Optimized Quantum Drude Oscillators for Atomic and Molecular Response Properties

TL;DR

This paper introduces an optimized quantum Drude oscillator model that accurately reproduces atomic and molecular response properties using only dipolar data, enhancing the development of quantum force fields for simulations.

Contribution

The paper presents a new parametrization of QDOs fixed by dipolar properties, improving accuracy and understanding of many-atom systems.

Findings

Accurately reproduces atomic polarization potentials.

Reproduces multipolar dispersion coefficients.

Enhances quantum-mechanical force field development.

Abstract

The quantum Drude oscillator (QDO) is an efficient yet accurate coarse-grained approach that has been widely used to model electronic and optical response properties of atoms and molecules, as well as polarization and dispersion interactions between them. Three effective parameters (frequency, mass, charge) fully characterize the QDO Hamiltonian and are adjusted to reproduce response properties. However, the soaring success of coupled QDOs for many-atom systems remains fundamentally unexplained and the optimal mapping between atoms/molecules and oscillators has not been established. Here, we present an optimized parametrization (OQDO) where the parameters are fixed by using only dipolar properties. For the periodic table of elements as well as small molecules, our OQDO model accurately reproduces atomic (spatial) polarization potentials and multipolar dispersion coefficients, elucidating the high promise of the presented model in the development of next-generation quantum-mechanical force fields for (bio)molecular simulations.