arXiv subjects

Umesh V. Waghmare

Publications and source records attributed to Umesh V. Waghmare.

At least 19 recordsLinked to original sources

arXiv2025

Modulation of quantum geometry and its coupling to pseudo-electric field by dynamic strain

Two-dimensional materials are a fertile ground for exploring quantum geometric phenomena, with Berry curvature and its first moment, the Berry curvature dipole, playing a central role in their electronic response. These geometric properties influence electronic transport and result in the anomalous and nonlinear Hall effects, and are typically controlled using static electric fields or strain. However, the possibility of modulating quantum geometric quantities in real-time remains unexplored. Here, we demonstrate the dynamic modulation of Berry curvature and its moments, as well as the generation of a pseudo-electric field using time-dependent strain. By placing heterostructures on a membrane, we introduce oscillatory strain together with an in-plane AC electric field and measure Hall signals that are modulated at linear combinations of the frequencies of strain and electric field. Our measurements reveal modulation of Berry curvature and its first moment. Notably, we provide direct experimental evidence of pseudo-electric field that results in an unusual dynamic strain-induced Hall response. This approach opens up a new pathway for controlling quantum geometry on demand, moving beyond conventional static perturbations. The pseudo-electric field provides a framework for external electric field-free anomalous Hall response and opens new avenues for probing the topological properties.

cond-mat.mes-hall↗

arXiv2025

Accelerating the Search for Superconductors Using Machine Learning

Prediction of critical temperature $(T_c)$ of a superconductor remains a significant challenge in condensed matter physics. While the BCS theory explains superconductivity in conventional superconductors, there is no framework to predict $T_c$ of unconventional, higher $T_{c}$ superconductors. Quantum Structure Diagrams (QSD) were successful in establishing structure-property relationship for superconductors, quasicrystals, and ferroelectric materials starting from chemical composition. Building on the QSD ideas, we demonstrate that the principal component analysis of superconductivity data uncovers the clustering of various classes of superconductors. We use machine learning analysis and cleaned databases of superconductors to develop predictive models of $T_c$ of a superconductor using its chemical composition. Earlier studies relied on datasets with inconsistencies, leading to suboptimal predictions. To address this, we introduce a data-cleaning workflow to enhance the statistical quality of superconducting databases by eliminating redundancies and resolving inconsistencies. With this improvised database, we apply a supervised machine learning framework and develop a Random Forest model to predict superconductivity and $T_c$ as a function of descriptors motivated from Quantum Structure Diagrams. We demonstrate that this model generalizes effectively in reasonably accurate prediction of $T_{c}$ of compounds outside the database. We further employ our model to systematically screen materials across materials databases as well as various chemically plausible combinations of elements and predict $\mathrm{Tl}_{5}\mathrm{Ba}_{6}\mathrm{Ca}_{6}\mathrm{Cu}_{9}\mathrm{O}_{29}$ to exhibit superconductivity with a $T_{c}$ $\sim$ 105 K. Being based on the descriptors used in QSD's, our model bypasses structural information and predicts $T_{c}$ merely from the chemical composition.

cond-mat.supr-con↗

arXiv2023

Entropic Stabilization and Descriptors of Structural Transformation in High Entropy Alloys

With first-principles theoretical analysis of the local structure using Bond Orientational Order parameters and Voronoi partitioning, we establish (a) HCP$\rightarrow$BCC structural transformation in high-entropy alloys (HEAs) Nb$_x$(HfZrTi)$_y$ at 16% Nb-concentration, and (b) that the internal lattice distortions (ILDs) peak at the transition. We demonstrate that the relative stability of HCP and BCC structures is driven by energetics, while the overall stability is achieved with contribution from the vibrational entropy that exceeds the configurational entropy of mixing. We show that along with atomic size mismatch, low average number ($< $5) of valence electrons and disparity in the crystal structures of constituent elements are responsible for larger ILDs in Nb$_x$(HfZrTi)$_y$ than in HEAs like Nb$_a$Mo$_b$W$_c$Ta$_d$.

