Roadmap for Molecular Benchmarks in Nonadiabatic Dynamics
arXiv:2502.14569 · doi:10.1021/acs.jpca.5c02171
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 (70)
- Unifying time evolution and optimization with matrix product states
- NWChem: Past, Present, and Future
- Time-evolution methods for matrix-product states
- Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
- Efficient simulation of strong system-environment interactions
- Exact factorization of the time-dependent electron-nuclear wavefunction
- Machine learning for electronically excited states of molecules
- 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
- Imaging the Photochemical Ring-Opening of 1,3-Cyclohexadiene by Ultrafast Electron Diffraction
- Perspectives on double-excitations in TDDFT
- BAGEL: Brilliantly Advanced General Electronic-structure Library
- Machine learning enables long time scale molecular photodynamics simulations
- A coupled-trajectory quantum-classical approach to decoherence in non-adiabatic processes
- Efficient simulation of finite-temperature open quantum systems
- Mapping Variable Ring Polymer Molecular Dynamics: A Path-Integral Based Method for Nonadiabatic Processes
- Femtosecond Intersystem Crossing in the DNA Nucleobase Cytosine
- Direct simulation of electron transfer using ring polymer molecular dynamics: Comparison with semiclassical instanton theory and exact quantum methods
- Multiconfigurational time-dependent Hartree approaches for indistinguishable particles
- Quantum-Classical Liouville Dynamics in the Mapping Basis
- Mapping quantum-classical Liouville equation: projectors and trajectories
- Generalized spin mapping for quantum-classical dynamics
- Nonadiabatic Dynamics in Open Quantum-Classical Systems: Forward-Backward Trajectory Solution
- Spin-mapping approach for nonadiabatic molecular dynamics
- Efficient and accurate surface hopping for long time nonadiabatic quantum dynamics
- Decoherence and Revival in Attosecond Charge Migration Driven by Non-adiabatic Dynamics
- Landau-Zener type surface hopping algorithms
- A mapping approach to surface hopping
- Discontinuities of the exchange-correlation kernel and charge-transfer excitations in time-dependent density functional theory
- Non-adiabatic molecular quantum dynamics with quantum computers
- Generalized Quantum Master Equations In and Out of Equilibrium: When Can One Win?
- Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
- Surface hopping from the perspective of quantum-classical Liouville dynamics
- On the identity of the identity operator in nonadiabatic linearized semiclassical dynamics
- Unified Formulation of Phase Space Mapping Approaches for Nonadiabatic Quantum Dynamics
- Coherent State Mapping Ring-Polymer Molecular Dynamics for Non-Adiabatic quantum propagations
- Direct observation of geometric phase in dynamics around a conical intersection
- Green's function methods for single molecule junctions
- Analog quantum simulation of chemical dynamics
- A multi-state mapping approach to surface hopping
- Improved population operators for multi-state nonadiabatic dynamics with the mixed quantum-classical mapping approach
- Nonadiabatic nuclear dynamics of the ammonia cation studied by surface hopping classical trajectory calculations
- Mapping the Complete Reaction Path of a Complex Photochemical Reaction
- A partially linearized spin-mapping approach for nonadiabatic dynamics. I. Derivation of the theory
- 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
- A tensor network view of multilayer multiconfiguration time-dependent Hartree methods
- Deciphering the Influence of Ground-State Distributions on the Calculation of Photolysis Observables
- A partially linearized spin-mapping approach for nonadiabatic dynamics. II. Analysis and comparison with related approaches
- Surface hopping methodology in laser-driven molecular dynamics
- Performance Evaluation of the Symmetrical Quasi-Classical Dynamics Method based on Meyer-Miller Mapping Hamiltonian in the Treatment of Site-Exciton Models
- Quantum simulation of real-space dynamics
- On the description of conical intersections between excited electronic states with LR-TDDFT and ADC(2)
- Quantum computation of stopping power for inertial fusion target design
- Ab-initio Symmetric Quasi-Classical Approach to Investigate Molecular Tully Models
- Quantum-classical nonadiabatic dynamics of Floquet driven systems
- Quasiclassical approaches to the generalized quantum master equation
- Survey of the Hierarchical Equations of Motion in Tensor-Train format for non-Markovian quantum dynamics
- 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
- Accurate and Efficient Prediction of Double Excitation Energies Using the Particle-Particle Random Phase Approximation
- 2500 vibronic eigenstates of the NO radical
- Exciting DeePMD: Learning excited state energies, forces, and non-adiabatic couplings
- Electronic structure of norbornadiene and quadricyclane
- Wave packet dynamics in the optimal superadiabatic approximation
- A coupled-trajectory approach for decoherence, frustrated hops and internal consistency in surface hopping