arXiv subjects

Anshul Kogar

Publications and source records attributed to Anshul Kogar.

At least 19 recordsLinked to original sources

arXiv2025

Dynamical crossover between stretched- and compressed-exponential relaxation in a photoexcited crystal

Anomalous relaxation is one of the hallmarks of disordered systems. Following perturbation by an external source, many glassy, jammed and amorphous systems relax as a stretched or compressed exponential as a function of time. However, despite their ubiquity, the origins of and the connection between these phenomenological relaxation functions remains to be understood. Here, we observe a tunable crossover from stretched- to compressed-exponential relaxation by photoexciting single crystal Ca3Ru2O7 across a structural phase transition. We present a simple lattice model that shows how spatial inhomogeneity and local, strain-mediated interactions cooperate to produce the dynamical crossover. Our work reveals anomalous relaxation dynamics in an idealized single crystal material and establishes photoexcited solids as promising platforms for probing the mechanisms underlying anomalous relaxation.

cond-mat.str-el↗

arXiv2025

Topological phase transition to a hidden charge density wave liquid

Charge density waves (CDWs), electronic crystals that form within a host solid, have long been speculated to melt into a spatially textured electronic liquid. Though they have not been previously detected, liquid CDWs may nonetheless be fundamental to the phase diagrams of many correlated electron systems, including high temperature superconductors and quantum Hall states. In one of the most promising candidate materials capable of hosting a liquid CDW, 1T-TaS2, a structural phase transition impedes its observation. Here, by irradiating the material with a femtosecond light pulse, we circumvent the structural phase transition to reveal how topological defect dynamics govern the otherwise invisible CDW correlations. Upon photoexcitation, the CDW diffraction peaks broaden azimuthally, initially revealing a hexatic state. At higher temperatures, photoexcitation completely destroys translational and orientational order and only a ring of diffuse scattering is observed, a key signature of a liquid CDW. Our work provides compelling evidence for a defect-unbinding transition to a CDW liquid and presents a protocol for uncovering states that are hidden by other transitions in thermal equilibrium.

cond-mat.str-el↗

arXiv2025

Metastable short-range charge order in superconducting CuxTiSe2

In a vast array of materials, including cuprates, transition metal dichalcogenides (TMDs) and rare earth tritellurides, superconductivity is found in the vicinity of short-range charge density wave (CDW) order. The crossover from long-range to short-range charge order often occurs as quenched disorder is introduced, yet it is unclear how this disorder disrupts the CDW. Here, using x-ray photon correlation spectroscopy (XPCS), we investigate the prototypical TMD superconductor CuxTiSe2 and show that disorder induces substantial CDW dynamics. We observe CDW phase fluctuations on a timescale of minutes to hours above the nominal transition temperature while the order parameter amplitude remains finite. These long timescale fluctuations prevent the system from finding the global free energy minimum upon cooling and ultimately traps it in a short-range ordered metastable state. Our findings demonstrate how correlated disorder can give rise to a distinct mechanism of domain formation that may be advantageous to the emergence of superconductivity.

cond-mat.str-el↗

arXiv2025

Jeff = 1/2 Diamond Magnet CaCo2TeO6: A Pathway toward New Spin Physics and Quantum Functions

Diamond lattice magnets, formed by a framework of corner-sharing tetrahedra of magnetic cations, offer unique opportunities to realize novel states of matter for potential utility in information technology. However, research has mostly focused on AB2X4 spinels with Td magnetic ions. This hinders the atomically enabled tunability of competing interactions at different energy scales and the ability to harness many-body electronic states in quantum materials, making the discovery of quantum fluctuations and spin dynamics less accessible. We discover a new material CaCo2TeO6 featuring a diamond lattice of two distinct Oh-Co2+ sites. This material displays strong quantum fluctuations, increased competing magnetic exchange interactions, and field-induced tunability of magnetic structures. The results demonstrate how simple, fundamental refinements in ligand fields can profoundly influence the phase space of quantum matter.