cond-mat.mtrl-sci↗

arXiv2022

Pressure-induced superconductivity in weak topological insulator BiSe

Quasi-two-dimensional layered BiSe, a natural super-lattice with Bi2Se3-Bi2-Bi2Se3 units, has recently been predicted to be a dual topological insulator, simultaneously weak topological insulator as well as topological crystalline insulator. Here using structural, transport, spectroscopic measurements and density functional theory calculations, we show that BiSe exhibits rich phase diagram with the emergence of superconductivity with Tc ~8K under pressure. Sequential structural transitions into SnSe-type energetically tangled orthorhombic and CsCl-type cubic structures having distinct superconducting properties are identified at 8 GPa and 13 GPa respectively. Our observation of weak-antilocalization in magneto-conductivity suggests that spin-orbit coupling (SOC) plays a significant role in retaining non-trivial band topology in the trigonal phase with possible realization of 2D topological superconductivity. Theoretical analysis reveals that SOC significantly enhances superconducting Tc of the high-pressure cubic phase through an increase in electron-phonon coupling strength. Simultaneous emergence of Dirac-like surface states suggests cubic BiSe as a suitable candidate for the 3D-topological superconductor.

cond-mat.supr-con↗

arXiv2022

Pressure tuning of structure, magnetic frustration and carrier conduction in Kitaev spin liquid candidate Cu$_2$IrO$_3$: X-ray, Raman, magnetic susceptibility, resistivity and first-principles analysis

The layered honeycomb lattice iridate Cu$_2$IrO$_3$ is the closest realization of the Kitaev quantum spin liquid, primarily due to the enhanced interlayer separation and nearly ideal honeycomb lattice. We report pressure-induced structural evolution of Cu$_2$IrO$_3$ by powder x-ray diffraction (PXRD) up to $\sim$17 GPa and Raman scattering measurements up to $\sim$25 GPa. A structural phase transition (monoclinic $C2/c \: \rightarrow$ triclinic $P\bar{1}$) is observed with a broad mixed phase pressure range ($\sim$4 to 15 GPa). The triclinic phase consists of heavily distorted honeycomb lattice with Ir-Ir dimer formation and a collapsed interlayer separation. In the stability range of the low-pressure monoclinic phase, structural evolution maintains the Kitaev configuration up to 4 GPa. This is supported by the observed enhanced magnetic frustration in dc susceptibility without emergence of any magnetic ordering and an enhanced dynamic Raman susceptibility. High-pressure resistance measurements up to 25 GPa in the temperature range 1.4--300 K show resilient non-metallic $R$($T$) behaviour with significantly reduced resistivity in the high-pressure phase. The Mott 3D variable-range-hopping conduction with much reduced characteristic energy scale $T_0$ suggests that the high-pressure phase is at the boundary of localized-itinerant crossover. Using first-principles density functional theoretical (DFT) calculations, we find that at ambient pressure $\rm Cu_2IrO_3$ exists in monoclinic $P2_1/c$ phase which is energetically lower than $C2/c$ phase (both the structures are consistent with experimental XRD pattern). DFT reveals structural transition from $P2_1/c$ to $P\bar{1}$ structure at 7 GPa (involving dimerization of Ir-Ir bonds) in agreement with experimentally observed transition pressure.

cond-mat.str-el↗

arXiv2022

Berry curvature dipole senses topological transition in a moiré superlattice

Topological aspects of electron wavefunction play a crucial role in determining the physical properties of materials. Berry curvature and Chern number are used to define the topological structure of electronic bands. While Berry curvature and its effects in materials have been studied, detecting changes in the topological invariant, Chern number, is challenging. In this regard, twisted double bilayer graphene (TDBG) has emerged as a promising platform to gain electrical control over the Berry curvature hotspots and the valley Chern numbers of its flat bands. In addition, strain induced breaking of the three-fold rotation (C3) symmetry in TDBG, leads to a non-zero first moment of Berry curvature called the Berry curvature dipole (BCD), which can be sensed using nonlinear Hall (NLH) effect. We reveal, using TDBG, that the BCD detects topological transitions in the bands and changes its sign. In TDBG, the perpendicular electric field tunes the valley Chern number and the BCD simultaneously allowing us a tunable system to probe the physics of topological transitions. Furthermore, we find hysteresis of longitudinal and NLH responses with electric field that can be attributed to switching of electric polarization in moiré systems. Such a hysteretic response holds promise for next-generation Berry curvature-based memory devices. Probing topological transitions, as we show, can be emulated in other 3D topological systems.

cond-mat.mes-hall↗

arXiv2021

Pressure-induced 1T to 3R structural phase transition in metallic VSe2: X-ray diffraction and first-principles theory

