Roadmap for Molecular Benchmarks in Nonadiabatic Dynamics

TL;DR

This paper discusses the need for standardized molecular benchmarks in nonadiabatic dynamics to improve method comparison and selection, proposing a community-driven roadmap following a dedicated workshop.

Contribution

It introduces a roadmap and preliminary observations toward establishing a standardized, community-driven molecular benchmark set for nonadiabatic molecular dynamics.

Findings

Identified key challenges in defining molecular benchmarks.

Proposed a roadmap for developing standardized benchmarks.

Emphasized the importance of community collaboration.

Abstract

Simulating the coupled electronic and nuclear response of a molecule to light excitation requires the application of nonadiabatic molecular dynamics. However, when faced with a specific photophysical or photochemical problem, selecting the most suitable theoretical approach from the wide array of available techniques is not a trivial task. The challenge is further complicated by the lack of systematic method comparisons and rigorous testing on realistic molecular systems. This absence of comprehensive molecular benchmarks remains a major obstacle to advances within the field of nonadiabatic molecular dynamics. A CECAM workshop, Standardizing Nonadiabatic Dynamics: Towards Common Benchmarks, was held in May 2024 to address this issue. This Perspective highlights the key challenges identified during the workshop in defining molecular benchmarks for nonadiabatic dynamics. Specifically, this work outlines some preliminary observations on essential components needed for simulations and proposes a roadmap aiming to establish, as an ultimate goal, a community-driven, standardized molecular benchmark set.