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Subrata Jana

Publications and source records attributed to Subrata Jana.

At least 19 recordsLinked to original sources

Symmetry-Engineered Nonlinear Hall Response and Optical Response in Strained Monolayer Janus AsTeBr

The nonlinear Hall effect (NLHE) enables the generation of a transverse charge current in nonmagnetic materials with broken inversion symmetry while preserving time-reversal symmetry through the Berry curvature dipole (BCD). However, in crystals with $C_{3v}$ symmetry, the threefold rotational symmetry forces the BCD to vanish, thereby suppressing the intrinsic NLHE despite the presence of finite local Berry curvature. Here, using first-principles density functional theory combined with Wannier-based transport calculations, we demonstrate that uniaxial strain induces the NLHE in monolayer Janus AsTeBr by lowering the crystal symmetry from $C_{3v}$ to $C_{1}$ and generating a finite BCD. The resulting anisotropic redistribution of Berry-curvature hotspots produces pronounced nonlinear Hall conductivity and nonlinear Hall current, with the maximum response obtained at 2\% tensile strain. To elucidate the accompanying electronic-structure evolution, we further investigate the strain-dependent optical properties through the joint density of states, dielectric function, optical absorption, and reflectance. The optical spectra exhibit a systematic red shift and enhanced low-energy interband transitions, consistent with the strain-induced reconstruction of the electronic structure. Our results establish a microscopic connection between symmetry breaking, Berry-phase geometry, nonlinear Hall transport, and optical response, demonstrating that uniaxial strain provides an effective strategy for tailoring multiple functional properties in Janus two-dimensional materials.

cond-mat.mtrl-sci

A Unified Dielectric-Dependent Hybrid Functional for Accurate Band Gaps across Dimensions

Predicting fundamental band gaps across material classes and dimensionalities remains a central challenge in electronic-structure theory. Here, we show that intrinsic dielectric screening provides a unified control parameter for nonlocal exchange from bulk to low-dimensional and heterogeneous materials. We introduce a geometry-independent dielectric response and incorporate it self-consistently into a nonempirical screened-dielectric-dependent hybrid functional. Benchmarks for 100 materials spanning bulk, two-dimensional, one-dimensional, and mixed-dimensional systems show near-GW accuracy at the computational cost of generalized Kohn-Sham theory. These results reveal a screening-exchange-gap relation in which reduced dimensionality weakens intrinsic dielectric screening, strengthens nonlocal exchange, and drives the opening of fundamental gaps.

cond-mat.mtrl-sci

Nonlocal Orbital-Free Kinetic Energy Functional from the Jellium-with-Gap Model for Finite Systems

The quasi-linear scaling of orbital-free density functional theory (OF-DFT) with system size makes it a computationally efficient alternative to conventional Kohn--Sham density functional theory for many condensed-matter applications. However, its applicability remains limited, particularly for finite systems such as molecular clusters, due to the lack of accurate kinetic energy density functionals. In this context, the development of nonlocal kinetic energy density functionals (NL-KEDFs) has significantly advanced the practical utility of OF-DFT. Here, following an alternative formulation based on the linear-response kernel derived from the jellium-with-gap model (JGM), we develop an NL-KEDF capable of accurately describing the diverse density regimes characteristic of finite systems, including molecular clusters. Benchmark calculations, together with an analysis of the corresponding Pauli potentials, demonstrate that the proposed functional achieves higher accuracy than state-of-the-art orbital-free approaches for finite systems. Furthermore, the optical properties computed using the present method show good agreement with reference results, highlighting its reliability. These results indicate that the proposed NL-KEDF provides a robust and efficient framework for extending OF-DFT to finite systems, with potential implications for nanomaterial design and a deeper understanding of nanoscale phenomena.

cond-mat.mtrl-sci

Frontier Orbital Engineering in Heteroatom-Doped Prototypical Organic Dyes for Dye-Sensitized Solar Cells

