arXiv subjects

Dmitry Reznik

Publications and source records attributed to Dmitry Reznik.

At least 19 recordsLinked to original sources

arXiv2026

Temperature-Dependent Raman Signatures of Local Symmetry Breaking in Vacancy Double Perovskite Cs$_2$SnI$_6$

Understanding and controlling the optical, thermal and mechanical properties of K$_2$PtCl$_6$-type double perovskites is essential for the design of lead-free, high-performance thermoelectric and optoelectronic materials. In this study, we investigate Cs$_2$SnI$_6$ using temperature-dependent near-resonance Raman scattering, complemented by density functional theory-based phonon calculations. The appearance of Raman-forbidden phonon modes in the Raman response at cryogenic temperatures provides strong evidence for local symmetry breaking that does not develop into a global structural phase transition. Through detailed analysis of phonon intensities, energies, and spectral lineshapes, we characterize the temperature evolution of the symmetry-broken structural response of Cs$_2$SnI$_6$. Below 200 K, multi-phonon scattering is strongly enhanced, and symmetry-forbidden Raman modes emerge. The temperature dependence of phonon intensities follows a phenomenological Arrhenius behavior, revealing an activation energy of 15-20 meV. These results establish temperature-dependent Raman spectroscopy as a sensitive probe of local structural distortions and anharmonic structural dynamics in Cs$_2$SnI$_6$, providing a robust experimental basis for discussing the microscopic origins of symmetry breaking and electron-phonon coupling in halide double perovskites.

cond-mat.mtrl-sci↗

arXiv2026

Harnessing Electrostructural Bistability to Control Defects in Polarizable Materials

Structural defects are central to the functionalities of materials. However, conventional approaches to defect control are often slow and imprecise. This work identifies and characterizes a distinct physical phenomenon of electrostructural bistability that provides a rapid and precise pathway for engineering materials with defect-controlled physical properties. A generalized theory of conductivity bistability is developed and experimentally validated to unify two distinct regimes: previously reported electrothermal bistability in weakly polarizable insulators, such as silicon, and electrostructural bistability in strongly polarizable materials, such as TiO$_2$. In agreement with the theory, experiments on TiO$_2$ demonstrate that bulk-homogeneous defect concentrations in electrostructurally bistable materials can be tuned rapidly and deterministically by controlling applied electric current. Abruptly interrupting the current quenches the system into long-lived, room-temperature metastable states with distinct properties. This establishes a practical, rapid, and scalable pathway for defect engineering with direct relevance to nonvolatile memory devices.

cond-mat.mtrl-sci↗

arXiv2026

Collapse of Jahn-Teller Phonons in La$_{1-x}$Sr$_{x}$MnO$_3$ with Weak Magnetoresistance

Perovskite manganites are quantum materials exhibiting competing interactions inducing colossal magnetoresistance (CMR). The prevailing theory of CMR highlights the essential role of electron-phonon coupling (EPC), but mounting evidence suggests the underlying mechanism is more complicated. Here, we investigate phonons and spin-phonon coupling in ferromagnetic CMR manganites La$_{1-x}$Sr$_x$MnO$_3$ ($x$=0.2,0.3) with relatively small CMR associated with melting of the magnetic order above room temperature. High-resolution neutron scattering experiments combined with density functional theory (DFT) show that the low-temperature ferromagnetic phase is conventional: neutron scattering from phonons agrees with DFT predictions and magnons follow sinusoidal dispersions. Fluctuating magnetic moments and low-energy phonons remain conventional in the high temperature paramagnetic phase, indicating the Mn and La/Sr sublattices are not strongly perturbed by melting of ferromagnetism. In contrast, the Jahn-Teller-active optical oxygen vibrations collapse entirely above the Curie temperature, despite low CMR in these compositions, with some of the lost spectral weight reappearing as quasielastic scattering. We attribute this highly anomalous behavior to giant EPC in the charge and/or orbital channel. It drives cooperative diffusive motion of quasistatic carrier-trapping oxygen sublattice distortions once ferromagnetism disappears. We hypothesize the magnitude of magnetoresistance correlates with the rate of diffusion rather than with the strength of Jahn-Teller EPC.

