Related papers: Semiclassical Nonadiabatic Molecular Dynamics Usin…
Accurately modeling photochemical reactions is difficult due to the presence of conical intersections and locally avoided crossings as well as the inherently multiconfigurational character of excited states. As such, one needs a multi-state…
We propose to measure nonadiabaticity of molecular quantum dynamics rigorously with the quantum fidelity between the Born-Oppenheimer and fully nonadiabatic dynamics. It is shown that this measure of nonadiabaticity applies in situations…
Nonadiabatic molecular dynamics simulations aim to describe the coupled electron-nuclear dynamics of molecules in excited electronic states. These simulations have been applied to understand a plethora of photochemical and photophysical…
A global hybrid extension of variational two-electron reduced-density matrix (v2RDM)-driven multiconfiguration pair-density functional theory (MCPDFT) is developed. Using a linear decomposition of the electron-electron repulsion term, a…
Modeling many-body quantum systems with strong interactions is one of the core challenges of modern physics. A range of methods has been developed to approach this task, each with its own idiosyncrasies, approximations, and realm of…
A single-term density functional model for nondynamic and strong correlation is presented, based on single-determinant Kohn-Sham density functional theory. It is derived from modeling the adiabatic connection and contains only two nonlinear…
A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…
We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…
A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…
We propose a computationally efficient approach to the nonadiabatic time-dependent density functional theory (TDDFT) which is based on a representation of the frequency-dependent exchange correlation kernel as a response of a set of damped…
We simulate the nonadiabatic dynamics of photo-induced isomerization and dissociation in ethylene using ab initio classical trajectories in an extended phase space of nuclear and electronic variables. This is achieved by employing the…
The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT)…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
Time-dependent density-functional theory (TDDFT) treats dynamical exchange and correlation (xc) via a single-particle potential, Vxc(r,t), defined as a nonlocal functional of the density n(r',t'). The popular adiabatic local-density…
We formulate a rigorous method for calculating a nonadiabatic (frequency-dependent) exchange-correlation (XC) kernel required for correct description of both equilibrium and nonequilibrium properties of strongly correlated systems within…
When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) emerge as the fundamental excitations…
A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…
Non-adiabatic dynamics simulations have become a standard approach to explore photochemical reactions. Such simulations require underlying potential energy surfaces and couplings between them, calculated at a chosen level of theory, yet…
Electronic friction and Langevin dynamics is a popular mixed quantum-classical method for simulating the nonadiabatic dynamics of molecules interacting with metal surfaces, as it can be computationally more efficient than fully quantum…
Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…