The computational design of heteroatom-doped organic dyes for dye-sensitized solar cells (DSSCs) remains challenging, as predictive methods must accurately describe long-range charge-transfer (CT) excitations while remaining computationally efficient for systematic materials screening. In this work, we investigate the electronic structure and excited-state properties using the range-separated hybrid functional LC-$ω$PBE in conjunction with linear-response time-dependent density functional theory (TDDFT) within the Tamm-Dancoff approximation (TDA). We employ a simplified, physically motivated, effective tuning protocol ($ω_{eff}$) to enable the rapid and reliable screening of electronic properties of organic dyes. Charge-transfer excitation energies and frontier orbital alignment the key factors governing light absorption and electron injection in DSSCs are analyzed through targeted heteroatom (N, O, and B) incorporation into donor-$π$-acceptor (D-$π$-A) organic dyes. A library of 27 mono-, di-, and tri-doped prototypical organic dyes is designed based on a carbazole donor and a cyanoacrylic acid acceptor through targeted doping at three positions of the $π$-bridge or linker. Distinct design trends emerge: electron-rich nitrogen and oxygen dopants increase the HOMO-LUMO gap and blue-shift CT excitations, with nitrogen exhibiting the strongest effect, whereas electron-deficient boron substitution narrows the gap and induces pronounced red shifts. Notably, the BBN-doped dye exhibits the smallest gap and lowest excitation energy, highlighting boron-rich motifs as promising candidates for enhanced solar light harvesting. Overall, this study establishes transferable heteroatom-doping guidelines and introduces an efficient, reliable, and cost-effective tuned DFT-TDDFT framework for high-throughput computational discovery and optimization of DSSC sensitizers.

physics.chem-ph

Accurate starting points for one-shot $G_0W_0$ and Bethe-Salpeter Equation calculations via effective tuning of range-separated hybrid functionals

The accuracy of one-shot $G_0W_0$ and Bethe-Salpeter equation (BSE) calculations depends strongly on the underlying starting-point eigensystem, which is commonly obtained from a mean-field density-functional approximation. Range-separated hybrid (RSH) functionals provide a particularly effective starting point, however, conventional optimally tuned RSH procedures often require costly, system-specific, multi-step optimizations of the range-separation parameter $ω$. In this work, we show that a recently proposed effective tuning protocol [Singh \textit{et. al.}, Journal of Physical Chemistry Letters, 16, 32, 8198-8208, (2025)] for RSH functionals can serve as an efficient alternative for determining $ω$ used in $G_0W_0$ and BSE calculations. This simplified tuning scheme yields range-separation parameters that are effectively equivalent to those obtained from more elaborate tuning strategies, while avoiding their substantial computational overhead. The resulting tuned RSH eigensystems provide reliable starting points for many-body perturbation theory. In particular, one-shot $G_0W_0$ calculations based on effectively tuned RSH orbitals reproduce reference ionization potentials with high accuracy, while subsequent BSE calculations yield quantitatively reliable neutral excitation energies, optical absorption spectra, and excitonic properties for a diverse set of molecular systems and clusters. These results demonstrate that effective RSH tuning offers a practical and broadly applicable route to accurate quasiparticle and excited-state calculations, combining the accuracy of optimally tuned starting points with the low computational cost required for routine applications of $G_0W_0$ and BSE.

physics.chem-ph

Electric-Field and Doping-Induced Non collinear Magnetic Interactions in Monolayer Ti$_2$Si

Two-dimensional (2D) silicides are an emerging class of materials whose magnetic and relativistic properties remain largely unexplored. Using first-principles calculations, we investigate how electric-field modulation and transition-metal doping influence the magnetic exchange, magnetocrystalline anisotropy, and antisymmetric Dzyaloshinskii-Moriya interaction (DMI) in monolayer Ti2Si. Pristine Ti2Si is a dynamically stable ferromagnetic metal with in-plane anisotropy and centrosymmetric bonding, which suppresses DMI even under strong perpendicular electric fields. To overcome this symmetry constraint, we introduce Pt and Co substitution at Ti sites. Co enhances the magnetic exchange, whereas Pt provides strong spin orbit coupling (SOC), and the combined chemical asymmetry breaks inversion symmetry sufficiently to induce a sizable DMI. A Wannier-based tight-binding model captures the orbital-resolved superexchange pathways and reveals a clear hierarchy between a weak Si-mediated channel and a dominant Pt-mediated interlayer channel. First-principles calculations confirm that the Pt-assisted pathway governs the magnitude and sign of the total DMI. Among all configurations, Pt0.5CoTi0.5Si exhibits the strongest chiral interaction, with its intralayer and interlayer contributions favoring opposite rotation senses, namely counterclockwise (CCW) and clockwise (CW). Our results establish chemically engineered Ti2Si monolayers as a promising platform for realizing and tuning chiral magnetic textures in 2D silicides.

