arXiv subjects

Dibyendu Dey

Publications and source records attributed to Dibyendu Dey.

At least 19 recordsLinked to original sources

arXiv2026

Anharmonic Lattice Dynamics and Anisotropic Electron-Phonon Coupling in Quasi-1-Dimensional Charge Density Wave Ta2NiSe7

The microscopic origin of charge density wave formation in quasi one dimensional Ta2NiSe7 remains actively debated, particularly regarding the relative contributions of Fermi surface nesting, electron phonon coupling, and lattice instabilities. Here, we combine temperature and orientation dependent polarized Raman spectroscopy with first principles calculations to uncover the anisotropic electronic and lattice interactions governing the CDW state in Ta2NiSe7. Heat capacity and electrical transport measurements identify an incommensurate CDW transition at 61 K. Raman spectroscopy reveals pronounced in plane anisotropy, with e ph coupling strength along intrachain b axis exceeding five times that along interchain c axis, whereas lattice anharmonicity is enhanced by threefold along c axis. First principles calculations identify Ta2 Se octahedral vibrations and Ta Se electronic states near the Fermi level as dominant channels mediating the anisotropic e ph interaction. Exceptionally strong and directional e ph coupling along b axis establishes lattice driven electronic instability as the primary mechanism underlying CDW modulation and highlights the dominance of intrachain interactions in strongly coupled Ta2NiSe7. Despite this strong coupling, the CDW remains incommensurate, indicating that lattice anharmonicity provides an additional degree of freedom. Enhanced anharmonicity along c axis suggests that anisotropic phonon phonon interactions reshape the free energy landscape and contribute to stabilizing incommensurate phase. These findings reveal a cooperative interplay between anisotropic e ph coupling and lattice anharmonicity in governing CDW formation in low dimensional quantum materials.

cond-mat.mtrl-sci↗

arXiv2024

Manipulating Spin-Lattice Coupling in Layered Magnetic Topological Insulator Heterostructure $via$ Interface Engineering

Induced magnetic order in a topological insulator (TI) can be realized either by depositing magnetic adatoms on the surface of a TI or engineering the interface with epitaxial thin film or stacked assembly of two-dimensional (2D) van der Waals (vdW) materials. Herein, we report the observation of spin-phonon coupling in the otherwise non-magnetic TI Bi$_\mathrm{2}$Te$_\mathrm{3}$, due to the proximity of FePS$_\mathrm{3}$ (an antiferromagnet (AFM), $T_\mathrm{N}$ $\sim$ 120 K), in a vdW heterostructure framework. Temperature-dependent Raman spectroscopic studies reveal deviation from the usual phonon anharmonicity originated from spin-lattice coupling at the Bi$_{2}$Te$_{3}$/FePS$_{3}$ interface at/below 60 K in the peak position (self-energy) and linewidth (lifetime) of the characteristic phonon modes of Bi$_{2}$Te$_{3}$ (106 cm$^{-1}$ and 138 cm$^{-1}$) in the stacked heterostructure. The Ginzburg-Landau (GL) formalism, where the respective phonon frequencies of Bi$_{2}$Te$_{3}$ couple to phonons of similar frequencies of FePS$_{3}$ in the AFM phase, has been adopted to understand the origin of the hybrid magneto-elastic modes. At the same time, the reduction of characteristic $T_\mathrm{N}$ of FePS$_3$ from 120 K in isolated flakes to 65 K in the heterostructure, possibly due to the interfacial strain, which leads to smaller Fe-S-Fe bond angles as corroborated by computational studies using density functional theory (DFT). Besides, inserting hexagonal boron nitride within Bi$_{2}$Te$_{3}$/FePS$_{3}$ stacking regains the anharmonicity in Bi$_{2}$Te$_{3}$. Controlling interfacial spin-phonon coupling in stacked heterostructure can have potential application in surface code spin logic devices.

cond-mat.mes-hall↗

arXiv2023

Possible routes to superconductivity in the surface layers of V-doped Mg$_{1-δ}$Ti$_2$O$_4$ through multiple charge transfers and suppression of Jahn-Teller activity

