arXiv subjects

Shivasheesh Varshney

Publications and source records attributed to Shivasheesh Varshney.

8 recordsLinked to original sources

arXiv2026

Light-Driven Ultrafast Control of Time-Reversal Symmetry in SrTiO3

Light-driven control of material symmetry enables the engineering of phenomena forbidden in equilibrium. Although electromagnetic fields have been used to break time-reversal symmetry, its dynamic control on ultrafast timescales in nonmagnetic insulating oxides remains virtually unexplored. Here, we demonstrate simultaneous magnetic symmetry lowering and timereversal-symmetry breaking in cubic SrTiO3 driven by an off-resonant, elliptically polarized THz pulse. Second harmonic generation (SHG) polarimetry reveals emergent SHG circular dichroism inconsistent with third-order nonlinear processes under cubic m3m symmetry. The SHG polar patterns exhibit mirror-symmetry breaking, indicating a transient reduction to tetragonal 4/mm'm' magnetic symmetry. Furthermore, the SHG response scales linearly with the angular momentum of THz pulse, providing direct evidence for THz-field-induced timereversal-symmetry breaking. These results establish a direct pathway for ultrafast symmetry control in non-magnetic oxides, enabling dynamic manipulation of emergent phases on ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2026

Wafer-scale High-k SrTiO3 Dielectrics with Rational Barrier-layer Design for Low Leakage and High Charge Density

High-k oxides such as SrTiO3 promise large capacitance, but their dielectric response is often limited by leakage currents due to reduced bandgaps. We show that introducing a thin barrier layer beneath SrTiO3 is a simple and effective way to suppress leakage and increase charge density. Using hybrid molecular beam epitaxy, we grew uniform SrTiO3 films on Nb:SrTiO3, CaSnO3/Nb:SrTiO3, and 2-inch SiO2/p-Si stacks to directly compare how different barrier layers influence device behavior. Both CaSnO3 and SiO2 reduce leakage, but the ultra-wide-bandgap SiO2 layer enables much higher operating voltages, yielding charge densities exceeding 5x10^13 cm^-2 at room temperature - more than a fivefold enhancement compared to devices without a barrier layer. This improvement comes with a predictable trade-off: the lower dielectric constant of SiO2 reduces overall capacitance, making its thickness an important design parameter. Together, these results demonstrate that rational barrier-layer engineering - including wafer-scale integration on Si - provides a clear pathway to achieving higher charge densities in SrTiO3-based dielectric devices.

cond-mat.mtrl-sci↗

arXiv2025

Superconducting Dome in Ionic Liquid Gated Homoepitaxial Strontium Titanate Thin Films

In this work, we patterned a two-dimensional electron gas (2DEG) on the surface of a SrTiO$_3$ thin film grown homoepitaxially on SrTiO$_3$ by hybrid molecular beam epitaxy (hMBE). We explored the superconducting dome in this material system by tuning electron density with ionic liquid gating. We found superconducting transitions up to 503 mK near an optimal electron density of approximately 3 $\times$ 10$^{13}$ cm$^{-2}$. This is a meaningful increase from the typical optimal transition near 350 mK in similar 2DEGs on SrTiO$_3$ single crystal substrate surfaces. Systematic tuning of 2DEG electron density revealed a consistent BCS scaling between superconducting critical temperature, coherence length, and electron mean free path. Substantial variation of transition width across the dome was described by a paraconductivity model combining Aslamazov-Larkin and Maki-Thompson contributions.

cond-mat.supr-con↗

arXiv2025

Interfacial strong coupling and negative dispersion of propagating polaritons in freestanding oxide membranes

Membranes of complex oxides like perovskite SrTiO3 extend the multi-functional promise of oxide electronics into the nanoscale regime of two-dimensional materials. Here we demonstrate that free-standing oxide membranes supply a reconfigurable platform for nano-photonics based on propagating surface phonon polaritons. We apply infrared near-field imaging and -spectroscopy enabled by a tunable ultrafast laser to study pristine nano-thick SrTiO3 membranes prepared by hybrid molecular beam epitaxy. As predicted by coupled mode theory, we find that strong coupling of interfacial polaritons realizes symmetric and antisymmetric hybridized modes with simultaneously tunable negative and positive group velocities. By resolving reflection of these propagating modes from membrane edges, defects, and substrate structures, we quantify their dispersion with position-resolved nano-spectroscopy. Remarkably, we find polariton negative dispersion is both robust and tunable through choice of membrane dielectric environment and thickness and propose a novel design for in-plane Veselago lensing harnessing this control. Our work lays the foundation for tunable transformation optics at the nanoscale using polaritons in a wide range of freestanding complex oxide membranes.

