Showing 1–45 of 45 results for author: Mandal, A

Multiconfigurational Mixed Quantum-Classical Approach for Correlated Many-Body Dynamics

Authors: Pritha Ghosh, Rajanya Sarkar, Arkajit Mandal

Abstract: In this work, we introduce a multiconfigurational mixed quantum-classical many-body approach for simulating the finite-temperature correlated multi-exciton dynamics in the presence of phonon-induced static and dynamic disorder. In this mixed quantum-classical approach, the excitonic subsystem is described using a multiconfigurational wavefunction that extends beyond the mean-field limit, while the… ▽ More In this work, we introduce a multiconfigurational mixed quantum-classical many-body approach for simulating the finite-temperature correlated multi-exciton dynamics in the presence of phonon-induced static and dynamic disorder. In this mixed quantum-classical approach, the excitonic subsystem is described using a multiconfigurational wavefunction that extends beyond the mean-field limit, while the phonons are evolved quasi-classically. Using this approach, we simulate a multi-excitonic dissipative system and show how the interplay between phonon-induced dynamic disorder and exciton-exciton many-body interactions determines excitation-dependent excitonic transport and spatial correlations. Our results show that while the mean-field approach produces semi-quantitatively accurate diffusive dynamics, it does not capture the spatial correlations as expected. We find that a mean-field path approximation, where we generate pre-computed trajectories using our mean-field mixed quantum-classical approach and then perform multiconfigurational dynamics, can reproduce the spatial correlations to a good accuracy, positioning this approach as an efficient method for capturing spatial correlations in complex systems. △ Less

Submitted 25 July, 2026; originally announced July 2026.

Topological Hall effect due to electron-skyrmion scattering

Authors: Arijit Mandal, Hareram Swain, B. R. K. Nanda, S. Satpathy

Abstract: Electron scattering from chiral spin textures such as skyrmions is fundamental to the understanding of transport in more complex systems, including skyrmion crystals. Most of the previous studies have focused on the weak-coupling regime, where the exchange interaction is small compared with the electron energy. Real materials, however, often lie in the strong-coupling regime, which exhibits qualit… ▽ More Electron scattering from chiral spin textures such as skyrmions is fundamental to the understanding of transport in more complex systems, including skyrmion crystals. Most of the previous studies have focused on the weak-coupling regime, where the exchange interaction is small compared with the electron energy. Real materials, however, often lie in the strong-coupling regime, which exhibits qualitatively different behavior. Using the Lippmann-Schwinger equation and Green's function formalism, valid for all coupling strengths, we uncover several new features in the scattering cross section, including Ramsauer-Townsend minima, pronounced intermediate-coupling resonances, and Landau-level resonances for skyrmions with larger winding numbers. These features strongly influence the topological and spin Hall conductivities, which depend sensitively on the incident electron energy. Our work provides important insights into the Hall transport in collective chiral spin textures such as the skyrmion crystal. △ Less

Submitted 1 July, 2026; originally announced July 2026.

Comments: 12 pages, 12 figures, and 1 table

Many-Body Second Order Green's Function Theory for Ab Initio Molecular Quantum Electrodynamics

Authors: Amirhosein Amini, Jaime Cerda, Leopoldo Mejía, Arkajit Mandal

Abstract: In this work, we develop two many-body quantum electrodynamic methods to calculate the ground-state energies of strongly coupled light-matter molecular systems. Specifically, we extend the second-order many-body Green's function theory (GF2) for electronic systems to incorporate electron-boson couplings. We employ two ansätze to treat the bosonic part of the system, namely the coherent-state (CS)… ▽ More In this work, we develop two many-body quantum electrodynamic methods to calculate the ground-state energies of strongly coupled light-matter molecular systems. Specifically, we extend the second-order many-body Green's function theory (GF2) for electronic systems to incorporate electron-boson couplings. We employ two ansätze to treat the bosonic part of the system, namely the coherent-state (CS) and Lang-Firsov (LF) transformed vacuum state. These are combined with the GF2 method to construct two new approaches, which we refer to as CS-GF2 and LF-GF2. We benchmark CS- and LF-GF2 by studying various molecular systems inside an optical cavity. We investigate $\mathrm{H}_2$ and $\mathrm{LiH}$ potential energy surfaces, keto-eneol tautomerization energy barrier, van-der Waals interactions between two $\mathrm{H_2}$ molecules and the torsional potential energy surface of the ethylene molecule, $\mathrm{C_2H_4}$. Both methods provide highly accurate energies, with only modest additional improvement observed in LF-GF2. △ Less

Submitted 24 June, 2026; originally announced June 2026.

Anomalous Hall Effect in Silicon-Compatible Altermagnetic alpha-MnTe Thin Films

Authors: Rajib Sarkar, Subhransu Kumar Negi, Arindom Das, Arijit Mandal, Pankaj Bhardwaj, Sohini Guin, Aryaman Das, Naresh Shyaga, Laxmipriya Nanda, B. R. K. Nanda, Dhavala Suri

Abstract: Integrating spin-dependent functionality with mainstream semiconductor technology is a central goal of modern spintronics, yet most candidate materials remain incompatible with silicon-based platforms. Here, we report the direct epitaxial integration of alpha-MnTe thin films on Si(111) via molecular beam epitaxy and demonstrate a robust anomalous Hall effect (AHE) in this silicon-compatible alterm… ▽ More Integrating spin-dependent functionality with mainstream semiconductor technology is a central goal of modern spintronics, yet most candidate materials remain incompatible with silicon-based platforms. Here, we report the direct epitaxial integration of alpha-MnTe thin films on Si(111) via molecular beam epitaxy and demonstrate a robust anomalous Hall effect (AHE) in this silicon-compatible altermagnetic system. Despite the absence of net magnetization, the films exhibit a pronounced hysteretic Hall response, providing clear evidence of finite Berry curvature generated by symmetry breaking in the thin-film geometry. High resolution structural and spectroscopic characterization confirms phase-pure, epitaxial growth with hexagonal NiAs-type symmetry, while magnetotransport measurements reveal correlated hysteresis in both transverse and longitudinal channels with systematic temperature evolution. First-principles calculations reveal substantial uncompensated Berry curvature arising from the spin-split band structure consistent with altermagnetic symmetry and the origin of the observed Hall response. These results establish MnTe/Si(111) as a silicon-compatible altermagnetic platform and chart a concrete pathway for embedding Berry-phase-driven functionalities into scalable semiconductor device architectures. △ Less

Submitted 25 May, 2026; originally announced May 2026.

Giant optical spin-orbit interactions in ferroelectric van der Waals waveguides

Authors: Ding Xu, Saeed Rahmanian Koshkaki, Vicente Galicia, Chun-Ying Huang, Victoria Quirós-Cordero, Jakhangirkhodja A. Tulyagankhodjaev, André Koch Liston, Daniel G. Chica, Emma Lian, Amirhosein Amini, Yongseok Hong, Taketo Handa, P. James Schuck, Xiaoyang Zhu, Xavier Roy, Arkajit Mandal, Milan Delor

Abstract: Optical spin-orbit interactions (SOI) link photonic spin to momentum, offering a route toward on-chip polarization control and beam steering. Nevertheless, achieving sufficient optical SOI and nonlinearities on sub-micrometer scales - a prerequisite for dense photonic integration - remains an outstanding challenge. Here, we show that highly birefringent van der Waals (vdW) waveguides provide an id… ▽ More Optical spin-orbit interactions (SOI) link photonic spin to momentum, offering a route toward on-chip polarization control and beam steering. Nevertheless, achieving sufficient optical SOI and nonlinearities on sub-micrometer scales - a prerequisite for dense photonic integration - remains an outstanding challenge. Here, we show that highly birefringent van der Waals (vdW) waveguides provide an ideal, chip-compatible platform to address this limitation. We focus on the ferroelectric semiconductor NbOI2, which exhibits record optical nonlinearities and dielectric anisotropy. Using femtosecond optical microscopy, we image light propagation and harmonic conversion beyond the total internal reflection barrier over tens of micrometers in NbOI2 slab waveguides. We report giant optical spin-splitting through the optical spin Hall effect, which facilitates spatial separation of optical spin currents on sub-micrometer scales, in quantitative agreement with a microscopic light-matter interaction model. We further leverage optical spin-momentum locking to realize polarization-controlled waveguide steering. We generalize these observations across various vdW waveguides and empirically confirm a scaling law linking dielectric anisotropy to geometric spin-splitting. Our results establish highly anisotropic vdW waveguides as an ideal platform for densely integrated opto-spintronic technologies. △ Less

Submitted 13 May, 2026; originally announced May 2026.