Superconductivity in the family of spinel oxides is very rare owing to their robust Mott-insulating nature. About half a century ago, LiTi$_2$O$_4$ became the first reported spinel compound to show superconductivity with a 12K transition temperature. Since then, several unsuccessful attempts were made to enhance the T$_c$ of this family of materials. However, a very recent experiment [arXiv:2209.02053] has reported superconductivity at a higher temperature (below 16K), in the V-doped Mg$_{1-δ}$Ti$_2$O$_4$ thin surface layer while its bulk counterpart remains Mott insulating. The superconducting T$_c$ of this material is significantly higher compared to other engineered MgTi$_2$O$_4$ thin films grown on different substrates. From our first-principles analysis, we have identified that Mg-depletion significantly reduces Jahn-Teller (JT) activity and antiferromagnetic superexchange at the surface layer of V-doped MgTi$_2$O$_4$ due to considerable charge transfer between various ions. The combined effect of a degraded antiferromagnetic order and reduced JT activity weakens the Mottness of the system, leading to the emergence of superconductivity at higher temperatures.

cond-mat.supr-con↗

arXiv2023

Descriptor-Enabled Rational Design of High-Entropy Materials Over Vast Chemical Spaces

The practically unlimited high-dimensional composition space of high-entropy materials (HEMs) has emerged as an exciting platform for functional materials design and discovery. However, the identification of stable and synthesizable HEMs and robust design rules remains a daunting challenge due to the difficulty in determining composition/structure-specific enthalpy and entropy contributions to the stability and formation of HEMs. In this work, using first-principles calculations, we find that (i) the stability and miscibility of HEMs strongly depend on the formation enthalpy of the HEM relative to the most stable completing phase rather than on the conventionally-viewed enthalpies of mixing over all possible competing phases, and (ii) the entropy forming ability of a HEM can be measured from the defect formation energy spectrum of tens of substitutional defects in ordered binary compounds, involving no sampling over numerous alloy configurations. Based on these findings, we propose a highly predictive Mixed Enthalpy-Entropy Descriptor (MEED), which enables the rational high-throughput first-principles design and screening of new HEMs over large chemical spaces. Applying the MEED to two structurally distinct material systems (i.e., 3D rocksalt carbides and 2D layered sulfides), not only all experimentally reported HEMs within each system are successfully identified, but a universal cutoff criterion for assessing their relative synthesizability also revealed. In addition, tens of new high entropy carbides and 2D high-entropy sulfides are also predicted. They have the potential for a wide variety of applications such as coating in aerospace devices, energy conversion and storage, and flexible electronics.

cond-mat.mtrl-sci↗

arXiv2022

Intrinsic ferromagnetism and restrictive thermodynamic stability in MA$_2$N$_4$ and Janus VSiGeN$_4$ monolayers

The seminal experimental discovery of the remarkably stable MoSi$_2$N$_4$ monolayer has led to a handful of predicted magnetic two-dimensional (2D) materials in the MA$_2$Z$_4$ family (M = transition metals, A = Si, Ge, and Z = N, P, As). These magnetic monolayers were predicted to be dynamically stable, but none of them has been synthesized to date. In this Research Letter, from first-principles thermodynamic stability analysis, we demonstrate that only the nitrides are thermodynamically stable and this occurs under N-rich conditions. Based on this finding, we propose two ferromagnetic, semiconducting Janus monolayers in the family: VSiGeN$_4$ and VSiSnN$_4$. They are both dynamically and thermally stable, but only the former is thermodynamically stable. Intriguingly, Janus VSiGeN$_4$ and VSiSnN$_4$ monolayers show weak in-plane anisotropy compared with the VSi$_2$N$_4$ monolayer. These two emerging Janus magnetic semiconductors offer opportunities for studying 2D magnetism and spin control for spintronics applications.

cond-mat.mtrl-sci↗

arXiv2021

Electron-Phonon Coupling and Quantum Correction to Topological Magnetoconductivity in Bi2GeTe4

We report on structure, vibrational properties and weak-antilocalization-(WAL-) induced quantum correction to magnetoconductivity in single crystal Bi2GeTe4. Surface band structure calculations show a single Dirac cone corresponding to topological surface states in Bi2GeTe4. An estimated phase coherence length, l_ϕ ~ 143 nm and prefactor α ~ - 1.54 from Hikami-Larkin-Nagaoka fitting of magnetoconductivity describe the quantum correction to conductivity. An anomalous temperature dependence of A1g Raman modes confirms enhanced electron-phonon interactions. Our results establish the involvement of vibrations of Bi-Te with existence of topological surface states and WAL in Bi2GeTe4.