cond-mat.mtrl-sci

Simplified, Physically Motivated, and Broadly Applicable Range-Separation Tuning

Range-separated hybrid functionals (RSH) with ``ionization energy'' and/or ``optimal tuning'' of the screening parameter have proven to be among the most practical and accurate approaches for describing excited-state properties across a wide range of systems, including condensed matter. However, this method typically requires multiple self-consistent calculations and can become computationally expensive and unstable, particularly for extended systems. In this work, we propose a very simple and efficient alternative approach to determine the screening parameter for RSH based solely on the total electron density of the system and the compressibility sum rule of density functional theory (DFT). This effective screening parameter achieves remarkable accuracy, particularly for charge-transfer excitations, surpassing the performance of previously suggested alternatives. Because it relies only on the electron density, the proposed approach is physically transparent and highly practical to automate DFT calculations in large and complex systems, including bulk solids, where ``tuning'' is not possible.

physics.chem-ph

Advancing excited-state properties of two-dimensional materials using a dielectric-dependent hybrid functional

Predicting accurate band gaps and optical properties of lower-dimensional materials, including two-dimensional van der Waals (vdW) materials and their heterostructures, remains a challenge within density functional theory (DFT) due to their unique screening compared to their bulk counterparts. Additionally, accurate treatment of the dielectric response is crucial for developing and applying screened-exchange dielectric-dependent range-separated hybrid functionals (SE-DD-RSH) for vdW materials. In this work, we introduce a SE-DD-RSH functional to the 2D vdW materials like MoS2, WS2, hBN, black phosphorus (BP), and \b{eta}-InSe. By accounting for in-plane and out-of-plane dielectric responses, our method achieves accuracy comparable to advanced many-body techniques like G0 W0 and BSE@G0 W0 at a lower computational cost. We demonstrate improved band gap predictions and optical absorption spectra for both bulk and layered structures, including some heterostructures like MoS2/WS2 . This approach offers a practical and precise tool for exploring electronic and optical phenomena in 2D materials, paving the way for efficient computational studies of layered systems.

cond-mat.mtrl-sci

Anomalous Power Factor Enhancement and Local Structural Transition in Ni-Doped TiCoSb

We report a significant enhancement (~269%) in the power factor (PF) and a local structural transition in Ni-doped TiCoSb samples (TiCo_{1-x}Ni_xSb, (x= 0.0, 0.01, 0.02, 0.03, 0.04, and 0.06). First-principles calculations reveal that even minute Ni doping induces a substantial shift in the Fermi level (EF) and alters the density of states (DOS). Structural analysis via Rietveld refinement of X-ray diffraction (XRD) data shows anomalous behavior at x = 0.02, supported by Williamson-Hall and modified methods. X-ray absorption spectroscopy (XAS) at the Ti and Co K-edges further confirms a pronounced local structural change at this composition. These structural transitions are consistent with temperature-dependent resistivity (ρ(T)) and thermopower (S(T)) data, which reflect changes in EF and disorder. Analysis of Lorentz number and scattering parameters reinforces the observed modifications in the electronic structure. The simultaneous enhancement of S and electrical conductivity at x = 0.02 is attributed to the disorder-to-order transition, leading to the marked rise in PF.

cond-mat.mtrl-sci

Meta-GGA dielectric-dependent and range-separated screened hybrid functional for reliable prediction of material properties

We propose a range-separated hybrid exchange-correlation functional to calculate solid-state material properties. The functional mixes Hartree-Fock exchange with the semilocal exchange of the meta-generalized gradient approximation (meta-GGA) and the fraction of Hartree-Fock exchange is determined from the dielectric function. First-principles calculations and comparison with other meta-GGA approximations show that the functional leads to reasonably good performance for the band gap and optical properties. We also show that the present functional also successfully resolves the well-known ``band gap problem'' of narrow gap Cu-based semiconductors, such as Cu3SbSe4 and Cu3AsSe4, where, in general, a considerably large band inversion energy leads to a ``false'' negative or metallic band gap for all other methods. Furthermore, reasonable accuracy for the occupied d-bands and transition energies is also obtained for bulk solids. Thus, overall, our results demonstrate the predictive power of range-separated meta-GGA hybrid functionals for quantum materials simulations.

cond-mat.mtrl-sci

Accurate and efficient prediction of the band gaps and optical spectra of chalcopyrite semiconductors from a non-empirical range-separated dielectric-dependent hybrid: Comparison with many-body perturbation theory