cond-mat.mtrl-sci↗

arXiv2024

Gapped commensurate antiferromagnetic response in a strongly underdoped model cuprate superconductor

It is a distinct possibility that spin fluctuations are the pairing interactions in a wide range of unconventional superconductors. In the case of the high-transition-temperature (high-$T_c$) cuprates, in which superconductivity emerges upon doping an antiferromagnetic Mott-insulating state, spin correlations might furthermore drive unusual pseudogap phenomena. Here we use polarized and unpolarized magnetic neutron scattering to study the simple tetragonal cuprate $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$ at very low doping ($T_c \approx 55$ K, hole concentration $p \approx 0.064$). In stark contrast to prior results for other underdoped cuprates, we find no evidence of incommensurate spin-density-wave, charge-spin stripe, or $q = 0$ magnetic order. Instead, the antiferromagnetic response in both the superconducting and pseudogap states is gapped below $Δ_\mathrm{AF} \approx 6$ meV, commensurate over a wide energy range, and disperses above about 55 meV. Given the documented model nature of $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$, which exhibits high structural symmetry and minimal point disorder effects, we conclude that the observed behavior signifies the unmasked response of the quintessential $\mathrm{CuO}_{2}$ planes near the Mott-insulating state. These results for $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$ can therefore be expected to serve as a benchmark for a refined theoretical understanding of the cuprates.

cond-mat.supr-con↗

arXiv2024

Structural and electronic transformations in TiO2 induced by electric current

In-situ diffuse neutron scattering experiments revealed that when electric current is passed through single crystals of rutile TiO2 under conditions conducive to flash sintering, it induces the formation of parallel planes of oxygen vacancies. Specifically, a current perpendicular to the c-axis generates planes normal to the (132) reciprocal lattice vector, whereas currents aligned with the c-axis form planes normal to the (132) and to the (225) vector. The concentration of defects increases with incresing current. The structural modifications are linked to the appearance of signatures of interacting Ti3+ moments in magnetic susceptibility, signifying a structural collapse around the vacancy planes. Electrical conductivity measurements of the modified material reveal several electronic transitions between semiconducting states (via a metal-like intermediate state) with the smallest gap being 27 meV. Pristine TiO2 can be restored by heating followed by slow cooling in air. Our work suggests a novel paradigm for achieving switching of electrical conductivity related to the flash phenomenon

cond-mat.mtrl-sci↗

arXiv2024

Magneto-synthesis effect on magnetic order, phonons, and magnons in single-crystal Sr$_2$IrO$_4$

It was shown earlier that applying a magnetic field during the growth of Sr$_2$IrO$_4$, also known as "field-alteration", induces significant changes to its structural, magnetic, and transport properties. However, the microscopic nature of these changes is enigmatic. In this study, we employed resonant elastic and inelastic x-ray scattering, as well as Raman scattering, to investigate samples from two batches of Sr$_2$IrO$_4$ grown in magnetic fields of different strengths. Our findings reveal that samples grown in a weaker magnetic field have similar magnetic order to non-altered samples, whereas those grown in a stronger field show a different stacking of weak in-plane ferromagnetic moments. Additionally, we observed significant softening and broadening of select Raman-active phonons in the field altered samples, with a stronger effect in the samples grown in the stronger field. We discuss insights that our results provide into the microscopic nature of field-alteration in Sr$_2$IrO$_4$.

cond-mat.str-el↗

arXiv2023

Structural changes induced by electric currents in a single crystal of Pr$_2$CuO$_4$

We demonstrate a novel approach to the structural and electronic property modification of perovskites, focusing on Pr$_2$CuO$_4$, an undoped parent compound of a class of electron-doped copper-oxide superconductors. Currents were passed parallel or perpendicular to the copper-oxygen layers with the voltage ramped up until a rapid drop in the resistivity was achieved, a process referred to as "flash". The current was then further increased tenfold in current-control mode. This state was quenched by immersion into liquid nitrogen. Flash can drive many compounds into different atomic structures with new properties, whereas the quench freezes them into a long-lived state. Single-crystal neutron diffraction of as-grown and modified Pr$_2$CuO$_4$ revealed a $\sqrt{10}$x$\sqrt{10}$ superlattice due to oxygen-vacancy order. The diffraction peak intensities of the superlattice of the modified sample were significantly enhanced relative to the pristine sample. Raman-active phonons in the modified sample were considerably sharper. Measurements of electrical resistivity, magnetization and two-magnon Raman scattering indicate that the modification affected only the Pr-O layers, but not the Cu-O planes. These results point to enhanced oxygen-vacancy order in the modified samples well beyond what can be achieved without passing electrical current. Our work opens a new avenue toward electric field/quench control of structure and properties of layered perovskite oxides.

