arXiv subjects

Ananth Govind Rajan

Publications and source records attributed to Ananth Govind Rajan.

9 recordsLinked to original sources

arXiv2026

MLIP Studio: An Open Platform for Interactive Benchmarking and Atomistic Simulations Using Machine Learning Interatomic Potentials

Universal machine learning interatomic potentials (MLIPs) are foundation AI models transforming atomistic simulations, but their practical use remains hindered by fragmented software ecosystems, dependency conflicts, and the lack of accessible benchmarking tools. These models approach first-principles density functional theory (DFT) accuracy at a fraction of the computational cost. We introduce MLIP Studio (available at https://mlipstudio.iisc.ac.in), an open and free platform that brings more than 60 universal MLIPs into a unified interactive interface for molecules and materials. The platform enables end-to-end MLIP-driven workflows, including property prediction, geometry optimization, vibrational and equation-of-state analysis, spin-state determination, custom model deployment, and high-throughput benchmarking against reference data. Automated parity plots and sortable error tables facilitate rapid identification of element-wise outliers and problematic data points. We demonstrate that MLIP-based pre-optimization can reduce subsequent DFT optimization effort by ~33$\times$. Additionally, the application enables benchmarking of computational performance. Through a comprehensive case study involving the 2D magnetic material CrCl$_3$ on a sapphire substrate, we show how cross-model comparisons of various properties and potential-energy landscapes can guide task-specific MLIP selection. Overall, MLIP Studio lowers the barrier to the reliable use of foundation models in end-to-end research workflows, benchmarking, and education in computational chemistry and materials science.

cond-mat.mtrl-sci↗

arXiv2026

Oxygen as a dual function regulator in MoS2 CVD synthesis: enhancing precursor evaporation while modulating reaction kinetics

Molybdenum disulfide (MoS2) is a promising 2D transition metal dichalcogenide (TMD) for optoelectronics and quantum technology applications, but faces challenges in scalable synthesis and defect engineering. Oxygen-assisted chemical vapor deposition (O-CVD), which introduces in-situ oxygen during growth, shows excellent potential in resolving both issues at once. Although co-flowing oxygen shows improvement in growth, the underlying mechanistic role of oxygen remains unclear. In this work, a combination of oxygen dosing experiments, density functional theory (DFT) calculations, computational fluid dynamics (CFD) simulations, and ab initio molecular dynamics (AIMD) simulations, uncover the dual role of oxygen in O-CVD. Firstly, AIMD reveals that oxygen increases MoO3 sublimation and enhances Mo3O9 supply. Concomitantly, DFT reveals that sulphur oxides, due to their bulkier nature than pure S2, limit the formation of reactive MoS6 intermediates. Subsequently, by experimentally varying the oxygen flow-interval, flow-rate, and flow-time, and correlating them with CFD simulations, we decouple oxygen's roles in source-poisoning prevention (i.e. MoO3 evaporation) and growth regulation. We find that maintaining a low sulphur-to-oxygen (S:O2) ratio at the MoO3 boat and substrate during nucleation, and a high S:O2 ratio at the substrate during growth is the key to obtaining large-area high-quality monolayer MoS2, confirmed by our optical measurements. Based on our understanding, we present a kinetic phase diagram for MoS2 synthesis, which will enable controlled oxygen dosing as a tuning parameter for scalable, defect-controlled monolayer MoS2 synthesis.

cond-mat.mtrl-sci↗

arXiv2026

Direct nanoscale mapping of band alignment in single-layer semiconducting lateral heterojunctions

Atomic-scale control over band alignment in single-layer lateral heterostructures (LHSs) of dissimilar transition metal dichalcogenides (TMDCs) is critical for nextgeneration electronic, optoelectronic, and quantum technologies. However, direct experimental access to interfacial electronic states with nanometer precision remains a significant challenge. Here, we employ angle-resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) to directly map the epitaxial alignment and valence band evolution across MoSe2-WSe2 LHSs. By combining nanoARPES with spatially resolved photoluminescence, we correlate the evolution of the valence band maximum and exciton features across both atomically sharp and compositionally graded diffusive interfaces. We identified type-II band alignments governed by both material composition and interstitial-induced modifications of band offsets, in close agreement with density functional theory calculations. These results reveal fundamental mechanisms of electronic structure modulation at 1D TMDC heterointerfaces and provide a robust platform for tailored band engineering in van der Waals materials.

cond-mat.mes-hall↗

arXiv2025

Tailored Vapor Deposition Unlocks Large-Grain, Wafer-Scale Epitaxial Growth of 2D Magnetic CrCl3

