Related papers: Detailed balance in mixed quantum-classical mappin…
Ring Polymer Surface-Hopping (RPSH) has been recently introduced as a well-tailored method for incorporating nuclear quantum effects (NQEs), such as zero-point energy and tunneling, into non-adiabatic molecular dynamics simulations. The…
Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…
Open quantum systems that comply with the master equation and detailed balance decay in a non-oscillatory manner to thermal equilibrium. Beyond the weak coupling limit, systems that break microreversibility (e.g., in the presence of…
We develop a surface hopping algorithm based on frozen Gaussian approximation for semiclassical matrix Schr\"odinger equations, in the spirit of Tully's fewest switches surface hopping method. The algorithm is asymptotically derived from…
The quantum-classical Liouville equation offers a rigorous approach to nonadiabatic quantum dynamics based on surface hopping type trajectories. However, in practice the applicability of this approach has been limited to short times owing…
The constraint coordinate-momentum \textit{phase space} (CPS) has recently been developed to study nonadiabatic dynamics in gas-phase and condensed-phase molecular systems. Although the CPS formulation is exact for describing the discrete…
Fewest-switches surface hopping (FSSH) has emerged as one of the leading methods for modeling the quantum dynamics of molecular systems. While its original formulation was limited to adiabatic populations, the growing interest in the…
We investigate quantum thermal state preparation algorithms based on system-bath interactions and uncover a surprising phenomenon in the weak-coupling regime. We rigorously prove that, if the system-bath interaction is engineered so that…
An extension of the CCS-method [Chem. Phys. 2004, 304, p. 103-120] for simulating non-adiabatic dynamics with quantum effects of the nuclei is put forward. The time-dependent Schr\"{o}dinger equation for the motion of the nuclei is solved…
We consider the optimization of Markovian dynamics to pursue the fastest convergence to the stationary state. The brachistochrone method is applied to the continuous-time master equation for finite-size systems. The principle of least…
We introduce energy-space quantum walks as a minimal framework to investigate equilibration, thermalization, and irreversibility from an effective-dynamics perspective. By mapping the configuration space of a walk onto a ladder of energy…
We perform extensive benchmark comparisons of surface hopping dynamics with numerically exact calculations for the spin-boson model over a wide range of energetic and coupling parameters as well as temperature. We find that deviations from…
We implement a rare-event sampling scheme for quantifying the rate of thermally-activated nonadiabatic transitions in the condensed phase. Our QM/MM methodology uses the recently developed INAQS package to interface between an elementary…
We present a new approach to calculate real-time quantum dynamics in complex systems. The formalism is based on the partitioning of a system's environment into "core" and "reservoir" modes, with the former to be treated quantum mechanically…
Many important quantities in quantum information science, such as entropy and entanglement, are non-linear functions of the density matrix and cannot be expressed as operator observables. Standard open-system approaches evolve only a single…
Systems of a large number N of globally coupled maps have become popular as a relatively simple prototype of high-dimensional dynamics, showing many interesting and typical phenomena like synchronisation, cluster formation and…
We propose a general framework for a hybrid continuous-discrete algorithm that integrates continuous-time deterministic dynamics with Metropolis-Hastings steps to combine search dynamics with and without detailed balance. Our purpose is to…
We present a novel quantum-classical approach to non-adiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the…
We consider the dynamics of a quantum system immersed in a dilute gas at thermodynamics equilibrium using a quantum Markovian master equation derived by applying the low-density limit technique. It is shown that the Gibbs state at the bath…
Using semiclassical methods, it is possible to construct very accurate approximations in the short wavelength limit of quantum dynamics that rely exclusively on classical dynamical input. For systems whose classical realization is strongly…