We study pressure-induced structural evolution of vanadium diselenide (VSe2), a 1T polymorphic member of the transition metal di-chalcogenide (TMD) family using synchrotron-based powder X-ray diffraction (PXRD) and first-principles density functional theory (DFT). Our XRD results reveal anomalies at P ~4 GPa in c/a ratio, V-Se bond length and Se-V-Se bond angle signalling an isostructural transition. This is followed by a first order structural transition from 1T (space group P-3m1) phase to a 3R (space group R-3m) phase at P ~11 GPa due to sliding of adjacent Se-V-Se layers. We present various scenarios to understand the experimental results within DFT and find that the 1T to 3R transition can be captured only after inclusion of enthalpic correction associated with errors in cell volume with underestimated transition pressure. The abrupt increase in the Debye-Waller factors of Se atoms by a factor of ~4 and hence the anharmonic effects across the structural transition pressure are hitherto not reported so far and hint a possible way to understand the mismatch between the experimental and theoretical transition pressure values.

cond-mat.mtrl-sci↗

arXiv2020

Tuning the structure of Skyrmion lattice system Cu2OSeO3 under pressure

The insulating ferrimagnet Cu2OSeO3 shows a rich variety of phases such as skyrmion lattice and helical magnetism controlled by interplay of different exchange interactions which can be tuned by external pressure. In this work we have investigated pressure-induced phase transitions at room temperature using synchrotron based x- ray diffraction and Raman scattering measurements. With first-principles theoretical analysis, we show that spin-spin exchange couplings in the ambient cubic phase are affected notably by hydrostatic pressure. The ambient cubic phase transforms to a monoclinic phase above 7 GPa and then to the triclinic phase above 11 GPa. Emergence of new phonon modes in the Raman spectra confirms these structural phase transitions. Notably, upon decompression, the crystal undergoes transition to a new monoclinic structure. Atomic coordinates have been refined in the low pressure cubic phase to capture the Cu-tetrahedra evolution responsible for the earlier reported magnetic behavior under pressure. Our experiments will motivate further studies of its emergent magnetic behavior under pressure.

cond-mat.mtrl-sci↗

arXiv2020

Predicting the DNA Conductance using Deep Feed Forward Neural Network Model

Double-stranded DNA (dsDNA) has been established as an efficient medium for charge migration, bringing it to the forefront of the field of molecular electronics as well as biological research. The charge migration rate is controlled by the electronic couplings between the two nucleobases of DNA/RNA. These electronic couplings strongly depend on the intermolecular geometry and orientation. Estimating these electronic couplings for all the possible relative geometries of molecules using the computationally demanding first-principles calculations requires a lot of time as well as computation resources. In this article, we present a Machine Learning (ML) based model to calculate the electronic coupling between any two bases of dsDNA/dsRNA of any length and sequence and bypass the computationally expensive first-principles calculations. Using the Coulomb matrix representation which encodes the atomic identities and coordinates of the DNA base pairs to prepare the input dataset, we train a feedforward neural network model. Our NN model can predict the electronic couplings between dsDNA base pairs with any structural orientation with a MAE of less than 0.014 eV. We further use the NN predicted electronic coupling values to compute the dsDNA/dsRNA conductance.

cond-mat.soft↗

arXiv2019

Prediction of Coupled Electronic and Phononic Ferroelectricity in Strained 2D h-NbN: First-principles Theoretical Analysis

Using first-principles density functional theoretical analysis, we predict coexisting ferroelectric and semi-metallic states in two-dimensional monolayer of h-NbN subjected to electric field and in-plane strain ($ε$). At strains close to $ε$=4.85%, where its out-of-plane spontaneous polarization changes sign without inverting the structure, we demonstrate a hysteretic response of its structure and polarization to electric field, and uncover a three-state (P=$\pm$P$_o$Po, 0) switching during which h-NbN passes through Dirac semi-metallic states. With first-principles evidence for a combination of electronic and phononic ferroelectricity, we present a simple model that captures the energetics of coupled electronic and structural polarization, and show that electronic ferroelectricity arises in a material which is highly polarizable (small bandgap) and exhibits a large electron-phonon coupling leading to anomalous dynamical charges. These insights will guide search for electronic ferroelectrics, and our results on 2D h-NbN will stimulate development of piezo-field effect transistors and devices based on the multi-level logic.