cond-mat.supr-con↗

arXiv2023

The nature of dynamic local order in CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$

Hybrid lead halide perovskites (LHPs) are a class of semiconductor with novel properties that are distinctively governed by structural fluctuations. Diffraction experiments sensitive to average, long-range order reveal a cubic structure in the device-relevant, high-temperature phase. Local probes find additional short-range order with lower symmetry that may govern the structure-function relationships of LHPs. However, the dimensionality, participating atoms, and dynamics of this short-range order are unresolved, impeding our understanding of technologically relevant properties including long carrier lifetimes and facile halide migration. Here, we determine the true structure of two prototypical hybrid LHPs, CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$, using a combination of single-crystal X-ray and neutron diffuse scattering, neutron inelastic spectroscopy, and molecular dynamics simulations. The remarkable collective dynamics we found are not suggested by previous studies and consist of a network of local two-dimensional, circular pancake-like regions of dynamically tilting lead halide octahedra (lower symmetry) that induce longer range intermolecular correlations within the CH$_3$NH$_3^+$ sublattice. The dynamic local structure can introduce transient ferroelectric or antiferroelectric domains that increase charge carrier lifetimes, and strongly affect the halide migration, a poorly understood degradation mechanism. Our approach of co-analyzing single-crystal X-ray and neutron diffuse scattering data with MD simulations will provide unparalleled insights into the structure of hybrid materials and materials with engineered disorder.

cond-mat.mtrl-sci↗

arXiv2023

Occupational Disorder as the Origin of Flattening of the Acoustic Phonon Branches in the Clathrate Ba$_{8}$Ga$_{16}$Ge$_{30}$

In the search for high-performance thermoelectrics, materials such as clathrates have drawn attention due to having both glass-like low phonon thermal conductivity and crystal-like high electrical conductivity. Ba$_{8}$Ga$_{16}$Ge$_{30}$ (BGG) has a loosely bound guest Ba atom trapped inside rigid Ga/Ge cage structures. Avoided crossings between acoustic phonons and the flat guest atom branches have been proposed to be the source of the low lattice thermal conductivity of BGG. Ga/Ge site disorder with Ga and Ge exchanging places in different unit cells has also been reported. We used time-of-flight neutron scattering to measure the complete phonon spectrum in a large single crystal of BGG and compared these results with predictions of density functional theory to elucidate the effect of the disorder on heat-carrying phonons. Experimental results agreed much better with the calculation assuming the disorder than with the calculation assuming the ordered configuration. Although atomic masses of Ga and Ge are nearly identical, we found that disorder strongly reduces phonon group velocities, which significantly reduces thermal conductivity. Our work points at a new path towards optimizing thermoelectrics.

cond-mat.mtrl-sci↗

arXiv2022

Electron-momentum dependence of electron-phonon coupling underlies dramatic phonon renormalization in YNi$_2$B$_2$C

Electron-phonon coupling, i.e., the scattering of lattice vibrations by electrons and vice versa, is ubiquitous in solids and can lead to emergent ground states such as superconductivity and charge-density wave order. Strong coupling of phonons to electrons near the Fermi surface, which reduces the phonon lifetimes and broadens the phonon peaks in scattering experiments, is often associated with Fermi surface nesting. Here, we show that strong phonon broadening can occur in the absence of both Fermi surface nesting and lattice anharmonicity, if electron-phonon coupling is strongly enhanced for specific values of electron-momentum, k. We use inelastic neutron scattering, soft x-ray angle-resolved photoemission spectroscopy measurements and ab-initio lattice dynamical and electronic band structure calculations to demonstrate this scenario in the highly anisotropic tetragonal electron-phonon superconductor YNi$_2$B$_2$C. This new scenario likely applies to a wide range of compounds.