cond-mat.mtrl-sci↗

arXiv2025

Light-induced reorientation transition in an antiferromagnetic semiconductor

Due to the lack of a net magnetic moment, antiferromagnets possess a unique robustness to external magnetic fields and are thus predicted to play an important role in future magnetic technologies. However, this robustness also makes them quite difficult to control, and the development of novel methods to manipulate these systems with external stimuli is a fundamental goal of antiferromagnetic spintronics. In this work, we report evidence for a metastable reorientation of the order parameter in an antiferromagnetic semiconductor triggered by an ultrafast quench of the equilibrium order via photoexcitation above the band gap. The metastable state forms less than 10 ps after the excitation pulse, and persists for longer than 150 ps before decaying to the ground state via thermal fluctuations. Importantly, this transition cannot be induced thermodynamically, and requires the system to be driven out of equilibrium. Broadly speaking, this phenomenology is ultimately the result of large magnetoelastic coupling in combination with a relatively low symmetry of the magnetic ground state. Since neither of these properties are particularly uncommon in magnetic materials, the observations presented here imply a generic path toward novel device technology enabled by ultrafast dynamics in antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2025

In-plane anisotropy of charge density wave fluctuations in 1$T$-TiSe$_2$

We report measurements of anisotropic triple-$q$ charge density wave (CDW) fluctuations in the transition metal dichalcogenide 1$T$-TiSe$_2$ over a large volume of reciprocal space with X-ray diffuse scattering. Above the transition temperature, $T_{\text{CDW}}$, the out-of-plane diffuse scattering is characterized by rod-like structures which indicate that the CDW fluctuations in neighboring layers are largely decoupled. In addition, the in-plane diffuse scattering is marked by ellipses which reveal that the in-plane fluctuations are anisotropic. Our analysis of the diffuse scattering line shapes and orientations suggests that the three charge density wave components contain independent phase fluctuations. At $T_{\text{CDW}}$, long range coherence is established in both the in-plane and out-of-plane directions, consistent with the large observed value of the CDW gap compared to $T_{\text{CDW}}$, and the predicted presence of a hierarchy of energy scales.

cond-mat.str-el↗

arXiv2024

Directionally asymmetric nonlinear optics in planar chiral MnTiO$_3$

Planar chiral structures possess a two dimensional handedness that is associated with broken mirror symmetry. Such motifs span vast length scales; examples include certain pinwheel molecules, nautilus shells, cyclone wind patterns and spiral galaxies. Although pervasive in nature, it has only recently been found that condensed matter systems can exhibit a form of planar chirality through toroidal arrangements of electric dipoles, known as ferro-rotational (FR) order. A key characteristic of such order is that enantiomorph conversion occurs when the solid is flipped by 180 degrees about an in-plane axis. Consequently, ferro-rotationally ordered materials may exhibit directionally asymmetric response functions, even while preserving inversion and time-reversal symmetry. Such an effect, however, has yet to be observed. Using second harmonic interferometry, we show here that when circularly polarized light is incident on MnTiO$_3$, the generated nonlinear signal exhibits directional asymmetry. Depending on whether the incident light is parallel or anti-parallel to the FR axis, we observe a different conversion efficiency of two right (left) circularly polarized photons into a frequency-doubled left (right) circularly polarized photon. Our work uncovers a fundamentally new optical effect in ordered solids and opens up the possibility for developing novel nonlinear and directionally asymmetric optical devices.

physics.optics↗

arXiv2024

Vector-based feedback of continuous wave radiofrequency compression cavity for ultrafast electron diffraction

The temporal resolution of ultrafast electron diffraction (UED) at weakly relativistic beam energies ($\lesssim$ 100 keV) suffers from space-charge induced electron pulse broadening. We describe the implementation of a radio frequency (RF) cavity operating in the continuous wave regime to compress high repetition rate electron bunches from a 40.4 kV DC photoinjector for ultrafast electron diffraction applications. Active stabilization of the RF amplitude and phase through a feedback loop based on the demodulated in-phase and quadrature components of the RF signal is demonstrated. This scheme yields 144$\pm$19 fs RMS temporal resolution in pump-probe studies.