cond-mat.mes-hall↗

arXiv2018

Phonons and Thermal Conducting Properties of Borocarbonitride (BCN) Nanosheets

Hexagonal borocarbonitrides (BCN) are a class of 2D materials, which display excellent catalytic activity for water splitting. Here, we report analysis of thermal stability, phonons and thermal conductivity of BCN monolayers over a wide range of temperatures using classical molecular dynamics simulations. Our results show that in contrast to the case of graphene and boron nitride monolayers, the out-of-plane phonons in BCN monolayers induce an asymmetry in the phonon density of states at all temperatures. Despite possessing lower thermal conducting properties compared to graphene and BN monolayers, the BCN nanosheets do not lose thermal conductivity as much as graphene and BN in the studied temperature range of 200-1000 K, and thus, the BCN nanosheets are suitable for thermal interface device applications over a wide range of temperatures. Besides their promising role in water splitting, the above results highlight the possibility of expanding the use of BCN 2D materials in thermal management applications and thermoelectrics.

cond-mat.mes-hall↗

arXiv2018

Origin of the monolayer Raman signature in hexagonal boron nitride: a first-principles analysis

Monolayers of hexagonal boron nitride (h-BN) can in principle be identified by a Raman signature, consisting of an upshift in the frequency of the E2g vibrational mode with respect to the bulk value, but the origin of this shift (intrinsic or support-induced) is still debated. Herein we use density functional theory calculations to investigate whether there is an intrinsic Raman shift in the h-BN monolayer in comparison with the bulk. There is universal agreement among all tested functionals in predicting the magnitude of the frequency shift upon a variation in the in-plane cell parameter. It is clear that a small in-plane contraction can explain the Raman peak upshift from bulk to monolayer. However, we show that the larger in-plane parameter in the bulk (compared to the monolayer) results from non-local correlation effects, which cannot be accounted for by local functionals or those with empirical dispersion corrections. Using a non-local-correlation functional, we then investigate the effect of finite temperatures on the Raman signature. We demonstrate that bulk h-BN thermally expands in the direction perpendicular to the layers, while the intralayer distances slightly contract, in agreement with observed experimental behavior. Interestingly, the difference in in-plane cell parameter between bulk and monolayer decreases with temperature, and becomes very small at room temperature. We conclude that the different thermal expansion of bulk and monolayer partially "erases" the intrinsic Raman signature, accounting for its small magnitude in recent experiments on suspended samples.

cond-mat.mtrl-sci↗

arXiv2017

Phonon Eigenspectrum-Based Formulation of the Atomistic Green's Function Method

While the atomistic Green's function (AGF) method has the potential to compute spectrally resolved phonon transport across interfaces, most prior formulations of the AGF method provide only the total phonon transmission function that includes contributions from all phonon branches or channels. In this work, we present a formulation of the conventional AGF technique in terms of phonon eigenspectra that provides a natural decomposition of the total transmission function into contributions from various phonon modes. The method involves the use of Dyson and Lippmann-Schwinger equations to determine surface Green's functions from the phonon eigenspectrum of the bulk, and establishes a direct connection between the transmission function and the bulk phonon spectra of the materials forming the interface. We elucidate our formulation of the AGF technique through its application to a microscopic picture of phonon mode conversion at Si-Ge interfaces with atomic intermixing. Intermixing of atoms near the interface is shown to increase the phase space available for phonon mode conversion and to enhance thermal interface conductance at moderate levels of atomic mixing. The eigenspectrum-based AGF (EAGF) method should be useful in determination of microscopic mechanisms of phonon scattering and identification of the specific modes that dominate thermal transport across an interface.

cond-mat.mes-hall↗

arXiv2017

On the origin of Blue Luminescence in Mg doped GaN

We uncover the origin of blue luminescence (BL) peak in Mg doped GaN thin film using a combination of experimental X-ray absorption near edge spectroscopy (XANES), first-principles calculations based on density functional theory and full multiple scattering theoretical analysis of various possible defect complexes and their XANES signatures. We demonstrate that a defect complex composed of Mg substituted at Ga site (MgGa) and Mg at interstitial site (Mgi) is primarily responsible for the observed BL by Donor-Acceptor Pair transition (DAP) associated with a deep donor state in the gap. It correlates with a higher (lower) oxidation state of N (Ga) in heavily Mg doped GaN than in its pristine structure, evident in our experiments as well as calculations. Physical and chemical mechanisms identified here point out a route to achieving efficient p-type GaN.