cond-mat.mes-hall↗

arXiv2025

Absence of two-phonon quasi-elastic scattering in the normal state of doped--SrTiO$_3$ by THz pump-probe spectroscopy

Multi-pulse nonlinear THz spectroscopies enable a new understanding of interacting metallic systems via their sensitivity to novel correlation functions. Here, we investigated the THz nonlinear properties of the dilute metallic phase of doped-SrTiO$_3$ thin films using nonlinear terahertz 2D coherent spectroscopy. We observed a large $\chi^{(3)}$ response in the low temperature region where the dc electrical resistivity follows a T$^2$-dependence. This is largely a pump-probe response, which we find is governed by a single energy relaxation rate that is much smaller at all temperatures than the momentum relaxation rates obtained from the optical conductivity. This indicates that the processes that dominate the resistive scattering are not the same as those that remove energy from the electronic system. Moreover the fact that the energy relaxation rate is an increasing function of temperature indicates that the excitations that do carry away energy from the electronic system cannot be considered as quasi-elastic and as such soft two-phonon electron scattering does not play a major role in the physics as proposed. This indicates that these materials' resistive T$^2$ scattering likely originates in electron-electron interactions despite the very small Fermi wave vectors at the lowest dopings.

cond-mat.str-el↗

arXiv2024

Epitaxially Grown Single-Crystalline SrTiO3 Membranes Using a Solution-Processed, Amorphous SrCa2Al2O6 Sacrificial Layer

Water-soluble sacrificial layers based on epitaxially-grown, single crystalline (Ca, Sr, Ba)3Al2O6 layer are widely used for creating free-standing perovskite oxide membranes. However, obtaining these sacrificial layers with intricate stoichiometry remains a challenge, especially for molecular beam epitaxy (MBE). In this study, we demonstrate the hybrid MBE growth of epitaxial, single crystalline SrTiO3 films using a solution processed, amorphous SrCa2Al2O6 sacrificial layer onto SrTiO3 (001) substrates. Prior to the growth, the oxygen plasma exposure was used to first create the crystalline SrCa2Al2O6 layer with well-defined surface crystallinity. Utilizing reflection high energy electron diffraction, x-ray diffraction, and atomic force microscopy, we observe an atomic layer-by-layer growth of epitaxial, single crystalline SrTiO3 film on the SrCa2Al2O6 layer with atomically smooth surfaces. The SrCa2Al2O6 layer was subsequently dissolved in de-ionized water to create free-standing SrTiO3 membranes that were transferred onto a metal-coated Si wafer. Membranes created with Sr-deficiency revealed ferroelectric-like behavior measured using piezo force microscopy whereas stoichiometric films remained paraelectric-like. These findings underscore the viability of using ex-situ deposited amorphous SrCa2Al2O6 for epitaxial, single crystalline growth, as well as the importance of point defects in determining the ferroic properties in membranes.

cond-mat.mtrl-sci↗

arXiv2024

Anomalous frequency and temperature dependent scattering in the dilute metallic phase in lightly doped-SrTiO$_3$

The mechanism of superconductivity in materials with aborted ferroelectricity and the emergence of a dilute metallic phase in systems like doped-SrTiO$_3$ are outstanding issues in condensed matter physics. This dilute metal has features both similar and different to those found in the normal state of other unconventional superconductors. We have investigated the optical properties of the dilute metallic phase in doped-SrTiO$_3$ using THz time-domain spectroscopy. At low frequencies the THz response exhibits a Drude-like form as expected for typical metal-like conductivity. We observed the frequency and temperature dependencies to the low energy scattering rate $\Gamma(\omega, T) \propto (\hbar\omega)^2 + (p \pi k_BT)^2 $ expected in a conventional Fermi liquid, despite the fact that densities are too small to allow current decay through electron-electron scattering. However we find the lowest known $p$ values of 0.39-0.72. As $p$ is 2 in a canonical Fermi liquid and existing models based on energy dependent elastic scattering bound $p$ from below to 1, our observation lies outside current explanation. Our data also gives insight into the high temperature regime and shows that the temperature dependence of the resistivity derives in part from strong T dependent mass renormalizations.

cond-mat.str-el↗

arXiv2023

Fast and Facile Synthesis Route to Epitaxial Oxide Membrane Using a Sacrificial Layer

The advancement in thin-film exfoliation for synthesizing oxide membranes has opened up new possibilities for creating artificially-assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques like Molecular Beam Epitaxy (MBE). This is where easy-to-grow binary alkaline earth metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of single-crystalline perovskite SrTiO3 (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba1-xCaxO films, employing a hybrid MBE method. Our results highlight the rapid (< 5 minutes) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution x-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate epitaxial STO membranes with bulk-like intrinsic dielectric properties. The employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding research possibilities.

physics.app-ph↗