cond-mat.supr-con↗

arXiv2021

Effect of the electronic charge gap on LO bond-stretching phonons in undoped La$_2$CuO$_4$ calculated using LDA+U

Typical density-functional theory calculations that wrongly predict undoped cuprates to be metallic also predict Cu-O half- and full-breathing phonon energies that are significantly softer than observed, presumably because of weak on-site Coulomb repulsion on the Cu 3d orbitals. We used DFT+U calculations with antiferromagnetic supercells of La$_2$CuO$_4$ to establish correlation between the on-site repulsion strength, tuned via adjusting the value of U, and phonon dispersions. We find that breathing and half-breathing phonons reach experimental values when U is tuned to obtain the correct optical gap and magnetic moments. We demonstrate that using distorted supercells within DFT+U is a promising framework to model phonons in undoped cuprates and other perovskite oxides with complex, interrelated structural and electronic degrees of freedom.

cond-mat.str-el↗

arXiv2021

Spinons and damped phonons in spin-1/2 quantum-liquid Ba$_{4}$Ir${}_3$O${}_{10}$ observed by Raman scattering

In spin-1/2 Mott insulators, non-magnetic quantum liquid phases are often argued to arise when the system shows no magnetic ordering, but identifying positive signatures of these phases or related spinon quasiparticles can be elusive. Here we use Raman scattering to provide three signatures for spinons in a possible spin-orbit quantum liquid material Ba${}_4$Ir${}_3$O${}_{10}$: (1) A broad hump, which we show can arise from Luttinger Liquid spinons in Raman with parallel photon polarizations normal to 1D chains; (2) Strong phonon damping from phonon-spin coupling via the spin-orbit interaction; and (3) the absence of (1) and (2) in the magnetically ordered phase that is produced when 2% of Ba is substituted by Sr ((Ba${}_{0.98}$Sr${}_{0.02}$)${}_4$Ir${}_3$O${}_{10}$). The phonon damping via itinerant spinons seen in this quantum-liquid insulator suggests a new mechanism for enhancing thermoelectricity in strongly correlated conductors, through a neutral quantum liquid that need not affect electronic transport.

cond-mat.str-el↗

arXiv2020

Unconventional Hund Metal in a Weak Itinerant Ferromagnet

The physics of weak itinerant ferromagnets is challenging due to their small magnetic moments and the ambiguous role of local interactions governing their electronic properties, many of which violate Fermi liquid theory. While magnetic fluctuations play an important role in the materials' unusual electronic states, the nature of these fluctuations and the paradigms through which they arise remain debated. Here we use inelastic neutron scattering to study magnetic fluctuations in the canonical weak itinerant ferromagnet MnSi. Data reveal that short-wavelength magnons continue to propagate until a mode crossing predicted for strongly interacting quasiparticles is reached, and the local susceptibility peaks at a coherence energy predicted for a correlated Hund metal by first-principles many-body theory. Scattering between electrons and orbital and spin fluctuations in MnSi can be understood at the local level to generate non-Fermi liquid character. These results provide crucial insight into the role of interorbital Hund's exchange within the broader class of enigmatic multiband itinerant, weak ferromagnets.

cond-mat.str-el↗

arXiv2020

Quest for New Quantum States via Field-Editing Technology

We report new quantum states in spin-orbit-coupled single crystals that are synthesized using a game-changing technology that "field-edits" crystal structures (borrowing from the phrase "genome editing") via application of magnetic field during crystal growth. This study is intended to fundamentally address a major challenge facing the research community today: A great deal of theoretical work predicting exotic states for strongly spin-orbit-coupled, correlated materials has thus far met very limited experimental confirmation. These conspicuous discrepancies are due chiefly to the extreme sensitivity of these materials to structural distortions. The results presented here demonstrate that the "field-edited" materials not only are much less distorted but also exhibit novel phenomena absent in their "non-edited" counterparts. The field-edited materials include an array of 4d and 5d transition metal oxides, and three representative materials presented here are Ba4Ir3O10, Ca2RuO4, and Sr2IrO4. This study provides an entirely new paradigm for discovery of new quantum states and materials otherwise unavailable.

