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The violation of detailed balance poses a serious problem for the majority of current quasiclassical methods for simulating nonadiabatic dynamics. In order to analyze the severity of the problem, we predict the long-time limits of the…
The formalism of the generalized quantum master equation (GQME) is an effective tool to simultaneously increase the accuracy and the efficiency of quasiclassical trajectory methods in the simulation of nonadiabatic quantum dynamics. The…
We describe a multiple electronic state adaptation of the mapping approach to surface hopping introduced recently by Mannouch and Richardson (J. Chem. Phys. 158, 104111 (2023)). This adaptation treats populations and coherences on an equal…
We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…
We use the effective Hamiltonian that we recently fitted against the first 306 experimentally observed vibronic transitions of NO2 [J. Chem. Phys. 119, 5923 (2003)] to investigate the time domain nonadiabatic dynamics of this molecule on…
Simulating the nonadiabatic dynamics of condensed-phase systems continues to pose a significant challenge for quantum dynamics methods. Approaches based on sampling classical trajectories within the mapping formalism, such as the linearized…
The exact factorization approach has led to the development of new mixed quantum-classical methods for simulating coupled electron-ion dynamics. We compare their performance for dynamics when more than two electronic states are occupied at…
We present a strategy for mapping the dynamics of a fermionic quantum system to a set of classical dynamical variables. The approach is based on imposing the correspondence relation between the commutator and the Poisson bracket, preserving…
We investigate detailed balance for a quantum system interacting with thermal radiation within mixed quantum-classical theory. For a two-level system coupled to classical radiation fields, three semiclassical methods are benchmarked: (1)…
Many quantum algorithms can be seen as a transition from a well-defined initial quantum state of a complex quantum system, to an unknown target quantum state, corresponding to a certain eigenvalue either of the Hamiltonian or of a…
Nonadiabatic quantum-classical mapping approaches have significantly gained in popularity in the past several decades because they have acceptable accuracy while remaining numerically tractable even for large system sizes. In the recent few…
We calculate the electronic relaxation of a single electron in a quantum dot with two electronic orbital states, and with the electronic coupling to the longitudinal optical modes of the lattice vibrations included in the multiple…
We present a new partially linearized mapping-based approach for approximating real-time quantum correlation functions in condensed-phase nonadiabatic systems, called spin-PLDM. Within a classical trajectory picture, partially linearized…
Experiments indicate that collective coupling of molecular ensembles to confined optical modes can modify excited-state dynamics and photochemical reactivity. To describe such cavity-induced effects at atomic resolution, semi-classical…
An alternative methodology to investigate indirect polyatomic processes with quasi-classical trajectories is proposed, which effectively avoids any binning or weighting procedure while provides rovibrational resolution. Initial classical…
We extend the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), a semiclassical method for computing real-time correlation functions, to electronically nonadiabatic systems using the Meyer-Miller-Stock-Thoss (MMST) Hamiltonian…
Trajectory-based methods that propagate classical nuclei on multiple quantum electronic states are often used to simulate nonadiabatic processes in the condensed phase. A long-standing problem of these methods is their lack of detailed…
An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely-spaced electronic states. We propose a mixed quantum-classical scheme…
We propose a trajectory-based quasiclassical method for approximating dynamics in condensed phase systems. Building upon the previously developed Optimized Mean Trajectory (OMT) approximation that has been used to compute linear and…
We propose a computationally efficient method to solve the dynamics of operators of bosonic quantum systems coupled to their environments. The method maps the operator under interest to a set of complex-valued functions, and its adjoint…