physics.acc-ph↗

arXiv2024

Light-induced electronic polarization in antiferromagnetic Cr2O3

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. External fields that couple to electronic order parameters have rarely been investigated, however, despite their potential importance to inducing exotic effects. Here, we show that when inversion symmetry is broken by the antiferromagnetic (AFM) order in Cr2O3, transmitting a linearly polarized light pulse through the crystal gives rise to an in-plane rotational symmetry breaking (from C3 to C1) via optical rectification. Using interferometric time-resolved second harmonic generation, we show that the ultrafast timescale of the symmetry reduction is indicative of a purely electronic response; the underlying spin and crystal structures remain unaffected. The symmetry-broken state exhibits a dipole moment, and its polar axis can be controlled with the incident light. Our results establish a coherent nonlinear optical protocol by which to break electronic symmetries and produce unconventional electronic effects in solids.

cond-mat.str-el↗

arXiv2023

Evidence for bootstrap percolation dynamics in a photo-induced phase transition

Upon intense femtosecond photo-excitation, a many-body system can undergo a phase transition through a non-equilibrium route, but understanding these pathways remains an outstanding challenge. Here, we use time-resolved second harmonic generation to investigate a photo-induced phase transition in Ca$_3$Ru$_2$O$_7$ and show that mesoscale inhomogeneity profoundly influences the transition dynamics. We observe a marked slowing down of the characteristic time, $τ$, that quantifies the transition between two structures. $τ$ evolves non-monotonically as a function of photo-excitation fluence, rising from below 200~fs to $\sim$1.4~ps, then falling again to below 200~fs. To account for the observed behavior, we perform a bootstrap percolation simulation that demonstrates how local structural interactions govern the transition kinetics. Our work highlights the importance of percolating mesoscale inhomogeneity in the dynamics of photo-induced phase transitions and provides a model that may be useful for understanding such transitions more broadly.

cond-mat.str-el↗

arXiv2022

Delamination-assisted ultrafast wrinkle formation in a freestanding film

The ability to synthesize and control two-dimensional (2D) crystals creates numerous opportunities for studying emergent states of matter and their novel functionalities. Freestanding films provide a particularly versatile platform for materials engineering in 2D thanks to additional structural motifs not found in films adhered to a flat substrate. A ubiquitous example is wrinkles, yet little is known about how they can develop over as fast as a few picoseconds due to a lack of experimental probes to visualize their dynamics in real time at the nanoscopic scale. Here, we use ultrafast electron diffraction to directly observe light-activated wrinkling formation in a freestanding La$_{2/3}$Ca$_{1/3}$MnO$_3$ film. Via a ``lock-in'' analysis of a single mode of oscillation in the diffraction peak position, intensity, and width, we are able to quantitatively reconstruct how wrinkles develop at the picosecond timescale. Contrary to the common assumption of a fixed boundary condition for freestanding films, we found that wrinkle development is associated with ultrafast delamination at the contact point between the film boundary and the underlying substrate, avoiding a strain build-up in the film. Not only does our work provide a generic protocol to quantify wrinkling dynamics in freestanding films, it also highlights the importance of film-substrate interaction for determining the properties of freestanding structures.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast formation of topological defects in a 2D charge density wave

Topological defects play a key role in nonequilibrium phase transitions, ranging from birth of the early universe to quantum critical behavior of ultracold atoms. In solids, transient defects are known to generate a variety of hidden orders not accessible in equilibrium, but how defects are formed at the nanometer lengthscale and femtosecond timescale remains unknown. Here, we employ an intense laser pulse to create topological defects in a 2D charge density wave, and track their morphology and dynamics with ultrafast electron diffraction. Leveraging its high temporal resolution and sensitivity in detecting weak diffuse signals, we discover a dual-stage growth of 1D domain walls within 1 ps, a process not dictated by the order parameter amplitude but instead mediated by a nonthermal population of longitudinal optical phonons. Our work provides a framework for ultrafast engineering of topological defects based on selective excitation of collective modes, opening new avenues for dynamical control of nonequilibrium phases in correlated materials.

