arXiv subjects

Sutirtha Paul

Publications and source records attributed to Sutirtha Paul.

7 recordsLinked to original sources

arXiv2026

Interface Engineering of Helium Confinement in Argon-Preplated MCM-41 Nanopores

Atomic-scale modification of mesopore interfaces provides a route to tune the confinement experienced by adsorbed fluids, but how a specific interface preparation translates into the resulting microscopic confinement potential remains unclear. Here, we show that preplating MCM-41 with an argon monolayer modifies the effective pore interface by occupying strongly attractive regions of the heterogeneous silica surface and screening its atomic-scale corrugation. Grand-canonical Monte Carlo simulations of argon adsorption, low-temperature molecular dynamics, and helium test-particle insertion are combined with adsorption isotherms and neutron-scattering measurements to characterize the preplated pore at the atomic scale. Helium test-particle insertion calculations show that the modified interface shifts the helium adsorption minimum to an annular region inside the pore and produces a confinement landscape dominated by a smooth radial component. The resulting radial confinement potential can be described by a continuum cylindrical model, providing microscopic support for the effective potential used in earlier quantum Monte Carlo studies. Residual corrugation persists over multiple spatial scales and is accurately captured by a Gaussian process surrogate. These results demonstrate how atomic preplating can tailor nanopore confinement and provide an experimentally constrained microscopic potential for predictive studies of confined quantum fluids.

cond-mat.mtrl-sci↗

arXiv2026

Bosonic Condensed Phase Real-time Dynamics from Ring Polymer Molecular Dynamics

We present a method for approximating real-time correlation functions and quantum transport coefficients of bosonic condensed phases. The direct evaluation of quantum real-time correlation functions in the path integral formulation is impossible due to a severe dynamical sign problem. Evaluating imaginary-time correlation functions and inverting them using analytic continuation is famously ill-posed. Ring polymer molecular dynamics (RPMD) provides an alternative approach resulting in accurate approximations for real-time correlation functions of condensed phases but neglects exchange effects. In this work, we develop a bosonic RPMD method, which is exact in the harmonic, short time, and high temperature limits. A critical enabling observation is that the Kubo-transformed correlation function for bosons is real only when the correlated observables are symmetric under exchange. We benchmark the method on harmonic and anharmonic model systems and then use it to directly obtain the Lieb-Liniger gas density-density real-time correlation functions at various temperatures and momentum transfers. This work enables the direct simulation of finite-temperature, real-time dynamics of large bosonic condensed phases using RPMD for the first time.

physics.chem-ph↗

arXiv2026

Physically Constrained Ensemble Gaussian Process Modelling for Expensive Quantum Systems with Heteroskedastic Noise

Accurate modeling of quantum many-body systems often requires computationally expensive simulations such as Density Matrix Renormalization Group (DMRG) or Quantum Monte Carlo (QMC) calculations. These methods, while precise, impose significant time and resource constraints, limiting their use in exhaustive parameter exploration. Moreover, these expensive simulations can contain variable errors over the large unknown parameter space, which needs to be quantified and propagated. Thus, predictive modelling is required to estimate the functional space accurately over scarcely sampled data with heteroskedastic noise, while preserving the physical relevance of the estimation. Therefore, we present a Physically Constrained Ensemble Gaussian Process (pc-EGP) framework designed to efficiently model complex and noisy quantum systems under physical consistency constraints. The proposed method first enforces physical constraints as a user controlled weighted penalty to the data-driven loss function of the Gaussian Process (GP) surrogates. Then an ensemble of such GP models is trained with variable noisy simulations via numerical quadrature method where these multiple GP(s) at different nodes is integrated as a quadrature weighted average. We first demonstrate the framework on synthetically generated data before applying to quantum systems. In the first case study, we leverage DMRG simulations of the Bose-Hubbard Model to predict the critical interaction parameter Uc governing the superfluid-to-Mott-insulator transition. In the second case study, we demonstrate our method on QMC simulations, of a quantum liquid confined inside a nanoporous silicate with the goal of optimizing a chemical environment to realize a one-dimensional superfluid. Compared to conventional GP, pc-EGP achieves a better balance of accuracy and physically meaningful predictions.

physics.comp-ph↗

arXiv2026

Accurate Helium-Benzene Potential: from CCSD(T) to Gaussian Process Regression

The accurate modeling of non-covalent interactions between helium and graphitic materials is important for understanding quantum phenomena in reduced dimensions, with the helium-benzene complex serving as the fundamental prototype. However, creating a quantitatively reliable potential energy surface (PES) for this weakly bound system remains a significant computational challenge. In this work, we present a comprehensive, multi-level investigation of the He-Bz interaction, establishing benchmark energies using high-level coupled-cluster singles-and-doubles with perturbative triples (CCSD(T)) methods extrapolated to the complete basis set limit and assessing higher-order (CCSDT(Q)) contributions. We use symmetry-adapted perturbation theory (SAPT) to benchmark it against CCSD(T) and to decompose the interaction into its physical components-confirming it is dominated by a balance between dispersion and exchange-repulsion. A continuous, three-dimensional PES is constructed from discrete ab initio points using multifidelity Gaussian process regression that combines density functional theory results with sparse coupled-cluster energies. The result is a highly accurate PES with sub-cm-1 accuracy that obeys physical laws. This new PES is applied to path integral Monte Carlo (PIMC) simulations to study the solvation of 4He atoms on benzene at low temperatures. Our PIMC results reveal qualitatively different solvation behavior, particularly in the filling of adsorption layers, when compared to simulations using commonly employed empirical Lennard-Jones potentials. This work provides a benchmark PES essential for accurate many-body simulations of helium on larger polycyclic aromatic hydrocarbons towards graphene.

