Related papers: Non-adiabatic dynamics of electrons and atoms unde…
We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…
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…
A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…
The combined quantum electron-nuclear dynamics is often associated with the Born-Huang expansion of the molecular wave function and the appearance of nonadiabatic effects as a perturbation. On the other hand, native multicomponent…
The molecular junction geometry is modelled in terms of nuclear degrees of freedom that are embedded in a stochastic quantum environment of non-equilibrium electrons. Time-evolution of the molecular geometry is governed via a mean force, a…
We propose a novel method to describe realistically ionization processes with absorbing boundary conditions in basis expansion within the formalism of the so-called Non-Adiabatic Quantum Molecular Dynamics. This theory couples…
In this paper we develop the Non-Equilibrium Green's Function (NEGF) formalism for a dissipative molecular junction that consists of a central molecular system with one-dimensional electronic transport coupled to a phonon environment and…
We develop a semi-classical method to simulate the motion of atoms in a dissipative optical lattice. Our method treats the internal states of the atom quantum mechanically, including all nonadiabatic couplings, while position and momentum…
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…
Dynamics of neutral atoms in nonuniform magnetic fields, typical of quadrupole magnetic traps, is considered by applying an accurate method for solving nonlinear systems of differential equations. This method is more general than the…
We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…
The theoretical investigation of non-adiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the…
Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport [Kershaw and Kosov, J.Chem. Phys. 2017, 147, 224109 and J. Chem. Phys. 2018, 149, 044121] is extended to the case of interacting electrons. We consider a…
In this review we consider those processes in condensed matter that involve the irreversible flow of energy between electrons and nuclei that follows from a system being taken out of equilibrium. We survey some of the more important…
Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…
Kinetic equations governing time evolution of positions and momenta of atoms in extended systems are derived using quantum-classical ensembles within the Non-Equilibrium Statistical Operator Method (NESOM). Ions are treated classically,…
Non-adiabatic dynamics at molecule-metal interfaces govern diverse and technologically important phenomena, from heterogeneous catalysis to dye-sensitized solar energy conversion and charge transport across molecular junctions. Realistic…
We present a detailed derivation and numerical tests of a new mixed quantum-classical scheme to deal with non-adiabatic processes. The method is presented as the zero-th order approximation to the exact coupled dynamics of electrons and…
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…
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…