Two-dimensional magnetic materials (2D-MM) are an exciting playground for fundamental research, and for spintronics and quantum sensing. However, their large-grain large-area synthesis using scalable vapour deposition methods is still an unsolved challenge. Here, we develop a tailored approach for centimetre-scale growth of semiconducting 2D-MM CrCl3 films on mica substrate, via physical vapour transport deposition. A controlled synthesis protocol, enabled via innovations concerning light management, very-high carrier-gas flow, precursor flux, and oxygen/moisture removal, is critical for wafer-scale growth. Optical, stoichiometric, structural, and magnetic characterization identify crystalline, phase-pure 2D-MM CrCl3. Substrate temperature tunes thickness of films from few-layers to tens of nanometres. Further, selective-area growth and large-area transfer are demonstrated. Substrate-dependent growth features are explained by density functional theory and state-of-the-art machine learning interatomic potential-based atomic-scale simulations. This scalable vapour deposition approach can be applied for growth of several 2D-MM, and low growth temperature (~500 C) will enable creation of hybrid heterostructures.

cond-mat.mtrl-sci↗

arXiv2024

Resolving the Debate Between Boltzmann and Gibbs Entropy: Relative Energy Window Eliminates Thermodynamic Inconsistencies and Allows Negative Absolute Temperatures

Small systems consisting of a few particles are increasingly technologically relevant. In such systems, an intense debate in microcanonical statistical mechanics has been about the correctness of Boltzmann's surface entropy versus Gibbs' volume entropy. Both entropies have shortcomings -- while Boltzmann entropy predicts unphysical negative/infinite absolute temperatures for small systems with unbounded energy, Gibbs entropy entirely disallows negative absolute temperatures, in disagreement with experiments. We consider a relative energy window, motivated by the Heisenberg energy-time uncertainty principle and eigenstate thermalization in quantum mechanics. The proposed entropy ensures positive, finite temperatures for systems without a maximum limit on their energy and allows negative absolute temperatures in bounded energy systems, e.g., with population inversion. It also closely matches canonical ensemble predictions for prototypical systems, thus correctly describing the zero-point energy of an isolated quantum harmonic oscillator. Overall, we enable accurate thermodynamic models for isolated systems with few degrees of freedom.

cond-mat.stat-mech↗

arXiv2023

Incorporating Ion-Specific van der Waals and Soft Repulsive Interactions in the Poisson-Boltzmann Theory of Electrical Double Layers

Electrical double layers (EDLs) arise when an electrolyte is in contact with a charged surface, and are encountered in several application areas including batteries, supercapacitors, electrocatalytic reactors, and colloids. In the modeling of EDLs, a prominent knowledge gap has been the exclusion of van der Waals (vdW) and soft repulsive interactions in modified Poisson-Boltzmann (PB) theories. Although more short-ranged as compared to electrostatic interactions, we show here that vdW interactions can play an important role in determining the structure of the EDL via the formation of a Stern layer and in modulating the differential capacitance of an electrode in solution. To this end, we incorporate ion-ion and wall-ion vdW attraction and soft repulsion via a 12-6 Lennard-Jones (LJ) potential, resulting in a modified PB-LJ approach. The wall-ion LJ interactions were found to have a significant effect on the electrical potential and concentration profiles, especially close to the wall. However, ion-ion LJ interactions do not affect the EDL structure at low bulk ion concentrations (< 1 M). We also derive dimensionless numbers to quantify the impact of ion-ion and wall-ion LJ interactions on the EDL. Furthermore, in the pursuit of capturing ion-specific effects, we apply our model by considering various combinations of ions. We observe how varying parameters such as the electrolyte concentration and electrode potential affect the structure of the EDL due to the competition between ion-specific LJ and electrostatic interactions. Lastly, we show that the inclusion of vdW and soft repulsion interactions as well as hydration effects lead to a better qualitative agreement of the PB models with experimental double-layer differential capacitance data. Overall, the modified PB-LJ approach presented herein will lead to more accurate theoretical descriptions of EDLs in various application areas.

cond-mat.soft↗

arXiv2022

Enumerating Stable Nanopores in Graphene and their Geometrical Properties Using the Combinatorics of Hexagonal Lattices