Effect of symmetry breaking on altermagnetism in CrSb and Formation of fragmented nodal curves

Authors: Arindom Das, Arijit Mandal, Nayana Devaraj, B. R. K. Nanda

Abstract: Phenomena concerning altermagnets have opened up a window for unconventional analysis of the momentum space spin polarization (MSSP) of antiferromagnetic materials. Taking the example of one of the widely investigated altermagnets, CrSb, we explore the underlying mechanisms leading to the formation or breaking of altermagnetism. With the aid of DFT calculation and symmetry analysis, we study the b… ▽ More Phenomena concerning altermagnets have opened up a window for unconventional analysis of the momentum space spin polarization (MSSP) of antiferromagnetic materials. Taking the example of one of the widely investigated altermagnets, CrSb, we explore the underlying mechanisms leading to the formation or breaking of altermagnetism. With the aid of DFT calculation and symmetry analysis, we study the behavior of MSSP in the altermagnetic bands of pristine CrSb, along with a few model structures designed from the pristine one by hypothetical vacancy engineering and interstitial doping. We show that the six-fold rotational symmetry of the pristine CrSb can be reduced to a two-fold rotational symmetry via vacancy and doping engineering. We discover the formation of fragmented nodal curves (FNCs) across the Brillouin zone when in an altermagnetic material when the symmetry is restricted to two-fold rotation. Unlike the typical nodal planes and axes, the location of the FNCs in the momentum space is found to be band-specific. The formation of FNCs is further validated by introducing uniaxial strain to CrSb and by examining the band structure of RbMnPO$_4$, as they both exhibit a two-fold rotational symmetry responsible for altermagnetism. We observe that, unlike the pristine case, these FNCs have the potential to manifest anomalous Hall conductivities (AHC), while the Néel vector orients along both in-plane and out-of-plane directions. This flexibility of the AHC will pave the way for the application of altermagnets in the futuristic quantum devices. △ Less

Submitted 24 February, 2026; originally announced February 2026.

Comments: 11 pages, 8 figures, and 2 tables

Mechanistic principles of exciton-polariton relaxation

Authors: Ian Haines, Arshath Manjalingal, Logan Blackham, Saeed Rahamanian Koshkaki, Arkajit Mandal

Abstract: Exciton-polaritons are light-matter hybrid quasi-particles that have emerged as a flexible platform for developing quantum technologies and engineering material properties. However, the fundamental mechanistic principles that govern their dynamics and relaxation remain elusive. In this work, we provide the microscopic mechanistic understanding of the exciton-polariton relaxation process that follo… ▽ More Exciton-polaritons are light-matter hybrid quasi-particles that have emerged as a flexible platform for developing quantum technologies and engineering material properties. However, the fundamental mechanistic principles that govern their dynamics and relaxation remain elusive. In this work, we provide the microscopic mechanistic understanding of the exciton-polariton relaxation process that follows from an excitation in the upper polariton. Using both mixed quantum-classical simulations and analytical analysis, we reveal that phonon-induced upper-to-lower polariton relaxation proceeds via two steps: the first step is a vertical inter-band transition from the upper to the lower polariton, which is followed by a second step that is a phonon-induced Fröhlich scattering within the lower polariton. We find that in materials of finite thickness (which include filled cavities), phonon-induced polaritonic intraband Fröhlich scattering is significantly suppressed. We show that the microscopic origin of this suppression is phonon-fluctuations synchronization (or self-averaging) due to the polaritonic spatial delocalization in the quantization direction. Finally, we show that the same phonon fluctuation-synchronization effect plays a central role across polaritonic relaxation pathways, and we derive simple analytical expressions that relate a material's finite thickness to the corresponding relaxation rate constants. △ Less

Submitted 13 January, 2026; originally announced January 2026.

On-the-Fly Cavity-Molecular Dynamics of Vibrational Polaritons

Authors: Sachith Wickramasinghe, Amirhosein Amini, Arkajit Mandal

Abstract: In this work, we combine the density functional tight-binding (DFTB) approach with a light-matter Hamiltonian beyond the long-wavelength approximation to propagate the dynamics of vibrational polaritons formed by coupling molecular vibrations to confined radiation inside a Fabry-Pérot optical cavity. Here, we develop a parallelized propagation scheme with lightweight inter-CPU communication by exp… ▽ More In this work, we combine the density functional tight-binding (DFTB) approach with a light-matter Hamiltonian beyond the long-wavelength approximation to propagate the dynamics of vibrational polaritons formed by coupling molecular vibrations to confined radiation inside a Fabry-Pérot optical cavity. Here, we develop a parallelized propagation scheme with lightweight inter-CPU communication by exploiting the sparse nature of the light-matter interactions in the real space representation. We find that the computationally expensive Born charges required for our propagation can be replaced with the computationally inexpensive Mulliken charges to obtain qualitatively accurate linear spectra especially when the nonlinearity (arising from molecular vibrations) of the light-matter interaction term is not substantial. However, the same approach may not be suitable to be used for studying cavity modification of energy transport or chemical dynamics as this approximation leads to spurious heating of the light-matter hybrid system. We demonstrate the utility of this on-the-fly approach to compute angle resolved polaritonic spectra of water. We implement our approach as an open-source computational package, CavOTF, which is available on GitHub. △ Less

Submitted 2 December, 2025; originally announced December 2025.

Quantum Dynamics of Electron Scattering from Skyrmions

Authors: Hareram Swain, Arijit Mandal, S. Satpathy, B. R. K. Nanda

Abstract: Scattering of electrons from chiral spin textures such as the skyrmions is an emerging research area due to its richness in topological quantum transport, which is significant for spintronic devices. We study the dynamical process of scattering of the spin-$\frac{1}{2}$ particles in the form of Gaussian wavepackets from skyrmions with the aid of the non-relativistic time-dependent Schrödinger equa… ▽ More Scattering of electrons from chiral spin textures such as the skyrmions is an emerging research area due to its richness in topological quantum transport, which is significant for spintronic devices. We study the dynamical process of scattering of the spin-$\frac{1}{2}$ particles in the form of Gaussian wavepackets from skyrmions with the aid of the non-relativistic time-dependent Schrödinger equation. The scattering cross section shows a rich angular dependence and is deterministically influenced by the iterative flipping of the spin state inside the skyrmion. The latter leads to a set of non-trivial outcomes which include finite transmission and reflection probabilities irrespective of interaction strength, formation of secondary wavefronts associated with back-converted spin components, and a long-lived quasi-bound state at the scattering center. In addition to the rich and intriguing physics, the numerical recipe developed here can be easily adopted for any arbitrary spin texture, which will prepare a playground to explore tunable spin transport. △ Less

Submitted 2 March, 2026; v1 submitted 23 September, 2025; originally announced September 2025.

Comments: 15 pages, 9 figures, 1 table

Unlocking Doping Effects on Altermagnetism in MnTe: Emergence of Quasi-altermagnetism

Authors: Nayana Devaraj, Anumita Bose, Arindom Das, Md Afsar Reja, Arijit Mandal, Awadhesh Narayan, B. R. K. Nanda

Abstract: Governed by specific symmetries, altermagnetism is an emerging field in condensed matter physics, characterized by unique spin-splitting of the bands in the momentum space co-existing with the compensated magnetization as in antiferromagnets. As crystals can have tailored and unintended defects, it is important to gain insights on how altermagnets are affected by the defects-driven symmetry-breaki… ▽ More Governed by specific symmetries, altermagnetism is an emerging field in condensed matter physics, characterized by unique spin-splitting of the bands in the momentum space co-existing with the compensated magnetization as in antiferromagnets. As crystals can have tailored and unintended defects, it is important to gain insights on how altermagnets are affected by the defects-driven symmetry-breaking which, in turn, can build promising perspectives on potential applications. In this study, considering the widely investigated MnTe as a prototype altermagnet, defects are introduced through substitutional doping to create a large configuration space of spin space groups. With the aid of density functional theory calculations, symmetry analysis, and model studies in this configuration space, we demonstrate the generic presence of spin-split of the antiferromagnetic bands in the momentum space. This is indicative of a wider class of quasi-altermagnetic materials, augmenting the set of ideal altermagnetic systems. Furthermore, we show that while pristine MnTe does not show anomalous Hall conductivity (AHC) with out-of-plane magnetization, suitable doping can be carried out to obtain finite and varied AHC. Our predictions of quasi-altermagnetism and doping-driven tailored AHC have the potential to open up as-yet-unexplored directions in this developing field. △ Less

Submitted 27 March, 2026; v1 submitted 27 August, 2025; originally announced August 2025.

