arXiv subjects

Romain Perriot

Publications and source records attributed to Romain Perriot.

7 recordsLinked to original sources

arXiv2026

Benchmarking Universal Machine Learning Force Fields for Crystal Structure Prediction of High-Energy Molecular Systems

Recent developments of universal machine learning interatomic potentials (UMLIPs) offer a fast route for screening molecular crystals based on geometry relaxation and energy ranking, but their reliability across chemically diverse energetic materials remains elusive. In particular, it is unclear whether or not these UMLIPs are over-sensitive to break the desired molecular connectivity for relaxing the periodic crystals. Herein we tested the hypothesis that classical force-field pre-relaxation can provide a more suitable starting geometry for subsequent UMLIP relaxation on a large database of high energy molecular crystals. Three models (MACE, MACE-OFF and UMA) in conjunction with the General Amber Force Field (GAFF) were applied to test this hypothesis. Among them, direct MACE-OFF and UMA showed very high relaxation success and preserved the reference geometries most closely, but they still exhibit failures for some rare cases. Using GAFF pre-relaxation can systematically reduce the number of failed relaxations with lower computational costs. Our comparative failure and robustness analyses revealed distinct trade-offs among the evaluated models. Among them, MACE-OFF achieves a better compromise between potential energy surface smoothness, structural fidelity, and stress convergence, serving as a good choice to provide a reliable foundation for automated structural optimization.

cond-mat.mtrl-sci↗

arXiv2025

Kinetic Monte Carlo prediction of the morphology of pentaerythritol tetranitrate

In this work, we develop an atomistic, graph-based kinetic Monte Carlo (KMC) simulation routine to predict crystal morphology. Within this routine, we encode the state of the supercell in a binary occupation vector and the topology of the supercell in a simple nearest-neighbor graph. From this encoding, we efficiently compute the interaction energy of the system as a quadratic form of the binary occupation vector, representing pairwise interactions. This encoding, coupled with a simple diffusion model for adsorption, is then used to model evaporation and adsorption dynamics at solid-liquid interfaces. The resulting intermolecular interaction-breaking energies are incorporated into a kinetic model to predict crystal morphology, which is implemented in the open-source Python package Crystal Growth Kinetic Monte Carlo (cgkmc). We then apply this routine to pentaerythritol tetranitrate (PETN), an important energetic material, showing excellent agreement with the attachment energy model.

cond-mat.mtrl-sci↗

arXiv2023

Spin-Polarized Extended Lagrangian Born-Oppenheimer Molecular Dynamics

We present a generalization of Extended Lagrangian Born-Oppenheimer molecular dynamics [Phys. Rev. Lett. vol. 100, 123004 (2008); Eur. Phys. J. B vol. 94, 164 (2021)] that also includes the electronic spin-degrees of freedom as extended dynamical variables. To integrate the combined spin and charge degrees of freedom, we use a preconditioned low-rank Krylov subspace approximation. Our approach is demonstrated for quantum-mechanical molecular dynamics simulations of iron, using spin-polarized self-consistent charge density functional tight-binding theory. We also show how the low-rank Krylov subspace approximation can be used to accelerate the self-consistent field convergence.

physics.chem-ph↗

arXiv2022

A Methodology to Generate Crystal-based Molecular Structures for Atomistic Simulations

We propose a systematic method to construct crystal-based molecular structures often needed as input for computational chemistry studies. These structures include crystal ``slabs" with periodic boundary conditions (PBCs) and non-periodic solids such as Wulff structures. We also introduce a method to build crystal slabs with orthogonal PBC vectors. These methods are integrated into our code, Los Alamos Crystal Cut (LCC), which is open source and thus fully available to the community. Examples showing the use of these methods are given throughout the manuscript.

cond-mat.mtrl-sci↗

arXiv2021

Pressure, temperature, and orientation dependent thermal conductivity of $α$-1,3,5-trinitro-1,3,5-triazinane ($α$-RDX)

We use reverse non-equilibrium molecular dynamics (RNEMD) simulations to determine the thermal conductivity in $α$-RDX in the <100>, <010>, and <001> crystallographic directions. Simulations are carried out with the Smith-Bharadwaj non-reactive empirical interatomic potential [Smith & Bharadwaj, J. Phys. Chem. B 103, 3570(1999)], which represents the thermo-elastic properties of RDX with good accuracy. As an illustration, we report the temperature and pressure dependence of lattice constants of $α$-RDX, which compare well with experimental and ab initio results, as do linear and volume thermal expansion coefficients, which we also calculate. We find that the thermal conductivity depends linearly on the inverse temperature in the 200-400K regime due to the decrease in the phonon mean free path. The thermal conductivity also exhibits anisotropy, with a maximum difference at 300K of 24% between the <001> and <010> directions, an effect that remains when temperature increases. Thermal conductivity in the <100> direction is mostly between the two other directions, although crossovers are predicted with <001> at high temperature, and <010> at low temperature under pressure. We observe that the thermal conductivity varies linearly with pressure up to 4 GPa. The data are fitted to analytical functions for interpolation/extrapolation and use in continuum simulations. MD results are validated against experiments using impulsive stimulated thermal scattering (ISTS) on RDX single crystals at 293K and ambient pressure, showing good qualitative and quantitative agreement: same ordering between the three principal orientations, and an average error of 10% between the experiments and the model. These results provide confidence that the extracted analytical functions using the RNEMD methodology and the Smith-Bharadwaj potential can be applied to model the thermal conductivity of $α$-RDX.

cond-mat.mtrl-sci↗

arXiv2017

Cost Models for Selecting Materialized Views in Public Clouds

Data warehouse performance is usually achieved through physical data structures such as indexes or materialized views. In this context, cost models can help select a relevant set ofsuch performance optimization structures. Nevertheless, selection becomes more complex in the cloud. The criterion to optimize is indeed at least two-dimensional, with monetary cost balancing overall query response time. This paper introduces new cost models that fit into the pay-as-you-go paradigm of cloud computing. Based on these cost models, an optimization problem is defined to discover, among candidate views, those to be materialized to minimize both the overall cost of using and maintaining the database in a public cloud and the total response time ofa given query workload. We experimentally show that maintaining materialized views is always advantageous, both in terms of performance and cost.

cs.DB↗

arXiv2016

Evidence for percolation diffusion of cations and material recovery in disordered pyrochlore from accelerated molecular dynamics simulations

We used classical and accelerated molecular dynamics simulations to characterize vacancy-mediated diffusion of cations in Gd$_2$Ti$_2$O$_7$ pyrochlore as a function of the disorder on the microsecond timescale. We find that cation vacancy diffusion is slow in materials with low levels of disorder. However, higher levels of disorder allow for fast cation diffusion, which is then also accompanied by fast antisite annihilation and ordering of the cations. The cation diffusivity is therefore not constant, but decreases as the material reorders. The results suggest that fast cation diffusion is triggered by the existence of a percolation network of antisites. This is in marked contrast with oxygen diffusion, which showed a smooth increase of the ionic diffusivity with increasing disorder in the same compound. The increase of the cation diffusivity with disorder is also contrary to observations from other complex oxides and disordered media models, suggesting a fundamentally different relation between disorder and mass transport. These results highlight the dynamic interplay between fast cation diffusion and the recovery of disorder and have important implications for understanding radiation damage evolution, sintering and aging, as well as diffusion in disorder oxides more generally.

cond-mat.mtrl-sci↗