Speeding-up Hybrid Functional-Based Ab Initio Molecular Dynamics Using Multiple Time-stepping and Resonance-Free Thermostat

Kar R, Mandal S, Thakkur V, Meyer B, Nair NN (2023)

Publication Type: Journal article

Publication year: 2023

Journal

Journal of Chemical Theory and Computation American Chemical Society

Abstract

Ab initio molecular dynamics (AIMD) based on density functional theory (DFT) has become a workhorse for studying the structure, dynamics, and reactions in condensed matter systems. Currently, AIMD simulations are primarily carried out at the level of generalized gradient approximation (GGA), which is at the second rung of DFT functionals in terms of accuracy. Hybrid DFT functionals, which form the fourth rung in the accuracy ladder, are not commonly used in AIMD simulations as the computational cost involved is 100 times or higher. To facilitate AIMD simulations with hybrid functionals, we propose here an approach using multiple time stepping with adaptively compressed exchange operator and resonance-free thermostat, that could speed up the calculations by ∼30 times or more for systems with a few hundred of atoms. We demonstrate that by achieving this significant speed up and making the compute time of hybrid functional-based AIMD simulations at par with that of GGA functionals, we are able to study several complex condensed matter systems and model chemical reactions in solution with hybrid functionals that were earlier unthinkable to be performed.

Authors with CRIS profile

Sagarmoy Mandal Sonderforschungsbereich 953/3 Synthetische Kohlenstoffallotrope Bernd Meyer Professur für Computational Chemistry

Involved external institutions

Indian Institute of Technology Kanpur (IITK)

India (IN)

How to cite

APA:

Kar, R., Mandal, S., Thakkur, V., Meyer, B., & Nair, N.N. (2023). Speeding-up Hybrid Functional-Based Ab Initio Molecular Dynamics Using Multiple Time-stepping and Resonance-Free Thermostat. Journal of Chemical Theory and Computation. https://dx.doi.org/10.1021/acs.jctc.3c00964

MLA:

Kar, Ritama, et al. "Speeding-up Hybrid Functional-Based Ab Initio Molecular Dynamics Using Multiple Time-stepping and Resonance-Free Thermostat." Journal of Chemical Theory and Computation (2023).

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