Comments: 17 pages, 11 figures, and 1 table

Journal ref: Phys. Rev. B, 113, 104438 (2026)

Tilted Material in an Optical Cavity: Light-Matter Moiré Effect and Coherent Frequency Conversion

Authors: Arshath Manjalingal, Saeed Rahmanian Koshkaki, Logan Blackham, Arkajit Mandal

Abstract: Exciton-polaritons formed inside optical cavities offer a highly tunable platform for exploring novel quantum phenomena. Here, we introduce and theoretically characterize a light-matter moiré effect (LMME) that arises when a 2D material is tilted inside a planar optical cavity, in contrast to stacking multiple layers at a twist angle as is done in forming 2D moiré hetero-structures. We show that t… ▽ More Exciton-polaritons formed inside optical cavities offer a highly tunable platform for exploring novel quantum phenomena. Here, we introduce and theoretically characterize a light-matter moiré effect (LMME) that arises when a 2D material is tilted inside a planar optical cavity, in contrast to stacking multiple layers at a twist angle as is done in forming 2D moiré hetero-structures. We show that this geometric tilt produces emergent periodicity in the light-matter coupling, yielding displaced replicas of the polariton dispersion and flat bands near the Brillouin-zone center. Through time-dependent quantum dynamical simulations, we demonstrate that LMME enables coherent frequency conversion and remains robust against phonon-induced decoherence. Our findings establish LMME as a new platform for engineering polariton band structures, the generation of flat bands and performing coherent frequency conversion relevant for developing polariton-based quantum devices. △ Less

Submitted 15 August, 2025; originally announced August 2025.

Mixed Quantum-Classical Methods for Polaron Spectral Functions

Authors: Haimi Nguyen, Arkajit Mandal, Ankit Mahajan, David R. Reichman

Abstract: In this work, using two distinct semiclassical approaches, namely the mean-field Ehrenfest (MFE) method and the mapping approach to surface hopping (MASH), we investigate the spectral function of a single charge interacting with phonons on a lattice. This quantity is relevant for the description of angle-resolved photoemission experiments. Focusing on the one-dimensional Holstein model, we compare… ▽ More In this work, using two distinct semiclassical approaches, namely the mean-field Ehrenfest (MFE) method and the mapping approach to surface hopping (MASH), we investigate the spectral function of a single charge interacting with phonons on a lattice. This quantity is relevant for the description of angle-resolved photoemission experiments. Focusing on the one-dimensional Holstein model, we compare the performance of these approaches across a range of coupling strengths and lattice sizes, exposing the relative strengths and weaknesses of each. We demonstrate that these approaches can be efficiently applied with reasonable accuracy to ab initio polaron models. Our work provides a route to the calculation of spectral properties in realistic electron-phonon-coupled systems in a computationally inexpensive manner with encouraging accuracy. △ Less

Submitted 22 October, 2025; v1 submitted 19 May, 2025; originally announced May 2025.

Mean-field Mixed Quantum-Classical Approach for Many-Body Quantum Dynamics of Exciton-Polaritons

Authors: Pritha Ghosh, Arshath Manjalingal, Sachith Wickramasinghe, Saeed Rahmanian Koshkaki, Arkajit Mandal

Abstract: In this work, we use a mixed quantum-classical (mean-field) many-body approach for simulating the quantum dynamics of excitons and exciton-polaritons beyond the single-excitation subspace. We combine the multitrajectory Ehrenfest approach, which propagates slow degrees of freedom classically, with the Gross-Pitaevskii method, which propagates fast degrees of freedom in a mean-field fashion. We use… ▽ More In this work, we use a mixed quantum-classical (mean-field) many-body approach for simulating the quantum dynamics of excitons and exciton-polaritons beyond the single-excitation subspace. We combine the multitrajectory Ehrenfest approach, which propagates slow degrees of freedom classically, with the Gross-Pitaevskii method, which propagates fast degrees of freedom in a mean-field fashion. We use this mean-field many-body Ehrenfest approach to analyze how the phonon-induced dynamic disorder and the many-body interaction affect the incoherent and coherent dynamics of excitons and exciton-polaritons. We examine how the number of excitations and the strength of repulsive exciton-exciton interaction nonlinearly influence the transport, Fröhlich scattering and decoherence. △ Less

Submitted 6 May, 2025; originally announced May 2025.

Exciton-Polariton Dynamics in Multilayered Materials

Authors: Saeed Rahmanian Koshkaki, Arshath Manjalingal, Logan Blackham, Arkajit Mandal

Abstract: Coupling excitons with quantized radiation has been shown to enable coherent ballistic transport at room temperature inside optical cavities. Previous theoretical works employ a simple description of the material, depicting it as a one-dimensional single layer placed in the middle of an optical cavity, thereby ignoring the spatial variation of the radiation field. In contrast, in most experiments,… ▽ More Coupling excitons with quantized radiation has been shown to enable coherent ballistic transport at room temperature inside optical cavities. Previous theoretical works employ a simple description of the material, depicting it as a one-dimensional single layer placed in the middle of an optical cavity, thereby ignoring the spatial variation of the radiation field. In contrast, in most experiments, the optical cavity is filled with organic molecules or multiple layers of two-dimensional materials. Here, we develop an efficient mixed-quantum-classical approach, introducing a bright layer description, to simulate the exciton-polariton quantum dynamics in three dimensions. Our simulations reveal that, for the same Rabi splitting, a multilayered material extends the quantum coherence lifetime and enhances transport compared to a single-layer material. We find that this enhanced coherence can be traced to a synchronization of phonon fluctuations over multiple layers, wherein the collective light-matter coupling in a multilayered material effectively suppresses the phonon-induced dynamical disorder. △ Less

Submitted 1 September, 2025; v1 submitted 18 February, 2025; originally announced February 2025.

Towards Accurate Mixed Quantum Classical Simulations of Vibrational Polaritonic Chemistry

Authors: Muhammad R. Hasyim, Arkajit Mandal, David R. Reichman

Abstract: Interest in vibrational polaritonic chemistry, where ground-state chemical kinetics are modified via confined optical modes in a cavity, has surged in recent years. Although models have been developed to understand cavity-modified reactions, fully quantum mechanical simulations remain out of reach for the collective regime that involves many molecules, a critical aspect of the phenomenon. Mixed qu… ▽ More Interest in vibrational polaritonic chemistry, where ground-state chemical kinetics are modified via confined optical modes in a cavity, has surged in recent years. Although models have been developed to understand cavity-modified reactions, fully quantum mechanical simulations remain out of reach for the collective regime that involves many molecules, a critical aspect of the phenomenon. Mixed quantum-classical (MQC) simulations offer a scalable alternative, but their accuracy requires testing and potential improvements even in the single-molecule limit. In this work, we take this step by first introducing the mapping approach to surface hopping (MASH) to address the limitations of traditional MQC methods. Second, we incorporate a quantum treatment of the cavity mode, moving beyond the classical approximations often employed in previous studies. Results for a single-molecule model of vibrational polaritonic chemistry show that combining MASH with a quantum cavity mode yields the most accurate rates. However, this scheme may produce different long-time population dynamics at zero coupling depending on whether the cavity mode is quantized; a problem known as size-inconsistency in MASH. We address this problem proposing the $ε$-MASH approach, which forbids hopping between states with negligible nonadiabatic couplings (NACs). Combining MASH with a quantum cavity mode thus provides a promising approach for scalable and accurate MQC simulations in the collective regime. △ Less

Submitted 6 February, 2025; originally announced February 2025.

Comments: 14 pages, 9 figures

Microscopic Theory of Polaron-Polariton Dispersion and Propagation

Authors: Logan Blackham, Arshath Manjalingal, Saeed R. Koshkaki, Arkajit Mandal

Abstract: We develop an analytical microscopic theory to describe the polaron-polariton dispersion, formed by hybridizing excitons, photons, and phonons, and their coherent dynamics inside optical cavities. Starting from a microscopic light-matter Hamiltonian, we derive a simple analytical model by pursuing a non-perturbative treatment of the phonon and photon couplings to excitons. Within our theoretical f… ▽ More We develop an analytical microscopic theory to describe the polaron-polariton dispersion, formed by hybridizing excitons, photons, and phonons, and their coherent dynamics inside optical cavities. Starting from a microscopic light-matter Hamiltonian, we derive a simple analytical model by pursuing a non-perturbative treatment of the phonon and photon couplings to excitons. Within our theoretical framework, the phonons are treated as classical fields that are then quantized via the Floquet formalism. We show that, to a good approximation, the entire polaron-polariton system can be described using a band picture despite the phonons breaking translational symmetry. Our theory also sheds light on the long-lived coherent ballistic motion of exciton-polaritons with high excitonic character that propagate with group velocities lower than is expected from pure exciton-polariton bands, offering a microscopic explanation for these puzzling experimental observations. △ Less

Submitted 12 March, 2025; v1 submitted 27 January, 2025; originally announced January 2025.