cond-mat.mtrl-sci↗

arXiv2021

Moiré skyrmions and chiral magnetic phases in twisted CrX$_{3}$ (X $=$ I, Br, Cl) bilayers

We present a comprehensive theory of the magnetic phases in twisted bilayer Cr-trihalides through a combination of first-principles calculations and atomistic simulations. We show that the stacking-dependent interlayer exchange leads to an effective moiré field that is mostly ferromagnetic with antiferromagnetic patches. A wide range of noncollinear magnetic phases can be stabilized as a function of the twist angle and Dzyaloshinskii-Moriya interaction as a result of the competing interlayer antiferromagnetic coupling and the energy cost for forming domain walls. In particular, we demonstrate that for small twist angles various skyrmion crystal phases can be stabilized in both CrI$_3$ and CrBr$_3$. Our results provide an interpretation for the recent observation of noncollinear magnetic phases in twisted bilayer CrI$_3$ and demonstrate the possibility of engineering further nontrivial magnetic ground states in twisted bilayer Cr-trihalides.

cond-mat.str-el↗

arXiv2020

Structural, electronic, and magnetic properties of Vanadium-based Janus dichalcogenide monolayers: A first-principles study

The structural, electronic, and magnetic properties of VSSe, VSeTe, VSTe monolayers in both 2H and 1T phases are investigated via first-principles calculations. The 2H phase is energetically favorable in VSSe and VSeTe, whereas the 1T phase is lower in energy in VSTe. For V-based Janus monolayers in the 2H phase, calculations of the magnetic anisotropy show an easy-plane for the magnetic moment. As such, they should not exhibit a ferromagnetic phase transition, but instead, a Berezinskii-Kosterlitz-Thouless (BKT) transition. A classical XY model with nearest-neighbor coupling estimates critical temperatures (T$_{BKT}$) ranging from 106 K for VSSe to 46 K for VSTe.

cond-mat.mtrl-sci↗

arXiv2020

Role of chemical pressure on the electronic and magnetic properties of spin-1/2 kagome mineral averievite

We investigate the electronic and magnetic properties of the kagome mineral averievite (CsCl)Cu$_5$V$_2$O$_{10}$ and its phosphate analog (CsCl)Cu$_5$P$_2$O$_{10}$ using first-principles calculations. The crystal structure of these compounds features Cu$^{2+}$ kagome layers sandwiched between Cu$^{2+}$-P$^{5+}$/Cu$^{2+}$-V$^{5+}$ honeycomb planes, with pyrochlore slabs made of corner-sharing Cu-tetrahedra being formed. The induced chemical pressure effect upon substitution of V by P causes significant changes in the structure and magnetic properties. Even though the in-plane antiferromagnetic (AFM) coupling (J$_1$) within the kagome layer is similar in the two materials, the inter-plane AFM coupling (J$_2$) between kagome and honeycomb layers is five times larger in the P-variant increasing the degree of magnetic frustration in the constituting Cu-tetrahedra.

cond-mat.mtrl-sci↗

arXiv2020

Ferroelectric Polarization in Antiferroelectric Chalcogenide Perovskite BaZrS3 Thin Film

Bulk chalcogenide perovskite BaZrS3 (BZS), with a direct band gap in visible region, is an important photovoltaic material, albeit with limited applicability owing to its antiferroelectric (AF) nature. Presently, ferroelectric (FE) perovskite-based photovoltaics are attracting enormous attention for environmental stability and better energy conversion efficiency through enhanced charge separation, owing to loss of center of inversion symmetry. We report on antiferroelectric-ferroelectric (AF-FE) phases of BZS thin film, grown with chemical vapor deposition (CVD), using temperature-dependent Raman investigations and first-principles calculations. The origin of FE phases is established from anomalous behavior of A7g ~ 300 cm-1 and B1g5 ~ 420 cm-1 modes, which involves the vibration of atoms at apical site of ZrS6 octahedra. Additionally, below 60 K, B1g1 and B2g2 ( ~ 85 cm-1) modes appear whereas B12g (~ 60 cm-1) disappears to stabilize the Pnma structure against ferroelectricity by local distortion. Here, B2g2 and B1g2 involve vibrations of Ba atoms in AF manner while B1g1 involves, in addition, the rotation of octahedra as well. Our first-principles calculations confirm that FE appears as a result of loss of center of inversion symmetry in ZrS6 octahedra due to existence of oxygen (O) impurities placed locally at apical sites of sulfur (S) atom.