cond-mat.str-el↗

arXiv2020

Ultrafast magnetic dynamics in insulating YBa$_2$Cu$_3$O$_{6+x}$ revealed by time resolved two-magnon Raman Scattering

Measurement and control of magnetic order and correlations in real time is a rapidly developing scientific area relevant for magnetic memory and spintronics [1,15]. In these experiments an ultra-short laser pulse (pump) is first absorbed by excitations carrying electric dipole moment. These then give their energy to the magnetic subsystem monitored by a time-resolved probe. A lot of progress has been made in investigations of ferromagnets but antiferromagnets are more challenging. Here we introduce time-resolved two-magnon Raman scattering as a novel real time probe of magnetic correlations especially well-suited for antiferromagnets. Its application to the antiferromagnetic charge transfer insulator YBa$_2$Cu$_3$O$_{6+x}$ revealed rapid demagnetization within 90fs of photoexcitation. The relaxation back to thermal equilibrium is characterized by much slower timescales. We interpret these results in terms of slow relaxation of the charge sector and rapid equilibration of the magnetic sector to a prethermal state characterized by parameters that change slowly as the charge sector relaxes.

cond-mat.str-el↗

arXiv2018

Electron-phonon coupling in undoped cuprate $YBa_2Cu_3O_6$ estimated from Raman and optical conductivity spectra

We study experimentally the Raman response of the undoped high-Tc parent compound $YBa_2Cu_3O_6$, and give a unified theory of the two-magnon Raman peak and optical conductivity based on the Hubbard-Holstein model with electron-phonon coupling (EPC). The Hubbard model without EPC can qualitatively account for the experimentally observed resonance of the Raman response, but only the Hubbard-Holstein model (i) reproduces asymmetry of the Raman spectrum, (ii) validates experimental visibility of the two-magnon peak, and (iii) predicts the correct shape and energy of the lower edge of the charge transfer gap in optical conductivity. Comparison of experiments with the theory gives the EPC strength $λ$ = 0.6. This result convincingly indicates the vital role of EPC in high-Tc cuprates providing a clue to the mechanism of high-Tc.

cond-mat.str-el↗

arXiv2017

Evidence for a nematic phase in La$_{1.75}$Sr$_{0.25}$NiO$_{4}$

Determining the nature of electronic states in doped Mott insulators remains a challenging task. In the case of tetragonal La$_{2-x}$Sr$_{x}$NiO$_{4}$, the occurrence of diagonal charge and spin stripe order in the ground state is now well established. In contrast, the nature of the high-temperature "disordered" state from which the stripe order develops has long been a subject of controversy, with considerable speculation regarding a polaronic liquid. Following on the recent detection of dynamic charge stripes, we use neutron scattering measurements on an $x=0.25$ crystal to demonstrate that the dispersion of the charge stripe excitations is anisotropic. This observation provides compelling evidence for the presence of electronic nematic order.

cond-mat.str-el↗

arXiv2016

Novel Electron-Phonon Relaxation Pathway in Graphite Revealed by Time-Resolved Raman Scattering and Angle-Resolved Photoemission Spectroscopy

Time dynamics of photoexcited electron-hole pairs is important for a number of technologies, in particular solar cells. We combined ultrafast pump-probe Raman scattering and photoemission to directly follow electron-hole excitations as well as the G-phonon in graphite after an excitation by an intense laser pulse. This phonon is known to couple relatively strongly to electrons. Cross-correlating effective electronic and phonon temperatures places new constraints on model-based fits. The accepted two-temperature model predicts that G-phonon population should start to increase as soon as excited electron-hole pairs are created and that the rate of increase should not depend strongly on the pump fluence. Instead we found that the increase of the G-phonon population occurs with a delay of $\sim$65 fs. This time-delay is also evidenced by the absence of the so-called self-pumping for G phonons. It decreases with increased pump fluence. We show that these observations imply a new relaxation pathway: Instead of hot carriers transferring energy to G-phonons directly, the energy is first transferred to optical phonons near the zone boundary K-points, which then decay into G-phonons via phonon-phonon scattering. Our work demonstrates that phonon-phonon interactions must be included in any calculations of hot carrier relaxation in optical absorbers even when only short timescales are considered.

cond-mat.mes-hall↗