Deterministic role of chemical bonding in the formation of altermagnetism: Reflection from correlated electron system NiS

Authors: Arijit Mandal, Arindom Das, B. R. K. Nanda

Abstract: Altermagnetism, a new collinear magnetic state, has gained significant attention in the last few years, and the underlying mechanisms driving this quantum phase are still evolving. Going beyond the group theoretical analyses, which focus on providing a binary description of the presence or absence of the altermagnetic state, in this work, we explore the role of crystal chemical bonding. As the lat… ▽ More Altermagnetism, a new collinear magnetic state, has gained significant attention in the last few years, and the underlying mechanisms driving this quantum phase are still evolving. Going beyond the group theoretical analyses, which focus on providing a binary description of the presence or absence of the altermagnetic state, in this work, we explore the role of crystal chemical bonding. As the latter successfully integrates the crystal and orbital symmetries and is tunable, it provides a quantitative and realistic mechanism to explain the formation of altermagnetism. From the first principles calculations and tight-binding models within the framework of the linear combination of atomic orbitals on NiS, we establish a set of selection rules for the formation of altermagnetism in the NiAs prototype compounds (e.g. CrSb, MnTe, etc.). Broadly, if single orbitals from Ni and S sites are involved in the bonding, the second neighbor interaction between the nonmagnetic atoms is a must to modulate the intra-sublattice interactions differently for the opposite spin sublattices so that the antiferromagnetic sublattice band degeneracy is lifted and momentum-dependent altermagnetic spin split (AMSS) appears. However, when multiple orbitals are involved from the Ni and S sites in the chemical bonding, altermagnetism is naturally present. Together, they amplify the AMSS. Further, we propose twelve antinodal regions in the NiAs type hexagonal crystals, where AMSS split is maximum. Specific to NiS, AMSS increases with correlation, and for the edge valence and conduction bands, it can go beyond 1eV. The present study opens up new pathways to design chemical bonding driven selection rules in addition to the existing crystal symmetry criteria to tailor tunable altermagnetism. △ Less

Submitted 27 June, 2025; v1 submitted 31 December, 2024; originally announced January 2025.

Comments: 15 pages, 15 figures, and 6 tables

Tuning the band topology and topological Hall effect in skyrmion crystals via the spin-orbit coupling

Authors: Arijit Mandal, S. Satpathy, B. R. K. Nanda

Abstract: The topological Hall effect is the result of spin-asymmetric deflection of charge carriers flowing through a non-collinear spin system. Effective manipulation of the topological Hall conductivity (THC) in skyrmions is currently a vigorous area of research with an eye towards potential spintronics application. Here, we show that the band topology and the THC in a skyrmion crystal can be tuned by ch… ▽ More The topological Hall effect is the result of spin-asymmetric deflection of charge carriers flowing through a non-collinear spin system. Effective manipulation of the topological Hall conductivity (THC) in skyrmions is currently a vigorous area of research with an eye towards potential spintronics application. Here, we show that the band topology and the THC in a skyrmion crystal can be tuned by changing the strength of the Rashba spin-orbit coupling (SOC), which can be accomplished via a perpendicular electric field. This results in the change of the subband Chern numbers and a transition between ordinary insulator and Chern insulator as the Rashba SOC is varied. For partially filled subbands, the Rashba SOC can tune the THC and reverse its sign, so that the direction of the Hall current is flipped. The critical Rashba strength for this depends on the skyrmion type and the carrier density. We extend our analysis to the cases of Dresselhaus and Weyl SOC as well, and show that they can be directly mapped to the Rashba SOC case and therefore lead to similar results. Our work opens up the scope to go beyond the existing avenues for the control of charge transport in skyrmion crystals. △ Less

Submitted 10 August, 2025; v1 submitted 10 November, 2024; originally announced November 2024.

Comments: 20 pages, 15 figures, 1 table

Simulating anharmonic vibrational polaritons beyond the long wavelength approximation

Authors: Dipti Jasrasaria, Arkajit Mandal, David R. Reichman, Timothy C. Berkelbach

Abstract: In this work we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical fram… ▽ More In this work we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity. Numerical simulations in model systems demonstrate the accuracy and applicability of our approach. △ Less

Submitted 12 September, 2024; originally announced September 2024.

Comments: 10 pages, 6 figures

Direct Electrical Detection of Spin Chemical Potential Due to Spin Hall Effect in $β$-Tungsten and Platinum Using a Pair of Ferromagnetic and Normal Metal Voltage probes

Authors: Soumik Aon, Abu Bakkar Miah, Arpita Mandal, Harekrishna Bhunia, Dhananjaya Mahapatra, Partha Mitra

Abstract: The phenomenon of Spin Hall Effect (SHE) generates a pure spin current transverse to an applied current in materials with strong spin-orbit coupling, although not detectable through conventional electrical measurement. An intuitive Hall effect like measurement configuration is implemented to directly measure pure spin chemical potential of the accumulated spins at the edges of heavy metal (HM) cha… ▽ More The phenomenon of Spin Hall Effect (SHE) generates a pure spin current transverse to an applied current in materials with strong spin-orbit coupling, although not detectable through conventional electrical measurement. An intuitive Hall effect like measurement configuration is implemented to directly measure pure spin chemical potential of the accumulated spins at the edges of heavy metal (HM) channels that generates large SHE. A pair of transverse linearly aligned voltage probes in placed in ohmic contact with the top surface of HM , one being a ferromagnetic metal (FM) with non-zero spin polarization and other is the reference metal (RM) with zero polarization of carriers. This combination of FM/RM electrodes is shown to induce an additional voltage proportional to a spin accumulation potential, which is anti symmetric with respect to opposite orientations of FM controlled by a 2D vector magnet. Proof of concept of the measurement scheme is verified by comparing the signs of voltages for HM channels of Tungsten (W) and Platinum (Pt) which are known to generate opposite spin accumulation under similar conditions of applied current. The same devices are also able to detect the reciprocal effect, inverse spin Hall effect (ISHE) by swapping the current and voltage leads and the results are consistent with reciprocity principle. Further, exploiting a characteristic feature of W thin film deposition, a series of devices were fabricated with W resistivity varying over a wide range of 10 - 750 $μΩ$-cm and the calculated spin Hall resistivity exhibits a pronounced power law dependence on resistivity. Our measurement scheme combined with almost two decades of HM resistivity variation provides the ideal platform required to test the underlying microscopic mechanism responsible for SHE/ISHE. △ Less

Submitted 5 April, 2024; originally announced April 2024.

Investigating the Collective Nature of Cavity Modified Chemical Kinetics under Vibrational Strong Coupling

Authors: Lachlan P. Lindoy, Arkajit Mandal, David R. Reichman

Abstract: In this paper we develop quantum dynamical methods capable of treating the dynamics of chemically reacting systems in an optical cavity in the vibrationally strong-coupling (VSC) limit at finite temperatures and in the presence of a dissipative solvent in both the few and many molecule limits. In the context of two simple models we demonstrate how reactivity in the {\em collective} VSC regime does… ▽ More In this paper we develop quantum dynamical methods capable of treating the dynamics of chemically reacting systems in an optical cavity in the vibrationally strong-coupling (VSC) limit at finite temperatures and in the presence of a dissipative solvent in both the few and many molecule limits. In the context of two simple models we demonstrate how reactivity in the {\em collective} VSC regime does not exhibit altered rate behavior in equilibrium, but may exhibit resonant cavity modification of reactivity when the system is explicitly out of equilibrium. Our results suggest experimental protocols that may be used to modify reactivity in the collective regime and point to features not included in the models studied which demand further scrutiny. △ Less

Submitted 6 March, 2024; originally announced March 2024.

Variational Lang-Firsov approach plus Møller-Plesset perturbation theory with applications to ab initio polariton chemistry

Authors: Zhi-Hao Cui, Arkajit Mandal, David R. Reichman

Abstract: We apply the Lang-Firsov (LF) transformation to electron-boson coupled Hamiltonians and variationally optimize the transformation parameters and molecular orbital coefficients to determine the ground state. Møller-Plesset (MP-$n$, with $n = 2$ and $4$) perturbation theory is then performed on top of the optimized LF mean-field state to improve the description of electron-electron and electron-boso… ▽ More We apply the Lang-Firsov (LF) transformation to electron-boson coupled Hamiltonians and variationally optimize the transformation parameters and molecular orbital coefficients to determine the ground state. Møller-Plesset (MP-$n$, with $n = 2$ and $4$) perturbation theory is then performed on top of the optimized LF mean-field state to improve the description of electron-electron and electron-boson correlations. The method (LF-MP) is applied to several electron-boson coupled systems, including the Hubbard-Holstein model, diatomic molecule dissociation ($\text{H}_2$, $\text{HF}$), and the modification of proton transfer reactions (malonaldehyde and aminopropenal) via the formation of polaritons in an optical cavity. We show that with a correction for the electron-electron correlation, the method gives quantitatively accurate energies comparable to exact diagonalization or coupled-cluster theory. The effect of multiple photon modes, spin polarization, and the comparison to the coherent state MP theory are also discussed. △ Less

Submitted 2 February, 2024; v1 submitted 19 October, 2023; originally announced October 2023.