cond-mat.mtrl-sci↗

arXiv2019

Fluorescence and FRET based mercury (II) sensor

A mercury (II) sensor has been proposed based on Fluorescence Resonance Energy Transfer (FRET) between N,N'-dioctadecyl thiacyanine perchlorate (NK) and Octadecyl rhodamine B chloride (RhB). Out of these two molecules NK is sensitive to Hg2+ ions due to presence of sulfur atom in it. Accordingly, presence of Hg2+ ions affects the NK fluorescence as well as FRET from NK to RhB. Our results showed that NK fluorescence intensity and FRET efficiency linearly decreases with increase in Hg2+ ion concentration. With proper optimization present system under investigations can be used to sense Hg2+ ions in aqueous solution with detection limit of 9.13 ppb. Advantage of this present system is that it is very simple compared to the other FRET based system and also it works under aqueous environment. This method has also been tested using real lake water and satisfactory results were obtained.

cond-mat.mtrl-sci↗

arXiv2019

Phonon dispersion, Raman spectra and evidence for spin-phonon coupling in MnV$_2$O$_4$ from first-principles

MnV$_2$O$_4$ in the spinel structure is known to exhibit coupled orbital and spin ordering, and its Raman spectra show interesting anomalies in its low-temperature phase. With a goal to explain this behavior involving coupled spins and phonons, we determine here the spin-phonon couplings in MnV$_2$O$_4$ from a theoretical analysis of its phonon spectra and their dependence on spin-ordering and electron correlations, obtained from first-principles density functional theoretical calculations. Using these in an analysis based on a Landau-like theory, we uncover the mechanism governing the Raman anomalies observed in its low-temperature phase.

cond-mat.mtrl-sci↗

arXiv2018

Rare Earth Doping and Effective Band-Convergence in SnTe for Improved Thermoelectric Performance

Thermoelectric performance of SnTe has been found to enhance with isovalent doping of alkaline and transition metal elements where most of these elements have solubility of less than 13%. We propose a strategy of doping rare earth element Yb to enhance the thermoelectric performance of SnTe. With heavy atomic mass and strong spin-orbit coupling, even the mild doping of Yb (~ 5%) is enough to create a degeneracy via band-convergence which enhances the density of states near Fermi level and improve overall performance. Our transport data and first-principles calculations corroborate that nearly 5% Yb is an efficient dopant to achieve thermoelectric response which is equivalent to 9% of Mn doping. The results are useful for understanding the environment-friendly thermoelectric SnTe.

cond-mat.mtrl-sci↗

arXiv2017

Nature of the spiral state, electric polarisation and magnetic transitions in Sr-doped YBaCuFeO$_5$: A first-principles study

Contradictory results on the ferroelectric response of type II multiferroic YBaCuFeO$_{5}$, in its incommensurate phase, has of late, opened up a lively debate. There are ambiguous reports on the nature of the spiral magnetic state. Using first-principles DFT calculations for the parent compound within LSDA+U+SO approximation, the multiferroic response and the nature of spiral state is revealed. The helical spiral is found to be more stable below the transition temperature as spins prefer to lie in ab plane. The Dzyaloshinskii-Moriya (DM) interaction and the spin current mechanism were earlier invoked to account for the electric polarisation in this system. However, the DM interaction is found to be absent, spin current mechanism is not valid in the helical spiral state and there is no electric polarisation thereof. These results are in good agreement with the recent single-crystal data. We also investigate the magnetic transitions in YBa$_{1-x}$Sr$_x$CuFeO$_5$ for the entire range $0\le x\le 1$ of doping. The exchange interactions are estimated as a function of doping and a quantum Monte Carlo (QMC) calculation on an effective spin Hamiltonian shows that the paramagnetic to commensurate phase transition temperature increases with doping till $x=0.5$ and decreases beyond. Our observations are consistent with experimental findings.

cond-mat.mtrl-sci↗

arXiv2016

First-Principles Correlated Approach to the Normal State of Strontium Ruthenate

The interplay between multiple bands, sizable multi-band electronic correlations and strong spin-orbit coupling may conspire in selecting a rather unusual unconventional pairing symmetry in layered Sr$_{2}$RuO$_{4}$. This mandates a detailed revisit of the normal state and, in particular, the $T$-dependent incoherence-coherence crossover. Using a modern first-principles correlated view, we study this issue in the actual structure of Sr$_{2}$RuO$_{4}$ and present a unified and quantitative description of a range of unusual physical responses in the normal state. Armed with these, we propose that a new and important element, that of dominant multi-orbital charge fluctuations in a Hund's metal, may be a primary pair glue for unconventional superconductivity. Thereby we establish a connection between the normal state responses and superconductivity in this system.

