DL_POLY Quantum 2.1 software: A suite of real-time path integral methods for the simulation of dynamical properties and vibrational spectra

TL;DR

DL_POLY Quantum 2.1 introduces advanced real-time path integral methods for large-scale molecular dynamics simulations, enabling accurate vibrational spectra and nuclear quantum effects modeling in complex condensed phase and interfacial systems.

Contribution

The paper presents new real-time path integral methods, including hybrid CMD, integrated into DL_POLY Quantum 2.1 for improved simulation of vibrational spectra with nuclear quantum effects.

Findings

Demonstrated accurate IR spectra simulation for water and ice at various temperatures.

Showcased large-scale electrolyte solution simulations with improved spectral accuracy.

Validated the hybrid CMD method's ability to overcome curvature and broadening issues.

Abstract

DL_POLY Quantum 2.1 is introduced here as a highly modular, sustainable, and scalable general-purpose molecular dynamics (MD) simulation software for large-scale long-time MD simulations of condensed phase and interfacial systems with the essential nuclear quantum effects (NQEs) included. The new release improves upon version 2.0 through the introduction of several emerging real-time path integral (PI) methods, including fast centroid molecular dynamics (f-CMD) and fast quasi-CMD (f-QCMD) methods, as well as our recently introduced hybrid CMD (h-CMD) method for the accurate and efficient simulation of vibrational infrared spectra. Several test cases, including liquid bulk water at 300 K and ice Ih at 150 K, are used to showcase the performance of different implemented PI methods in simulating the infrared spectra at both ambient conditions and low temperatures where NQEs become more apparent. Additionally, using different salt-in-water (i.e., dilute) and water-in-salt (i.e., concentrated) lithium bis(trifluoromethanesulfonyl)imide (Li-TFSI) aqueous electrolyte solutions, we demonstrate the applicability of our recently introduced h-CMD method implemented in DL_POLY Quantum 2.1 for the large scale simulation of IR spectra of complex heterogeneous systems. We show that h-CMD can overcome the curvature problem of CMD and the artificial broadening of T-RPMD for the accurate simulation of the vibrational spectra of complex, heterogeneous systems with NQEs included.