The accurate prediction of electronic and optical properties in chalcopyrite semiconductors has been a persistent challenge for density functional theory (DFT) based approaches. Addressing this issue, we demonstrate that very accurate results can be obtained using a non-empirical screened dielectric-dependent hybrid (DDH) functional. This novel approach showcases its impressive capability to accurately determine band gaps, optical bowing parameters, and optical absorption spectra for chalcopyrite systems. What sets the screened DDH functional apart is its adeptness in capturing the many-body physics associated with highly localized $d$ electrons. Notably, the accuracy is comparable to the many-body perturbation based methods (such as $G_0W_0$ or its various approximations for band gaps and Bethe-Salpeter equation (BSE) on the top of the $G_0W_0$ or its various approximations for optical spectra) with less computational cost, ensuring a more accessible application across various research domains. The present results show the predictive power of the screened DDH functional, pointing toward promising applications where computational efficiency and predictive accuracy are crucial considerations. Overall, the screened DDH functional offers a compelling balance between cost-effectiveness and precision, making it a valuable tool for future endeavors in exploring chalcopyrite semiconductors and beyond.

cond-mat.mtrl-sci

Adiabatic connection interaction strength interpolation method made accurate for the uniform electron gas

The adiabatic connection interaction strength interpolation (ISI)-like method provides a high-level expression for the correlation energy, being in principle exact in the weak-interaction limit, where it recovers the second-order Görling-Levy perturbation term, but also in the strong-interaction limit that is described by the strictly correlated electron approach. In this work, we construct the genISI functional made accurate for the uniform electron gas, a solid-state physics paradigm that is a very difficult test for ISI-like correlation functionals. We assess the genISI functional for various jellium spheres with the number of electrons Z $\leq$ 912 and for the non-relativistic noble atoms with Z $\leq$ 290. For the jellium clusters, the genISI is remarkably accurate, while for the noble atoms, it shows a good performance, similar to other ISI-like methods. Then, the genISI functional can open the path using the ISI-like method in solid-state calculations.

physics.chem-ph

Semilocal Meta-GGA Exchange-Correlation Approximation From Adiabatic Connection Formalism: Extent and Limitations

The incorporation of a strong interaction regime within the approximate, semilocal exchange-correlation functionals still remains a very challenging task for density functional theory. One of the promising attempts in this direction is the recently proposed adiabatic connection semilocal correlation (ACSC) approach [Phys. Rev. B 2019, 99, 085117] allowing to construct the correlation energy functionals by interpolation of the high and low-density limits for the given semi-local approximation. The current study extends the ACSC method to the meta-GGA level of theory, providing some new insights. As an example, we construct the correlation energy functional base on the high and low-density limits of the Tao-Perdew-Starverov-Scuseria (TPSS) functional. Arose in this way TPSS-ACSC functional is one electron self-interaction free, accurate for the strictly correlated, and quasi-two-dimensional regimes. Based on simple examples, we show the advantages and disadvantages of ACSC semi-local functionals and provide some new guidelines for future developments in this context.

cond-mat.other

Simple and accurate screening parameters for dielectric-dependent hybrids

A simple effective screening parameter for screened range-separated hybrid is constructed from the compressibility sum rule in the context of linear-response time-dependent Density Functional Theory. When applied to the dielectric-dependent hybrid (DDH), it becomes remarkably accurate for bulk solids compared to those obtained from fitting with the model dielectric function or depending on the valence electron density of materials. The present construction of the screening parameter is simple and realistic. The screening parameter developed in this way is physically appealing and practically useful as it is straightforward to obtain using the average over the unit cell volume of the bulk solid, bypassing high-level calculations of the dielectric function depending on random-phase approximation. Furthermore, we have obtained a very good accuracy for energy band gaps, positions of the occupied d-bands, ionization potentials, optical properties of semiconductors and insulators, and geometries of bulk solids (equilibrium lattice constants and bulk moduli) from the constructed DDH.

cond-mat.mtrl-sci

Efficient and improved prediction of the band offsets at semiconductor heterojunctions from meta-GGA density functionals

