Related papers: Why do mixed quantum-classical methods describe sh…
We analyze two approaches to the quantum-classical Liouville (QCL) formalism that differ in the order of two operations: Wigner transformation and projection onto adiabatic electronic states. The analysis is carried out on a two-dimensional…
We present a means of studying rare reactive pathways in open quantum systems using Transition Path Theory and ensembles of quantum jump trajectories. This approach allows for elucidation of reactive paths for dissipative, nonadiabatic…
Nonadiabatic effects appear due to avoided crossings or conical intersections that are either intrinsic properties in field-free space or induced by a classical laser field in a molecule. It was demonstrated that avoided crossings in…
We investigate the role of the geometric phase (GP) in an internal conversion process when the system changes its electronic state by passing through a conical intersection (CI). Local analysis of a two-dimensional linear vibronic coupling…
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…
Beyond the adiabatic regime, our understanding of quantum dynamics in coupled systems remains limited, and the choice of representation continues to obscure physical interpretation and simulation accuracy. Here we propose a natural and…
We developed a general theoretical approach and a user-ready computer code that permit to study the dynamics of collisional energy transfer and ro-vibrational energy exchange in complex molecule-molecule collisions. The method is a mixture…
We consider the dynamics of interacting quantum and classical systems in the Heisenberg representation. Unlike the usual construction in standard quantum mechanics, mixed quantum-classical systems involve the interplay of unitary operators…
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…
The powerful molecular dynamics (MD) simulation is basically based on a picture that the atoms experience classical-like trajectories under the exertion of classical force field determined by the quantum mechanically solved electronic…
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…
The exact nuclear time-dependent potential energy surface arises from the exact decomposition of electronic and nuclear motion, recently presented in [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)]. Such…
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…
Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses, to control the formation of photoproducts. Such molecular processes can in principle be simulated with various nonadiabatic…
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…
The thawed Gaussian Ehrenfest dynamics is a single-trajectory method that partially includes both nuclear quantum and electronically nonadiabatic effects by combining the thawed Gaussian wavepacket dynamics with Ehrenfest dynamics. First,…
The direct observation of non-adiabatic dynamics at conical intersections is a long-standing goal of molecular physics. Novel time-resolved spectroscopies have been proposed which are sensitive to electronic coherences induced by the…
We derive a model of quantum-classical hybrids for a simplified model of quantum electrodynamics in the framework of the stochastic variational method. In this model, charged particle trajectories are affected by the interaction with…
On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…
The geometric phase stands as a foundational concept in quantum physics, revealing deep connections between geometric structures and quantum dynamical evolution. Unlike dynamical phases, geometric phases exhibit intrinsic resilience to…