Comments: 16 pages, 8 figures

Journal ref: J. Chem. Theory Comput. (2024)

Room temperature reversible colossal volto-magnetic effect in all-oxide metallicmagnet/topotactic-phase-transition material heterostructures

Authors: Sourav Chowdhury, Supriyo Majumder, Rajan Mishra, Arup Kumar Mandal, Anita Bagri, Satish Yadav, Suman Karmarkar, D. M. Phase, R. J. Choudhary

Abstract: Multiferroic materials have undergone extensive research in the past two decades in an effort to produce a sizable room-temperature magneto-electric (ME) effect in either exclusive or composite materials for use in a variety of electronic or spintronic devices. These studies have looked into the ME effect by switching the electric polarization by the magnetic field or switching the magnetism by th… ▽ More Multiferroic materials have undergone extensive research in the past two decades in an effort to produce a sizable room-temperature magneto-electric (ME) effect in either exclusive or composite materials for use in a variety of electronic or spintronic devices. These studies have looked into the ME effect by switching the electric polarization by the magnetic field or switching the magnetism by the electric field. Here, an innovative way is developed to knot the functional properties based on the tremendous modulation of electronics and magnetization by the electric field of the topotactic phase transitions (TPT) in heterostructures composed of metallic-magnet/TPT-material. It is divulged that application of a nominal potential difference of 2-3 Volts induces gigantic changes in magnetization by 100-250% leading to colossal Voltomagnetic effect, which would be tremendously beneficial for low-power consumption applications in spintronics. Switching electronics and magnetism by inducing TPT through applying an electric field requires much less energy, making such TPT-based systems promising for energy-efficient memory and logic applications as well as opening a plethora of tremendous opportunities for applications in different domains. △ Less

Submitted 8 August, 2023; originally announced August 2023.

Formation of spin-orbital entangled 2D electron gas in layer delta-doped bilayer iridate La$_δ$Sr$_3$Ir$_2$O$_7$

Authors: Amit Chauhan, Arijit Mandal, B. R. K. Nanda

Abstract: 5$d$ transition metal oxides host a variety of exotic phases due to the comparable strength of Coulomb repulsion and spin-orbit coupling. Herein, by pursuing density-functional studies on a delta-doped quasi-two-dimensional iridate Sr$_3$Ir$_2$O$_7$, where a single SrO layer is replaced by LaO layer, we predict the formation of a spin-orbital entangled two-dimensional electron gas (2DEG) which is… ▽ More 5$d$ transition metal oxides host a variety of exotic phases due to the comparable strength of Coulomb repulsion and spin-orbit coupling. Herein, by pursuing density-functional studies on a delta-doped quasi-two-dimensional iridate Sr$_3$Ir$_2$O$_7$, where a single SrO layer is replaced by LaO layer, we predict the formation of a spin-orbital entangled two-dimensional electron gas (2DEG) which is sharply confined on two IrO$_2$ layers close to the LaO layer. In this bilayer crystal structure, an existing potential well is further augmented with the inclusion of positively charged LaO layer which results in confining the extra valence electron made available by the La$^{3+}$ ion. The confined electron is bound along crystal $a$ direction and is highly mobile in the $bc$ plane. From the band structure point of view, now the existing half-filled $J_{eff}$ = 1/2 states are further electron doped to destroy the antiferromagnetic Mott insulating state of IrO$_2$ layers near to the delta-doped layer. This leads to partially occupied Ir upper-Hubbard subbands which host the spin-orbital entangled 2DEG. The IrO$_2$ layers far away from the interface remain insulating and preserve the collinear G-type magnetic ordering of pristine Sr$_3$Ir$_2$O$_7$. The conductivity tensors calculated using semi-classical Boltzmann theory at room temperature reveal that the 2DEG exhibits large electrical conductivity of the order of 10$^{19}$. △ Less

Submitted 14 November, 2023; v1 submitted 19 June, 2023; originally announced June 2023.

Impact of capping agent on structural and optical properties of ZnS nanoparticles

Authors: Samiran Mandal, Sk Irsad Ali, Subhamay Pramanik, Atis Chandra Mandal

Abstract: Nanocrystalline samples of pristine capped and uncapped zinc sulphide were synthesized via the sol-gel technique. The nanocrystallinity of the samples were confirmed by the X-ray diffraction technique, where size of the particle size decreases with the increasing of mol. concentration (x = 0.00, 0.02, 0.03, 0.04 Mol). of capping agent sodium dodecyle sulphate. The obtained crystallite sizes were f… ▽ More Nanocrystalline samples of pristine capped and uncapped zinc sulphide were synthesized via the sol-gel technique. The nanocrystallinity of the samples were confirmed by the X-ray diffraction technique, where size of the particle size decreases with the increasing of mol. concentration (x = 0.00, 0.02, 0.03, 0.04 Mol). of capping agent sodium dodecyle sulphate. The obtained crystallite sizes were found to be in the range 4.6 nm to 2.7 nm respectively. The optical band gaps of the samples were estimated by using ultra-violet visible spectroscopic techniques and the band gap values were in the range 3.8 eV to 4.4 eV. All the samples showed quantum confinement behavior compared to bulk sample. Fluorescence (FL) spectra showed three emission peaks at the emission wavelengths around 434 nm, 520 nm, 545 nm, 628 nm, and 694 nm. The FL intensities were proportional to the concentration of capping agent. △ Less

Submitted 26 April, 2023; originally announced April 2023.

Comments: 11 pages, 6 figures, conference

Microscopic Theory of Multimode Polariton Dispersion in Multilayered Materials

Authors: Arkajit Mandal, Ding Xu, Ankit Mahajan, Joonho Lee, Milan E. Delor, David R. Reichman

Abstract: We develop a microscopic theory for the multimode polariton dispersion in materials coupled to cavity radiation modes. Starting from a microscopic light-matter Hamiltonian, we devise a general strategy for obtaining simple matrix models of polariton dispersion curves based on the structure and spatial location of multi-layered 2D materials inside the optical cavity. Our theory exposes the connecti… ▽ More We develop a microscopic theory for the multimode polariton dispersion in materials coupled to cavity radiation modes. Starting from a microscopic light-matter Hamiltonian, we devise a general strategy for obtaining simple matrix models of polariton dispersion curves based on the structure and spatial location of multi-layered 2D materials inside the optical cavity. Our theory exposes the connections between seemingly distinct models that have been employed in the literature and resolves an ambiguity that has arisen concerning the experimental description of the polaritonic band structure. We demonstrate the applicability of our theoretical formalism by fabricating various geometries of multi-layered perovskite materials coupled to cavities and demonstrating that our theoretical predictions agree with the experimental results presented here. △ Less

Submitted 19 March, 2023; originally announced March 2023.

Room-temperature multiferroicity in GaFeO$_3$ thin film grown on (100)Si substrate

Authors: Sudipta Goswami, Shubhankar Mishra, Kausik Dana, Ashok Kumar Mandal, Nitai Dey, Prabir Pal, Biswarup Satpati, Mrinmay Mukhopadhyay, Chandan Kumar Ghosh, Dipten Bhattacharya

Abstract: Room-temperature magnetoelectric multiferroicity has been observed in c-axis oriented GaFeO$_3$ thin films (space group $Pna2_1$), grown on economic and technologically important (100)Si substrates by pulsed laser deposition technique. Structural analysis and comprehensive mapping of Ga:Fe ratio across a length scale range of 10$^4$ reveal coexistence of epitaxial and chemical strain. It induces f… ▽ More Room-temperature magnetoelectric multiferroicity has been observed in c-axis oriented GaFeO$_3$ thin films (space group $Pna2_1$), grown on economic and technologically important (100)Si substrates by pulsed laser deposition technique. Structural analysis and comprehensive mapping of Ga:Fe ratio across a length scale range of 10$^4$ reveal coexistence of epitaxial and chemical strain. It induces formation of finer magnetic domains and large magnetoelectric coupling - decrease in remanent polarization by $\sim$21\% under $\sim$50 kOe. Magnetic force microscopy reveals presence of both finer ($<$100 nm) and coarser ($\sim$2 $μ$m) magnetic domains. Strong multiferroicity in epitaxial GaFeO$_3$ thin films, grown on (100)Si substrate, brighten the prospect of their integration with Si-based electronics and could pave the way for development of economic and more efficient electromechanical, electrooptic or magnetoelectric sensor devices. △ Less

Submitted 20 November, 2022; originally announced November 2022.