Accurate theoretical prediction of the band offsets at interfaces of semiconductor heterostructures can often be quite challenging. Although density functional theory has been reasonably successful to carry out such calculations and efficient and accurate semilocal functionals are desirable to reduce the computational cost. In general, the semilocal functionals based on the generalized gradient approximation (GGA) significantly underestimate the bulk band gaps. This, in turn, results in inaccurate estimates of the band offsets at the heterointerfaces. In this paper, we investigate the performance of several advanced meta-GGA functionals in the computational prediction of band offsets at semiconductor heterojunctions. In particular, we investigate the performance of r2SCAN (revised strongly-constrained and appropriately-normed functional), rMGGAC (revised semilocal functional based on cuspless hydrogen model and Pauli kinetic energy density functional), mTASK (modified Aschebrock and Kümmel meta-GGA functional), and LMBJ (local modified Becke-Johnson) exchange-correlation functionals. Our results strongly suggest that these meta-GGA functionals for supercell calculations perform quite well, especially, when compared to computationally more demanding GW calculations. We also present band offsets calculated using ionization potentials and electron affinities, as well as band alignment via the branch point energies. Overall, our study shows that the aforementioned meta-GGA functionals can be used within the DFT framework to estimate the band offsets in semiconductor heterostructures with predictive accuracy.

cond-mat.mtrl-sci

Bandgap of two-dimensional materials: Thorough assessment of modern exchange-correlation functionals

The density functional theory (DFT) approximations that are the most accurate for the calculation of band gap of bulk materials are hybrid functionals like HSE06, the MBJ potential, and the GLLB-SC potential. More recently, generalized gradient approximations (GGA), like HLE16, or meta-GGAs, like (m)TASK, have proven to be also quite accurate for the band gap. Here, the focus is on 2D materials and the goal is to provide a broad overview of the performance of DFT functionals by considering a large test set of 298 2D systems. The present work is an extension of our recent studies [Rauch et al., Phys. Rev. B 101, 245163 (2020) and Patra et al., J. Phys. Chem. C 125, 11206 (2021)]. Due to the lack of experimental results for the band gap of 2D systems, $G_{0}W_{0}$ results were taken as reference. It is shown that the GLLB-SC potential and mTASK functional provide the band gaps that are the closest to $G_{0}W_{0}$. Following closely, the local MBJ potential has a pretty good accuracy that is similar to the accuracy of the more expensive hybrid functional HSE06.

cond-mat.mtrl-sci

Correct and accurate polymorphic energy ordering of transition-metal monoxides obtained from semilocal and onsite-hybrid exchange-correlation approximations

The relative energetic stability of the structural phases of common antiferromagnetic transition-metal oxides (MnO, FeO, CoO, and NiO) within the semilocal and hybrid density functionals are fraught with difficulties. In particular, MnO is known to be the most difficult case for almost all common semilocal and hybrid density approximations. Here, we show that the meta-generalized gradient approximation (meta-GGA) constructed from the cuspless hydrogen model and Pauli kinetic energy density (MGGAC) can lead to the correct ground state of MnO. The relative energy differences of zinc-blende (zb) and rock-salt (rs) structures as computed using MGGAC are found to be in nice agreement with those obtained from high-level correlation methods like the random phase approximation or quantum Monte Carlo techniques. Besides, we have also applied the onsite hybrid functionals (closely related to DFT+U ) based on GGA and meta-GGA functionals, and it is shown that a relatively high amount of Hartree-Fock exchange is necessary to obtain the correct ground-state structure. Our present investigation suggests that the semilocal MGGAC and onsite hybrids, both being computationally cheap, as methods of choice for the calculation of the relative stability of antiferromagnetic transition-metal oxides having potential applications in solid-state physics and structural chemistry.

cond-mat.mtrl-sci

Renormalization group analysis of weakly interacting van der Waals Fermi system

Weak-coupling phenomena of the two-dimensional Hubbard model is gaining momentum as a new interesting research field due to its extraordinarily rich behavior as a function of the carrier density and model parameters. Salmhofer [{\it Commun. Math. Phys}. \textbf{194}, 249 (1998);{\it Phys. Rev. Lett}. {\bf 87}, 187004 (2001)] developed a new renormalization-group method for interacting Fermi systems and Metzner [{\it Phys. Rev. B} {\bf 61}, 7364 (2000);{\it Phys. Rev. Lett}. {\bf 85}, 5162 (2000)] implemented this renormalization group analysis of the two-dimensional Hubbard model. In this work, we demonstrate the spin-wave dependent susceptibility behavior of model graphene-phosphorene van der Waals heterostructure in the framework of renormalization group approach. We implement signlet vertex response function for the weakly interacting van der Waals Fermi system with nearest-neighbor hopping amplitudes. This analytical approach is further correlated with {\it ab initio} simulation results and extended for spin-wave dependent susceptibility behavior with possible experimental protocols. We present the resulting compressibility and phase diagram in the vicinity of half-filling, and also results for the density dependence of the critical energy scale.

cond-mat.mes-hall