physics.chem-ph↗

arXiv2025

Combining Harmonic Sampling with the Worm Algorithm to Improve the Efficiency of Path Integral Monte Carlo

We propose an improved Path Integral Monte Carlo (PIMC) algorithm called Harmonic PIMC (H-PIMC) and its generalization, Mixed PIMC (M-PIMC). PIMC is a powerful tool for studying quantum condensed phases. However, it often suffers from a low acceptance ratio for solids and dense confined liquids. We develop two sampling schemes especially suited for such problems by dividing the potential into its harmonic and anharmonic contributions. In H-PIMC, we generate the imaginary time paths for the harmonic part of the potential exactly and accept or reject it based on the anharmonic part. In M-PIMC, we restrict the harmonic sampling to the vicinity of local minimum and use standard PIMC otherwise, to optimize efficiency. We benchmark H-PIMC on systems with increasing anharmonicity, improving the acceptance ratio and lowering the auto-correlation time. For weakly to moderately anharmonic systems, at $\beta \hbar \omega=16$, H-PIMC improves the acceptance ratio by a factor of 6-16 and reduces the autocorrelation time by a factor of 7-30. We also find that the method requires a smaller number of imaginary time slices for convergence, which leads to another two- to four-fold acceleration. For strongly anharmonic systems, M-PIMC converges with a similar number of imaginary time slices as standard PIMC, but allows the optimization of the auto-correlation time. We extend M-PIMC to periodic systems and apply it to a sinusoidal potential. Finally, we combine H- and M-PIMC with the worm algorithm, allowing us to obtain similar efficiency gains for systems of indistinguishable particles.

physics.comp-ph↗

arXiv2025

Localization and Wetting of 4He Inside Pre-plated Nanopores

Low dimensional quantum fluids, where one can probe the effects of enhanced thermal and quantum fluctuations on macroscopic quantum wavefunctions, can be experimentally realized through transverse physical confinement of superfluid helium on scales smaller than the coherence length. Reaching this scale is difficult, requiring confinement in single or multiple pores with nanometer radii. Porous silicates such as MCM-41 have a pore radius larger than the coherence length of 4He, and in this work we systematically explore the possibility of pre-plating pores with different elements to reduce the pore size without localizing the confined superfluid. Through a direct solution of the few-body Schrodinger equation combined with quantum Monte Carlo simulations, we explore the behavior of helium confined inside cylindrical nanopores for a range of pre-plating elements, including rare gases and alkali metals. For rare gases, we find that helium remains strongly attracted to the pore walls and any atoms in the core form an incompressible liquid. For alkali metals such as Cs, weak interactions between helium and the pre-plating material prevent localization near the walls and enable delocalization in the pore center. Our results extend previous results for helium wetting on flat two dimensional coated substrates to the curved geometry inside nanopores, and demonstrate that alkali pre-plated nanopores may enable a tunable one-dimensional confined quantum liquid of helium.

cond-mat.mes-hall↗

arXiv2025

Novel Experimental Platform to realize One-dimensional Quantum Fluids

Templated porous materials, such as MCM-41, due to the uniformity of their onedimensional structure and scalability in synthesis, have emerged as an attractive medium for studying one-dimensional quantum fluids. However, the experimental challenge of synthesizing these materials with pore radii smaller than 15 Angstroms hinders the realization of a one-dimensional quantum liquid of helium within such systems, as the coherence length of helium is shorter than the pore radius. Recently, DelMaestro et. al. have preplated MCM-41 with Ar resulting in a reduction of the pore size and a softening of the adsorption potential allowing them to observe 1D Tomanga-Luttinger liquid like behavior. In this paper we present a novel method to obtain an even more ideal environment for studying the behavior of 1D 4He. We propose preplating MCM-41 pores with cesium (Cs) metal. The non-wetting nature of helium on a Cs-coated surface, coupled with the large atomic radius of cesium, creates an optimal environment for confining a quantum liquid of helium in one-dimensional geometry. We present preliminary measurements of adsorption isotherms and Small Angle X-ray Scattering studies that 1reveal a reduction in pore radius upon preplating MCM-41 with Cs, demonstrating promising prospects for facilitating the realization of one-dimensional quantum fluids in templated porous materials.

cond-mat.mtrl-sci↗