cond-mat.str-el↗

arXiv2016

The Iso-electronic Series $Ca_{2-x}Sr_{x}RuO_{4}$: Structural Distortion, Effective Dimensionality, Spin Fluctuations and Quantum Criticality

The iso-electronic $d^{4}$ compounds of the $4d$ series show rich phase diagrams due to competing spin, charge and orbital degrees of freedom in presence of strong correlations and structural distortions. One such iso-electronic series, $Ca_{2-x}Sr_{x}RuO_{4}$, is studied within the GGA (and spin-orbit coupled GGA) plus DMFT formalism using the hybridization expansion of continuous time Quantum Monte Carlo solver. While the local dynamical correlations make $Sr_{2}RuO_{4}$ a Hund's metal, they drive $Ca_{2}RuO_{4}$ to a Mott insulating ground state. We study the dynamic and static single-particle and local irreducible vertex-corrected two-particle responses at three different points ($x = 2.0, 0.5, 0.0$) to understand the anomalous cross-over from Hund's metal ($x = 2.0 $) to a Mott insulator ($x = 0 $) and find that a structural distortion is likely to be responsible for the cross-over. Further, dynamical correlations reveal that the band-width ($W$) of the Hund's metal is larger than its effective local Hubbard $U$, and a finite Hund's coupling $J_{H}$ helps it remain in a bad metallic and nearly spin-frozen state over a large temperature range. $Ca_{2}RuO_{4}$, on the other hand, is intrinsically driven to the proximity of a Mott transition due to narrowing of band width ($U/W > 1.5$), though its finite temperature excitations indicate bad metallicity. We show that there is a critical end point of second-order structural transition at $x = 0.5$, where spin fluctuations become critically singular and follow the exact scaling of conformally invariant boundary field theory. The critical end point of quasi-$3D$ nature is associated with an effective dimensional cross-over between the $x = 2.0$ and $x=0.0$ quasi-$2D$ structures. Finally we draw a modified magnetic phase diagram of the material, showing a fan-like region starting from the quantum critical end point at $x = 0.5.$

cond-mat.str-el↗

arXiv2015

Orbital Ordering in Fe$_{1-x}$Mn$_x$V$_2$O$_4$: A First Principles Study

Long range orbital order has been investigated in Fe$_{1-x}$Mn$_x$V$_2$O$_4$ as a function of doping (x) using first principles density functional theory calculations including the effects of Coulomb correlation and spin-orbit interaction within GGA+U and GGA+U+SO approximations. Through a detailed analysis of corresponding Wannier orbital projections of the Vanadium d bands, we have clearly established that for x$\le$0.6, the orbital order at V sites consists of a linear superposition of d$_{xz}$ and d$_{yz}$ orbitals of the type d$_{xz}\pm$d$_{yz}$. Within each ab-plane a ferro-orbital ordering of either d$_{xz}$+d$_{yz}$ or d$_{xz}$-d$_{yz}$ is observed which alternates in successive ab-planes along the c-direction. On the contrary, for x$>$0.6, it is the d$_{xz}$ or d$_{yz}$ orbital which orders at V sites in successive ab-planes along c-direction (so called A-type ordering). At Fe sites, we observe an orbital ordering of d$_{x^2-y^2}$ orbitals for x$\le$0.6 and d$_{z^2}$ orbitals for x$>$0.6. Effect of spin-orbit interaction on orbital ordering is found to be not significant in the entire range of doping studied.

cond-mat.str-el↗

arXiv2014

Formation of fluorescent H aggregates of a cyanine dye in LB films and its effect on energy transfer

Here we report the formation of fluorescent H aggregates of a cyanine dye Oxa18 in ultrathin film and its effect on energy transfer between Oxa18 and sRhb. Ideally H aggregate do not fluoresce. However, due to imperfect stacking of Oxa18 molecules in the aggregates, fluorescence occurred from Oxa18 H aggregates. This H aggregated band has substantial effect on the enhancement of energy transfer from Oxa18 to sRhb both in solution and in ultrathin film.

cond-mat.mtrl-sci↗