cond-mat.mtrl-sci↗

arXiv2017

Chemical exfoliation of MoS2 leads to semiconducting 1T' phase and not the metallic 1T phase

A trigonal phase existing only as small patches on chemically exfoliated few layer, thermodynamically stable 1H phase of MoS2 is believed to influence critically properties of MoS2 based devices. This phase has been most often attributed to the metallic 1T phase. We investigate the electronic structure of chemically exfoliated MoS2 few layered systems using spatially resolved (lesser than 120 nm resolution) photoemission spectroscopy and Raman spectroscopy in conjunction with state-of-the-art electronic structure calculations. On the basis of these results, we establish that the ground state of this phase is a small gap (~90 meV) semiconductor in contrast to most claims in the literature; we also identify the specific trigonal (1T') structure it has among many suggested ones.

cond-mat.mtrl-sci↗

arXiv2016

Molecular Dynamics Simulations of Chemically Disordered Ferroelectric (Ba,Sr)TiO$_3$ with a Semi-Empirical Effective Hamiltonian

We present a semi-empirical effective Hamiltonian to capture effects of disorder associated with Ba and Sr cations occupying $A$ sites in (Ba$_{x}$Sr$_{1-x}$)TiO$_3$ on its ferroelectric phase transition. Averaging between the parameters of first-principles effective Hamiltonians of end members BaTiO$_3$ and SrTiO$_3$, we include a term with an empirical parameter to capture the local polarization and strains arising from the difference between ionic radii of Ba and Sr. Using mixed-space molecular dynamics of the effective Hamiltonian, we determine $T$-dependent ferroelectric phase transitions in (Ba$_{x}$Sr$_{1-x}$)TiO$_3$ which are in good agreement with experiment. Our scheme of determination of semi-empirical parameters in effective Hamiltonian should be applicable to other perovskite-type ferroelectric solid solutions.

cond-mat.mtrl-sci↗

arXiv2016

High-temperature large-gap quantum anomalous Hall insulator in ultrathin double perovskite films

Motivated by the goal of realizing topological phases in thin films and heterostructures of correlated oxides, we propose here a quantum anomalous Hall insulator (QAHI) in ultrathin films of double perovskites based on mixed 3d-5d or 3d-4d transition metal ions, grown along the [111] direction. Considering the specific case of ultrathin Ba2FeReO6, we present a theoretical analysis of an effective Hamiltonian derived from first-principles. We establish that a strong spin-orbit coupling at Re site, t2g symmetry of the low-energy d-bands, polarity of its [111] orientation of perovskite structure, and mixed 3d-5d chemistry results in room temperature magnetism with a robust QAHI state of Chern number C=1 and a large band-gap. We uncover and highlight a non-relativistic orbital-Rashba-type effect in addition to the spin-orbit coupling, that governs this QAHI state. Our prediction of a large topological band-gap of ~100 meV in electronic structure, and a magnetic transition temperature Tc~300K estimated by Monte Carlo simulations, is expected to stimulate experimental efforts at synthesis of such films and enable possible practical applications of its dissipationless edge currents.

cond-mat.str-el↗

arXiv2016

Evidence of a pseudogap driven by competing orders of multi-band origin in the ferromagnetic superconductor Sr$_{0.5}$Ce$_{0.5}$FBiS$_2$

From temperature and magnetic field dependent point-contact spectroscopy on the ferromagnetic superconductor Sr$_{0.5}$Ce$_{0.5}$FBiS$_2$ (bulk superconducting $T_c$ = 2.5 K) we observe (a) a pseudogap in the normal state that sustains to a remarkably high temperature of 40 K and (b) two-fold enhancement of $T_c$ upto 5 K in the point-contact geometry. In addition, Andreev reflection spectroscopy reveals a superconducting gap of 6 meV for certain point-contacts suggesting that the mean field $T_c$ of this system could be approximately 40 K, the onset temperature of pseudo-gap. Our results suggest that quantum fluctuations originating from other competing orders in Sr$_{0.5}$Ce$_{0.5}$FBiS$_2$ forbid a global phase coherence at high temperatures thereby suppressing $T_c$. Apart from the known ordering to a ferromagnetic state, our first-principles calculations reveal nesting of a multi-band Fermi surface and a significant electron-phonon coupling that could result in charge density wave-like instabilities.

cond-mat.supr-con↗