cond-mat.mtrl-sci↗

arXiv2022

Dynamics of topological defects after a photo-induced melting of a charge-density wave

Charge-density-wave order in a solid can be temporarily "melted" by a strong laser pulse. Here we use the discrete Gross-Pitaevskii equation on a cubic lattice to simulate the recovery of the CDW long-range phase coherence following such a pulse. Our simulations indicate that the recovery process is dramatically slowed down by the three-dimensional topological defects - CDW dislocations - created as a result of strongly nonequilibrium heating and cooling of the system. Overall, the simulated CDW recovery was found to be remarkably reminiscent of a recent pump-probe experiment in LaTe$_3$.

cond-mat.str-el↗

arXiv2022

Light-induced dimension crossover in 1T-TiSe$_2$ dictated by excitonic correlations

In low-dimensional systems with strong electronic correlations, the application of an ultrashort laser pulse often yields novel phases that are otherwise inaccessible. The central challenge in understanding such phenomena is to determine how dimensionality and many-body correlations together govern the pathway of a non-adiabatic transition. To this end, we examine a layered compound, 1T-TiSe$_2$, whose three-dimensional charge-density-wave (3D CDW) state also features exciton condensation due to strong electron-hole interactions. We find that photoexcitation suppresses the equilibrium 3D CDW while creating a nonequilibrium 2D CDW. Remarkably, the dimension reduction does not occur unless bound electron-hole pairs are broken. This relation suggests that excitonic correlations maintain the out-of-plane CDW coherence, settling a long-standing debate over their role in the CDW transition. Our findings demonstrate how optical manipulation of electronic interaction enables one to control the dimensionality of a broken-symmetry order, paving the way for realizing other emergent states in strongly correlated systems.

cond-mat.str-el↗

arXiv2021

Unconventional light-induced states visualized by ultrafast electron diffraction and microscopy

Exciting electrons in solids with intense light pulses offers the possibility of generating new states of matter through nonthermal means and controlling their macroscopic properties on femto- to picosecond timescales. One way to manipulate a solid is by altering its lattice structure, which often underlies the electronic, magnetic and other phases. Here, we review how structures of solids are affected by photoexcitation and how their ultrafast dynamics are captured with time-resolved electron diffraction and microscopy. Specifically, we survey how a strong light pulse has been used to tailor the nonequilibrium characteristics to yield on-demand properties in various material classes. In the existing literature, four main routes have been exploited to control material structures: (i) phase competition, (ii) electronic correlations, (iii) excitation of coherent modes, and (iv) defect generation. In this review, we discuss experiments relevant to all four schemes and finish by speculating about future directions.

cond-mat.mtrl-sci↗

arXiv2021

Role of equilibrium fluctuations in light-induced order

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host "hidden" orders after laser excitation.

cond-mat.mtrl-sci↗

arXiv2020

The Future of the Correlated Electron Problem

A central problem in modern condensed matter physics is the understanding of materials with strong electron correlations. Despite extensive work, the essential physics of many of these systems is not understood and there is very little ability to make predictions in this class of materials. In this manuscript we share our personal views on the major open problems in the field of correlated electron systems. We discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.

cond-mat.str-el↗

arXiv2020

The spontaneous symmetry breaking in Ta$_2$NiSe$_5$ is structural in nature

The excitonic insulator is an electronically-driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta$_2$NiSe$_5$ being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals surprising spectroscopic fingerprints that are only compatible with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the electronic gap opening. Not only do our results uncover the long-sought mechanism driving the phase transition of Ta$_2$NiSe$_5$, but they also conclusively rule out any substantial excitonic character in this instability.

cond-mat.str-el↗