017

Photoinduced Enhancement of the Charge Density Wave Amplitude

Symmetry breaking and the emergence of order is one of the most fascinating phenomena in condensed matter physics. It leads to a plethora of intriguing ground states found in antiferromagnets, Mott insulators, superconductors, and density-wave systems. Exploiting states of matter far from equilibrium can provide even more striking routes to symmetry-lowered, ordered states. Here, we demonstrate for the case of elemental chromium that moderate ultrafast photo-excitation can transiently enhance the charge-density-wave (CDW) amplitude by up to 30% above its equilibrium value, while strong excitations lead to an oscillating, large-amplitude CDW state that persists above the equilibrium transition temperature. Both effects result from dynamic electron-phonon interactions, providing an efficient mechanism to selectively transform a broad excitation of the electronic order into a well defined, long-lived coherent lattice vibration. This mechanism may be exploited to transiently enhance order parameters in other systems with coupled degrees of freedom.

cond-mat.str-el↗

arXiv2014

Condensation of collective charge ordering in Chromium

Here we report on the dynamics of the structural order parameter in a chromium film using synchrotron radiation in response to photo-induced ultra-fast excitations. Following transient optical excitations the effective lattice temperature of the film rises close to the Néel temperature and the charge density wave (CDW) amplitude is reduced. Although we expect the electronic charge ordering to vanish shortly after the excitation we observe that the CDW is never completely disrupted, which is revealed by its unmodified period at elevated temperatures. We attribute the persistence of the CDW to the long-lived periodic lattice displacement in chromium. The long-term evolution shows that the CDW revives to its initial strength within 1 ns, which appears to behave in accordance with the temperature dependence in equilibrium. This study highlights the fundamental role of the lattice distortion in charge ordered systems and its impact on the re-condensation dynamics of the charge ordered state in strongly correlated materials.

cond-mat.str-el↗

arXiv2012

Probing the three-dimensional strain inhomogeneity and equilibrium elastic properties of single crystal Ni nanowires

We employ three dimensional x-ray coherent diffraction imaging to map the lattice strain distribution, and to probe the elastic properties of a single crystalline Ni (001) nanowire grown vertically on an amorphous Si02 || Si substrate. The reconstructed density maps show that with increasing wire width, the equilibrium compressive stress in the core region decreases sharply while the surface tensile strain increases, and gradually trends to a nonzero constant. We use the retrieved projection of lattice distortion to predict the Young's Modulus of the wire based on the elasticity theory.

cond-mat.mes-hall↗

arXiv2011

Nanoscale imaging of the electronic and structural transitions in vanadium dioxide

We investigate the electronic and structural changes at the nanoscale in vanadium dioxide (VO2) in the vicinity of its thermally driven phase transition. Both electronic and structural changes exhibit phase coexistence leading to percolation. In addition, we observe a dichotomy between the local electronic and structural transitions. Nanoscale x-ray diffraction reveals local, non-monotonic switching of the lattice structure, a phenomenon that is not seen in the electronic insulator-to-metal transition mapped by near-field infrared microscopy.

cond-mat.str-el↗

arXiv2009

Infrared spectroscopy and nano-imaging of the insulator-to-metal transition in vanadium dioxide

We present a detailed infrared study of the insulator-to-metal transition (IMT) in vanadium dioxide (VO2) thin films. Conventional infrared spectroscopy was employed to investigate the IMT in the far-field. Scanning near-field infrared microscopy directly revealed the percolative IMT with increasing temperature. We confirmed that the phase transition is also percolative with cooling across the IMT. We present extensive near-field infrared images of phase coexistence in the IMT regime in VO2. We find that the coexisting insulating and metallic regions at a fixed temperature are static on the time scale of our measurements. A novel approach for analyzing the far-field and near-field infrared data within the Bruggeman effective medium theory was employed to extract the optical constants of the incipient metallic puddles at the onset of the IMT. We found divergent effective carrier mass in the metallic puddles that demonstrates the importance of electronic correlations to the IMT in VO2. We employ the extended dipole model for a quantitative analysis of the observed near-field infrared amplitude contrast and compare the results with those obtained with the basic dipole model.

cond-mat.str-el↗

arXiv2007

Pressure-Tuned Spin and Charge Ordering in an Itinerant Antiferromagnet

Elemental chromium orders antiferromagnetically near room temperature, but the ordering temperature can be driven to zero by applying large pressures. We combine diamond anvil cell and synchrotron x-ray diffraction techniques to measure directly the spin and charge order in the pure metal at the approach to its quantum critical point. Both spin and charge order are suppressed exponentially with pressure, well beyond the region where disorder cuts off such a simple evolution, and they maintain a harmonic scaling relationship over decades in scattering intensity. By comparing the development of the order parameter with that of the magnetic wavevector, it is possible to ascribe the destruction of antiferromagnetism to the growth in electron kinetic energy relative to the underlying magnetic exchange interaction.

cond-mat.str-el↗

arXiv2007

Direct measurement of antiferromagnetic domain fluctuations

Measurements of magnetic noise emanating from ferromagnets due to domain motion were first carried out nearly 100 years ago and have underpinned much science and technology. Antiferromagnets, which carry no net external magnetic dipole moment, yet have a periodic arrangement of the electron spins extending over macroscopic distances, should also display magnetic noise, but this must be sampled at spatial wavelengths of order several interatomic spacings, rather than the macroscopic scales characteristic of ferromagnets. Here we present the first direct measurement of the fluctuations in the nanometre-scale spin- (charge-) density wave superstructure associated with antiferromagnetism in elemental Chromium. The technique used is X-ray Photon Correlation Spectroscopy, where coherent x-ray diffraction produces a speckle pattern that serves as a "fingerprint" of a particular magnetic domain configuration. The temporal evolution of the patterns corresponds to domain walls advancing and retreating over micron distances. While the domain wall motion is thermally activated at temperatures above 100K, it is not so at lower temperatures, and indeed has a rate which saturates at a finite value - consistent with quantum fluctuations - on cooling below 40K. Our work is important because it provides an important new measurement tool for antiferromagnetic domain engineering as well as revealing a fundamental new fact about spin dynamics in the simplest antiferromagnet.

cond-mat.str-el↗

arXiv2006

Capillary Filling of Anodized Alumina Nanopore Arrays

The filling behavior of a room temperature solvent, perfluoromethylcyclohexane, in approximately 20 nm nanoporous alumina membranes was investigated in situ with small angle x-ray scattering. Adsorption in the pores was controlled reversibly by varying the chemical potential between the sample and a liquid reservoir via a thermal offset, $Δ$T. The system exhibited a pronounced hysteretic capillary filling transition as liquid was condensed into the nanopores. These results are compared with Kelvin-Cohan theory, with a modified Derjaguin approximation, as well as with predictions by Cole and Saam.

cond-mat.soft↗

arXiv2006

Microscopic and Macroscopic Signatures of Antiferromagnetic Domain Walls

Magnetotransport measurements on small single crystals of Cr, the elemental antiferromagnet, reveal the hysteretic thermodynamics of the domain structure. The temperature dependence of the transport coefficients is directly correlated with the real-space evolution of the domain configuration as recorded by x-ray microprobe imaging, revealing the effect of antiferromagnetic domain walls on electron transport. A single antiferromagnetic domain wall interface resistance is deduced to be of order $5\times10^{-5}\mathrm{μΩ\cdot cm^{2}}$ at a temperature of 100 K.

cond-mat.mtrl-sci↗