Nanopores in two-dimensional (2D) materials, including graphene, can be used for a variety of applications, such as gas separations, water desalination, and DNA sequencing. So far, however, all plausible isomeric shapes of graphene nanopores have not been enumerated. Instead, a probabilistic approach has been followed to predict nanopore shapes in 2D materials, due to the exponential increase in the number of nanopores as the size of the vacancy increases. For example, there are 12 possible isomers when N=6 atoms are removed, a number that theoretically increases to 11.7 million when N=20 atoms are removed from the graphene lattice. The development of a smaller, exhaustive dataset of stable nanopore shapes can help future experimental and theoretical studies focused on using nanoporous 2D materials in various applications. In this work, we use the theory of 2D triangular "lattice animals" to create a library of all stable graphene nanopore shapes based on a modification of a well-known algorithm in the mathematical combinatorics of polyforms known as Redelmeier's algorithm. We show that there exists a correspondence between graphene nanopores and triangular polyforms (called polyiamonds) as well as hexagonal polyforms (called polyhexes). We develop the concept of a polyiamond ID to identify unique nanopore isomers. We also use concepts from polyiamond and polyhex geometry to eliminate unstable nanopores containing dangling atoms, bonds, and moieties. The exclusion of such unstable nanopores leads to a remarkable reduction in the possible nanopores from 11.7 million for N=20 to only 0.184 million nanopores, thereby indicating that the number of stable nanopores is almost two orders of magnitude lower and is much more tractable. Not only that, by extracting the polyhex outline, our algorithm allows searching for nanopores with dimensions and shape factors in a specified range.

cond-mat.mtrl-sci↗

arXiv2022

How Grain Boundaries and Interfacial Electrostatic Interactions Modulate Water Desalination Via Nanoporous Hexagonal Boron Nitride

Researchers are currently exploring nanoporous two-dimensional materials, such as hexagonal boron nitride (hBN), as potential desalination membranes. Here, we study the effect of grain boundaries (GBs) and interfacial electrostatic interactions on the desalination performance of bicrystalline nanoporous hBN, using classical molecular dynamics simulations supported by quantum-mechanical density functional theory (DFT) calculations. We investigate three different nanoporous bicrystalline hBN configurations, with symmetric tilt GBs having misorientation angles of 13.2°, 21.8°, and 32.2°. We find that grain boundaries alter the areas and shapes of nanopores in bicrystalline hBN, as compared to the nanopores in monocrystalline hBN. We observe that, although bicrystalline nanoporous hBN with a misorientation angle of 13.2° shows improved water flow rate by ~30%, it demonstrates reduced Na$^\mathrm{+}$ ion rejection by ~6%, as compared to monocrystalline hBN. We also uncover the role of the nanopore shape in water desalination, finding that more elongated pores with smaller sizes (in 21.8°- and 32.2°-misoriented bicrystalline hBN) can match the water permeation through less elongated pores of slightly larger sizes, with a concomitant ~3-4% drop in Na$^\mathrm{+}$ rejection. Simulations also predict that the water flow rate is significantly affected by interfacial electrostatic interactions. Indeed, the water flow rate is the highest when altered partial charges on B and N atoms were determined using DFT calculations, as compared to when no partial charges or bulk partial charges (i.e., charged hBN) were considered. Overall, our work on water/ion transport through nanopores in bicrystalline hBN indicates that the presence of GBs and surface charge can lead, respectively, to a drop in the ion rejection and water permeation performance of hBN membranes.

cond-mat.mtrl-sci↗

arXiv2019

Observation and Spectral Assignment of a Family of Hexagonal Boron Nitride Lattice Defects

Atomic vacancy defects in single unit cell thick hexagonal boron nitride are of significant interest because of their photophysical properties, including single-photon emission, and promising applications in quantum communication and computation. The spectroscopic assignment of emission energies to specific atomic vacancies within the triangular lattice is confounded by the exponential scaling of defect candidates with the number of removed atoms. Herein, we collect more than 1000 spectra consisting of single, isolated zero-phonon lines between 1.69 and 2.25 eV, observing 6 quantized zero-phonon lines arising from hexagonal boron nitride vacancies. A newly developed computational framework for isomer cataloguing significantly narrows the number of candidate vacancies. Direct lattice imaging of hexagonal boron nitride, electronic structure calculations, and subsequent boric acid etching are used to definitively assign the 6 features. Systematic chemical etching supports the assignment by demonstrating the sequence of growth of successively larger vacancy centres from smaller ones, with the defects including a single B vacancy and a 16-atom triangular defect. These features exhibit a range of emission lifetimes from 1 to 6 ns, and phonon sidebands offset by the dominant lattice phonon in hexagonal boron nitride near 1370 cm-1. This assignment should significantly advance the solid-state chemistry and photophysics of such vacancy emitters.

cond-mat.mtrl-sci↗