Comments: 8 pages, 9 figures, accepted for publication in J. Appl. Phys

Journal ref: J. Appl. Phys. 132, 214101 (2022)

Quantum Dynamics of Vibrational Polariton Chemistry

Authors: Lachlan P. Lindoy, Arkajit Mandal, David R. Reichman

Abstract: We employ an exact quantum mechanical simulation technique to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling to either the reaction coordinate or a non-reactive mode, and the coupling of the cavity to lossy modes. Thus, many of the most important features needed for r… ▽ More We employ an exact quantum mechanical simulation technique to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling to either the reaction coordinate or a non-reactive mode, and the coupling of the cavity to lossy modes. Thus, many of the most important features needed for realistic modeling of the cavity modification of chemical reactions are included. We find that when a molecule is coupled to an optical cavity it is essential to treat the problem quantum mechanically in order to obtain a quantitative account of alterations to reactivity. We find sizable and sharp changes in the rate constant that are associated with quantum mechanical state splittings and resonances. The features that emerge from our simulations are closer to those observed in experiments than are previous calculations, even for realistically small values of coupling and cavity loss. This work highlights the importance of a fully quantum treatment of vibrational polariton chemistry. △ Less

Submitted 11 October, 2022; originally announced October 2022.

Carrier thermalization and zero-point bandgap renormalization in halide perovskites from the Urbach tails of the emission spectrum

Authors: Kingshuk Mukhuti, Arnab Mandal, Basabendra Roy, Sayan Bhattacharyya, Bhavtosh Bansal

Abstract: We develop techniques to study the temperature dependent localization, thermalization, and the effects of phonon scattering on the excitons in halide perovskites from the analysis of the emission spectra. The excitonic Urbach edge, when inferred from the low energy tails of the temperature dependent luminescence spectra, is shown to be sensitive to the electron distribution and thermalization. A m… ▽ More We develop techniques to study the temperature dependent localization, thermalization, and the effects of phonon scattering on the excitons in halide perovskites from the analysis of the emission spectra. The excitonic Urbach edge, when inferred from the low energy tails of the temperature dependent luminescence spectra, is shown to be sensitive to the electron distribution and thermalization. A method to observe the Urbach focus is devised for halide perovskites where the temperature dependence of the excitonic gap is anomalous. The value of the zero-point bandgap renormalization is inferred to be about 33 meV. This small value of the bandgap renormalization rules out the formation of small polarons and points to weak electron-phonon coupling. The experiments are performed on the nanosheets of the archetypal halide perovskite, CsPbBr$_3$. △ Less

Submitted 10 October, 2022; originally announced October 2022.

MsSpec-DFM (Dielectric function module): Towards a multiple scattering approach to plasmon description

Authors: Aditi Mandal, Sylvain Tricot, Rakesh Choubisa, Didier Sebilleau

Abstract: We present here the MsSpec Dielectric Function module (MsSpec-DFM), which generates dielectric functions in an electron gas or a liquid, either isolated or embedded into an environment. In addition to standard models such as the plasmon pole and the RPA, this module also provides more involved methods incorporating local field corrections (in order to account for correlations), Boltzmann-Vlasov hy… ▽ More We present here the MsSpec Dielectric Function module (MsSpec-DFM), which generates dielectric functions in an electron gas or a liquid, either isolated or embedded into an environment. In addition to standard models such as the plasmon pole and the RPA, this module also provides more involved methods incorporating local field corrections (in order to account for correlations), Boltzmann-Vlasov hydrodynamical methods, the relaxation-damped Mermin and the diffusion-damped Hu-O'Connell methods, as well as moment-based methods using either a Nevanlinna function or a memory function. Ultimately, through the use of form factors, the MsSpec-DFM module will be able to address a wide range of materials such as metals, semiconductors, including inversion layers, hetero-structures, superconductors, quantum wells, quantum wires, quantum dots, Dirac materials such as graphene, and liquids. △ Less

Submitted 20 July, 2022; originally announced July 2022.

Photosensitive SrMnO3

Authors: Arup Kumar Mandal, Aprajita Joshi, Surajit Saha, Binoy Krishna De, Sourav Chowdhury, VG Sathe, U. Deshpande, D. Shukla, Amandeep Kaur, D. M. Phase, R. J. Choudhary

Abstract: In recent years, photosensitive materials have been in huge demand because of their fascinating ability to convert absorbed photon energy to generate strain and henceforth tuning the physical properties. In this report we detect the photosensitive activity of SrMnO3. Using the power dependent and temperature dependent Raman study with different laser sources having wavelengths across the optical b… ▽ More In recent years, photosensitive materials have been in huge demand because of their fascinating ability to convert absorbed photon energy to generate strain and henceforth tuning the physical properties. In this report we detect the photosensitive activity of SrMnO3. Using the power dependent and temperature dependent Raman study with different laser sources having wavelengths across the optical band gap of SrMnO3, we divulge the photosensitive character of SrMnO3 thin films. Upon laser light illumination, Raman modes soften and softening further increases with increase in laser power. Similar kind of mode variation is observed with increasing temperature at fixed laser power. XAS in presence of laser illumination, reveals the change in crystal field splitting associated with mode softening. △ Less

Submitted 18 May, 2022; originally announced May 2022.

Comments: 28,13

Resonant Cavity Modification of Ground State Chemical Kinetics

Authors: Lachlan P. Lindoy, Arkajit Mandal, David R. Reichman

Abstract: Recent experiments have suggested that ground state chemical kinetics can be suppressed or enhanced by coupling the vibrational degrees of freedom of a molecular system with a radiation mode inside an optical cavity. Experiments show that the chemical rate is strongly modified when the photon frequency is close to characteristic vibrational frequencies. The origin of this remarkable effect remains… ▽ More Recent experiments have suggested that ground state chemical kinetics can be suppressed or enhanced by coupling the vibrational degrees of freedom of a molecular system with a radiation mode inside an optical cavity. Experiments show that the chemical rate is strongly modified when the photon frequency is close to characteristic vibrational frequencies. The origin of this remarkable effect remains unknown. In this work, we develop an analytical rate theory for cavity-modified ground state chemical kinetics based on the Pollak-Grabert-Hänggi rate theory. Unlike previous work, our theory covers the complete range of solvent friction values, from the energy-diffusion limited to the spatial-diffusion limited regimes. We show that the chemical reaction rate can either be enhanced or suppressed depending on the bath friction; when bath friction is weak chemical kinetics is enhanced as opposed to the case of strong bath friction, where chemical kinetics is suppressed. Further, we show that the photon frequency at which maximum modification of chemical rate is achieved is close to the reactant well, and hence resonant rate modification occurs. In the strong friction limit the {\it resonant} photon frequency is instead close to the barrier frequency, as obtained using the Grote-Hynes rate theory. Finally, we observe that the rate changes (as a function of photon frequency) are much sharper and more sizable in the weak friction limit than in the strong friction limit, and become increasingly sharp with decreasing well frequency. △ Less

Submitted 10 May, 2022; originally announced May 2022.

Structural and electronic phase transitions in Zr$_{1.03}$Se$_{2}$ at high pressure

Authors: Bishnupada Ghosh, Mrinmay Sahu, Debabrata Samanta, Pinku Saha, Anshuman Mandal, Goutam Dev Mukherjee

Abstract: A detailed high pressure investigation is carried out using x-ray diffraction, Raman spectroscopy and low temperature resistivity measurements on hexagonal ZrSe$_{2}$ having an excess of 3 at.\% Zr. Structural studies show that the sample goes through a gradual structural transition from hexagonal to monoclinic phase, with a mixed phase in the pressure range 5.9 GPa to 14.8 GPa. Presence of a mini… ▽ More A detailed high pressure investigation is carried out using x-ray diffraction, Raman spectroscopy and low temperature resistivity measurements on hexagonal ZrSe$_{2}$ having an excess of 3 at.\% Zr. Structural studies show that the sample goes through a gradual structural transition from hexagonal to monoclinic phase, with a mixed phase in the pressure range 5.9 GPa to 14.8 GPa. Presence of a minimum in the $c/a$ ratio in the hexagonal phase and a minimum in the full width half maximum of the $A_{1g}$ mode at about the same pressure indicates an electronic phase transition. The sample shows a metallic characteristic in its low temperature resistivity data at ambient pressure, which persist till about 5.1 GPa and can be related the presence of slight excess Zr. At and above 7.3 GPa, the sample shows a metal to semiconductor transition with the opening of a very small band gap, which increases with pressure. The low temperature resistivity data show an upturn, which flattens with an increase in pressure. The phenomenological analysis of the low temperature resistivity data indicates the presence of Kondo effect in the sample, which may be due to the excess Zr. △ Less

Submitted 3 May, 2022; originally announced May 2022.

