Roadmap for Molecular Benchmarks in Nonadiabatic Dynamics

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.

Third version after acceptance by JPCA

References in corpus (26)

• NWChem: Past, Present, and Future
• Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
• Polynomial-time quantum algorithm for the simulation of chemical dynamics
• Nuclear quantum effects in solids using a colored-noise thermostat
• Colored-noise thermostats à la carte
• BAGEL: Brilliantly Advanced General Electronic-structure Library
• Femtosecond Intersystem Crossing in the DNA Nucleobase Cytosine
• Generalized spin mapping for quantum-classical dynamics
• Landau-Zener type surface hopping algorithms
• Unified Formulation of Phase Space Mapping Approaches for Nonadiabatic Quantum Dynamics
• Coherent State Mapping Ring-Polymer Molecular Dynamics for Non-Adiabatic quantum propagations
• Nonadiabatic nuclear dynamics of the ammonia cation studied by surface hopping classical trajectory calculations
• Tree tensor network state approach for solving hierarchical equations of motion
• Which Electronic Structure Method to Choose in Trajectory Surface Hopping Dynamics Simulations? Azomethane as a Case Study
• Ab-initio Symmetric Quasi-Classical Approach to Investigate Molecular Tully Models
• Quantum-classical nonadiabatic dynamics of Floquet driven systems
• Energy-Conserving Coupled Trajectory Mixed Quantum Classical Dynamics
• Validating Fewest-Switches Surface Hopping in the Presence of Laser Fields
• How important are the residual nonadiabatic couplings for an accurate simulation of nonadiabatic quantum dynamics in a quasidiabatic representation?
• Prediction of Photodynamics of 200 nm Excited Cyclobutanone with Linear Response Electronic Structure and Ab Initio Multiple Spawning
• Including photoexcitation explicitly in trajectory-based nonadiabatic dynamics at no cost
• 2500 vibronic eigenstates of the NO${}_3$ radical
• Exciting DeePMD: Learning excited state energies, forces, and non-adiabatic couplings
• Accurate and Efficient Prediction of Double Excitation Energies Using the Particle-Particle Random Phase Approximation
• Electronic structure of norbornadiene and quadricyclane
• A coupled-trajectory approach for decoherence, frustrated hops and internal consistency in surface hopping

Cited by in corpus (1)

• Efficient Quantum Simulation of Non-Adiabatic Molecular Dynamics with Precise Electronic Structure