Ultrafast imaging of polariton propagation and interactions

Authors: Ding Xu, Arkajit Mandal, James M. Baxter, Shan-Wen Cheng, Inki Lee, Haowen Su, Song Liu, David R. Reichman, Milan Delor

Abstract: Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach tha… ▽ More Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP-phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP-phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions. △ Less

Submitted 15 June, 2023; v1 submitted 2 May, 2022; originally announced May 2022.

Model dielectric functions for fluctuation potential calculations in electron gas: a critical assessment

Authors: Aditi Mandal, Sylvain Tricot, Rakesh Choubisa, Didier Sébilleau

Abstract: In this article, we report a critical assessment of dielectric function calculations in electron gas through the comparison of different modelling methods. This work is motivated by the fact that the dielectric function is a key quantity in the multiple scattering description of plasmon features in various electron-based spectroscopies. Starting from the standard random phase approximation (RPA) e… ▽ More In this article, we report a critical assessment of dielectric function calculations in electron gas through the comparison of different modelling methods. This work is motivated by the fact that the dielectric function is a key quantity in the multiple scattering description of plasmon features in various electron-based spectroscopies. Starting from the standard random phase approximation (RPA) expression, we move on to correlation-augmented RPA, then damped RPA models. Finally, we study the reconstruction of the dielectric function from its moments, using the Nevanlinna and memory function approaches. We find the memory function method to be the most effective, being highly flexible and customizable. △ Less

Submitted 24 January, 2022; originally announced January 2022.

Comments: 14 pages, 9 figures

Theory of Vibrational Polariton Chemistry in the Collective Coupling Regime

Authors: Arkajit Mandal, Xinyang Li, Pengfei Huo

Abstract: We theoretically demonstrate that chemical reaction rate constant can be significantly suppressed by coupling molecular vibrations with an optical cavity, exhibiting both the collective coupling effect and the cavity-frequency modification of the rate constant. When a reaction coordinate is strongly coupled to the solvent molecules, the reaction rate constant is reduced due to the dynamical caging… ▽ More We theoretically demonstrate that chemical reaction rate constant can be significantly suppressed by coupling molecular vibrations with an optical cavity, exhibiting both the collective coupling effect and the cavity-frequency modification of the rate constant. When a reaction coordinate is strongly coupled to the solvent molecules, the reaction rate constant is reduced due to the dynamical caging effect. We demonstrate that collectively coupling the solvent to the cavity can further enhance this dynamical caging effect, leading to additional suppression of the chemical kinetics. This effect is further amplified when cavity loss is considered. △ Less

Submitted 8 July, 2021; originally announced July 2021.

Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in LaNi_{x}V_{1-x}O_{3} thin films

Authors: Anupam Jana, Sophia Sahoo, Sourav Chowdhury, Arup Kumar Mandal, R. J. Choudhary, D. M. Phase, A. K. Raychaudhuri

Abstract: The room temperature (300 K) electronic structure of pulsed laser deposited LaNi_{x}V_{1-x}O_{3} thin films have been demonstrated. The substitution of early-transition metal (TM) V in LaVO_{3} thin films with late-TM Ni leads to the decreasing in out-of-plane lattice parameter. Doping of Ni does not alter the formal valence state of Ni and V in LaNi_{x}V_{1-x}O_{3} thin films, divulging the absen… ▽ More The room temperature (300 K) electronic structure of pulsed laser deposited LaNi_{x}V_{1-x}O_{3} thin films have been demonstrated. The substitution of early-transition metal (TM) V in LaVO_{3} thin films with late-TM Ni leads to the decreasing in out-of-plane lattice parameter. Doping of Ni does not alter the formal valence state of Ni and V in LaNi_{x}V_{1-x}O_{3} thin films, divulging the absence of carrier doping into the system. The valence band spectrum is observed to comprise of incoherent structure owing to the localized V 3d band along with the coherent structure at Fermi level. With increase in Ni concentration, the weight of the coherent feature increases, which divulges its origin to the Ni 3d-O 2p hybridized band. The shift of Ni 3d-O 2p hybridized band towards higher energy in Ni doped LaVO_{3} films compared to the LaNiO_{3} film endorses the modification in ligand to metal charge transfer (CT) energy. The Ni doping in Mott-Hubbard insulator LaVO_{3} leads to the closure of Mott-Hubbard gap by building of spectral weight that provides the delocalized electrons for conduction. A transition from bandwidth control Mott-Hubbard insulator LaVO_{3} to negative CT metallicity character in LaNiO_{3} film is observed. The study reveals that unlike in Mott-Hubbard insulators where the strong Coulomb interaction between the 3d electrons decides the electronic structure of the system, CT energy can deliver an additional degree of freedom to optimize material properties in Ni doped LaVO_{3} films. △ Less

Submitted 11 June, 2021; originally announced June 2021.

Comments: 30 pages, 8 figures

Nonlinear optical responses of all-inorganic lead halide perovskite nanostructures by time-resolved beam-deflection technique

Authors: Samrat Roy, Arnab Mandal, Akshay Raj R., Sayan Bhattacharyya, Bipul Pal

Abstract: We have investigated nonlinear refraction in all-inorganic halide perovskites, the CsPbBr$_3$ and CsPbBr$_{1.5}$I$_{1.5}$ nanosheet and quantum dot colloids in toluene, by a novel beam deflection technique using near-resonant continuous wave lasers. The nonlinear refraction and its time-evolution measured here have originated from thermal lensing effect. Nonlinear behaviour of heat transport in te… ▽ More We have investigated nonlinear refraction in all-inorganic halide perovskites, the CsPbBr$_3$ and CsPbBr$_{1.5}$I$_{1.5}$ nanosheet and quantum dot colloids in toluene, by a novel beam deflection technique using near-resonant continuous wave lasers. The nonlinear refraction and its time-evolution measured here have originated from thermal lensing effect. Nonlinear behaviour of heat transport in terms of intensity dependent thermal diffusion rate has been observed. Effects of convective heat flow have been measured at high intensities. Quantum dots have higher nonlinear refraction as compared to the corresponding nanosheet samples, presumably due to reduced dimensionality. The effective values of nonlinear refractive index, estimated here for near-resonant excitations, exceed those reported in the literature for organic-inorganic hybrid perovskites in the nonresonant excitation regime, by several orders of magnitude. △ Less

Submitted 11 November, 2019; originally announced November 2019.

Comments: 08 pages, 08 figures, 02 tables

Quasi-Diabatic Scheme for Non-adiabatic On-the-fly Simulations

Authors: Wanghuai Zhou, Arkajit Mandal, Pengfei Huo

Abstract: This paper provides the first ab-initio on-the-fly example of using the Quasi-Diabatic (QD) scheme for non-adiabatic simulations with diabatic dynamics approaches. The QD scheme provides a seamless interface between diabatic quantum dynamics approaches and {\it adiabatic} electronic structure calculations. It completely avoids additional theoretical efforts to reformulate the equation of motion fr… ▽ More This paper provides the first ab-initio on-the-fly example of using the Quasi-Diabatic (QD) scheme for non-adiabatic simulations with diabatic dynamics approaches. The QD scheme provides a seamless interface between diabatic quantum dynamics approaches and {\it adiabatic} electronic structure calculations. It completely avoids additional theoretical efforts to reformulate the equation of motion from diabatic to adiabatic representation, or construct global diabatic surfaces. This scheme enables many recently developed diabatic quantum dynamics approaches for ab-inito on-the-fly simulations, providing the non-adiabatic community a wide variety of approaches (such as the real-time path integral method and symmetric quasi-classical approach) beyond the well-explored methods (like trajectory surface-hopping or ab-initio multiple-spawning). The QD scheme also enables using realistic test cases (like ethylene photodynamics) that go beyond simple model systems to assess the accuracy and limitation of recently developed quantum dynamics approaches. △ Less

Submitted 14 August, 2019; originally announced August 2019.

Tailoring the crack-tip microstructure: A novel approach

Authors: Khilesh Kumar Bhandari, Arka Mandal, Md. Basiruddin Sk, Arghya Deb, Debalay Chakrabarti

Abstract: This investigation demonstrates a way to innovatively modify the ferritic microstructure at a local scale, particularly at the failure prone area such as Charpy V-notch (CVN) root. Tensile pre-strain (PS) up to 6 percent and 12 percent were employed before annealing (An) the samples at 650°C for 15 minutes. Ferrite grain size increased sharply and gradually (along the distance ahead of the notch r… ▽ More This investigation demonstrates a way to innovatively modify the ferritic microstructure at a local scale, particularly at the failure prone area such as Charpy V-notch (CVN) root. Tensile pre-strain (PS) up to 6 percent and 12 percent were employed before annealing (An) the samples at 650°C for 15 minutes. Ferrite grain size increased sharply and gradually (along the distance ahead of the notch root) within the microstructurally modified region in 6-12 percent pre-strained and annealed samples, respectively. Critical strain which promotes strain induced boundary migration (SIBM), was found to be 0.1 which resulted in abnormally coarse ferrite grains. △ Less

Submitted 23 February, 2019; originally announced February 2019.

Comments: 13 pages, 4 figures

Effect of isothermal holding temperature on the precipitation hardening in Vanadium-microalloyed steels with varying carbon and nitrogen levels

Authors: Anish Karmakar, Abhisek Mandal, Subrata Mukherjee, Saurbh Kundu, Dinesh Srivastava, Rahul Mitra, Debalay Chakrabarti

Abstract: Combined effect of Carbon and Nitrogen levels and isothermal holding temperature on the microstructure, precipitation and the tensile properties of Vanadium microalloyed steels with 0.05 weight percent Vanadium were studied. Two different Vanadium steels, one having higher Carbon and lower Nitrogen content, HCLN steel, and the other having lower Carbon and higher Nitrogen content, LCHN steel, were… ▽ More Combined effect of Carbon and Nitrogen levels and isothermal holding temperature on the microstructure, precipitation and the tensile properties of Vanadium microalloyed steels with 0.05 weight percent Vanadium were studied. Two different Vanadium steels, one having higher Carbon and lower Nitrogen content, HCLN steel, and the other having lower Carbon and higher Nitrogen content, LCHN steel, were prepared and subjected to isothermal holding treatment over a temperature range of 500 to 750 degree Celsius, after hot-deformation. Maximum precipitation strengthening from fine Vanadium carbonitride precipitates has been found at intermediate isothermal holding temperatures i.e. 600 to 650 degree Celsius in both the steels. In spite of the significantly smaller fraction of pearlite and bainite, coarser average ferrite grain size and lower interaction of precipitation and dislocation in the ferrite matrix, the yield strength of LCHN steel was close to HCLN steel. This can be attributed to the higher precipitation strengthening ranging from 20 to 50 MPa resulted from the finer Vanadium precipitates in LCHN steel than that of HCLN steel. △ Less

Submitted 10 July, 2016; originally announced July 2016.

Comments: The combined manuscript contains total 26 pages. 13 figures are there including sub-figures

Topological delocalization and tuning of surface channel separation in Bi2Se2Te Topological Insulator Thin films

Authors: R. K. Gopal, Sourabh Singh, Arpita Mandal, Jit Sarkar, Chiranjib Mitra

Abstract: The surface states of a 3D topological insulator (TI) exhibit topological protection against backscattering. However, the contribution of bulk electrons to the transport data is an impediment to the topological protection of surface. We report the tuning of the chemical potential in the bulk of Bi2Se2Te TI thin films, pinning it near the center of the bulk band gap, thereby suppressing the bulk ca… ▽ More The surface states of a 3D topological insulator (TI) exhibit topological protection against backscattering. However, the contribution of bulk electrons to the transport data is an impediment to the topological protection of surface. We report the tuning of the chemical potential in the bulk of Bi2Se2Te TI thin films, pinning it near the center of the bulk band gap, thereby suppressing the bulk carriers. The temperature dependent resistance of these films shows activated behavior down to 50K, followed by a metallic transition at lower temperatures, a hallmark of the robustness of TI surface states. Manifestation of topological protection and surface dominated transport is explained by 2D weak antilocalization phenomenon. We further explore the effect of surface to bulk coupling in TI in this work, which is captured by the number of effective conducting surface channels that participate in the transport. The presence of a single conducting channel indicates a strong surface to bulk coupling which is detrimental to purely topological transport. We demonstrate the decoupling of topological surface states on opposite surfaces of thin films, thereby suppressing the bulk transport. Our findings provide a deeper understanding of surface to bulk coupling along with topological transport behavior and their respective tunability. △ Less

Submitted 1 December, 2016; v1 submitted 26 May, 2015; originally announced May 2015.

Comments: Revised Version, with further experimental data included

Magnetodielectric effect in nickel nanosheet-Na-4 mica composites

Authors: Sreemanta Mitra, Amrita Mandal, Anindya Datta, Sourish Banerjee, Dipankar Chakravorty

Abstract: Nickel nanosheets of thickness 0.6 nm were grown within the nanochannels of Na-4 mica template. The specimens show magnetodielectric effect at room temperature with a change of dielectric constant as a function of magnetic field, the electric field frequency varying from 100 to 700 kHz. A decrease of 5% in the value of dielectric constant was observed up to a field of 1.2 Tesla. This is explained… ▽ More Nickel nanosheets of thickness 0.6 nm were grown within the nanochannels of Na-4 mica template. The specimens show magnetodielectric effect at room temperature with a change of dielectric constant as a function of magnetic field, the electric field frequency varying from 100 to 700 kHz. A decrease of 5% in the value of dielectric constant was observed up to a field of 1.2 Tesla. This is explained by an inhomogeneous two-component composite model as theoretically proposed recently. The present approach will open up synthesis of various nanocomposites for sensor applications. △ Less

Submitted 7 May, 2012; originally announced May 2012.

Comments: 11 pages, 7 figures

Journal ref: EuroPhys. Lett. vol. 92, 26003, (2010)

Ferromagnetic behavior of ultrathin manganese nanosheets

Authors: Sreemanta Mitra, Amrita Mandal, Anindya Datta, Sourish Banerjee, Dipankar Chkaravorty

Abstract: Ferromagnetic behaviour has been observed experimentally for the first time in nanostructured Manganese. Ultrathin ($\sim$ 0.6 nm) Manganese nanosheets have been synthesized inside the two dimensional channels of sol-gel derived Na-4 mica. The magnetic properties of the confined system are measured within 2K-300K temperature range. The confined structure is found to show a ferromagnetic behaviour… ▽ More Ferromagnetic behaviour has been observed experimentally for the first time in nanostructured Manganese. Ultrathin ($\sim$ 0.6 nm) Manganese nanosheets have been synthesized inside the two dimensional channels of sol-gel derived Na-4 mica. The magnetic properties of the confined system are measured within 2K-300K temperature range. The confined structure is found to show a ferromagnetic behaviour with a nonzero coercivity value. The coercivity value remains positive throughout the entire temperature range of measurement. The experimental variation of susceptibility as a function of temperature has been satisfactorily explained on the basis of a two dimensional system with a Heisenberg Hamiltonian involving direct exchange interaction. △ Less

Submitted 7 May, 2012; originally announced May 2012.

Comments: 13 pages, 9 figures

Journal ref: J. Phys. Chem. C vol.115, No.30, pp 14673-14677, (2011)

Enhanced magnetic anisotropy of Nickel nanosheet prepared in Na-4 mica

Authors: Sreemanta Mitra, Amrita Mandal, Anindya Datta, Sourish Banerjee, Dipankar Chakravorty

Abstract: Nanosheets of nickel with thickness equal to 0.6 nm have been grown within the interlayer spaces of Na-4 mica. The sheets are made up of percolative clusters of nanodisks. Magnetization characteristics indicate a superparamagnetic behavior with a blocking temperature of 428 K.The magnetic anisotropy constant as extracted from the coercivity data has been found to be higher than that of bulk nickel… ▽ More Nanosheets of nickel with thickness equal to 0.6 nm have been grown within the interlayer spaces of Na-4 mica. The sheets are made up of percolative clusters of nanodisks. Magnetization characteristics indicate a superparamagnetic behavior with a blocking temperature of 428 K.The magnetic anisotropy constant as extracted from the coercivity data has been found to be higher than that of bulk nickel by two orders of magnitude. This is ascribed to a large aspect ratio of the nickel nanophase. The Bloch exponent is also found to be considerably different from that of bulk nickel because of a size effect. The Bloch Equation is still found to be valid for the two dimensional structures. △ Less

Submitted 2 May, 2012; originally announced May 2012.

Comments: 14 pages, 9 figures

Journal ref: Journal of Magnetism and Magnetic Materials 324 (2012) 2452-2457