Related papers: Mixed quantum-classical dynamics on the exact time…
Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…
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 generalise the celebrated semiclassical wavepacket approach from the adiabatic to the non-adiabatic regime. A unified description covering both of these regimes is particularly desired for systems with spatially varying band structures…
The exact factorization of the time-dependent electron-nuclear wavefunction has been employed successfully in the field of quantum molecular dynamics simulations for interpreting and simulating light-induced ultrafast processes. In this…
A novel treatment of non-adiabatic couplings is proposed. The derivation starts from the long-known, but not well-known, fact that the wave function of the complete system of elctrons and nuclei can be written, without approximation, as a…
The time-dependent exchange-correlation potential has an unusual task in directing fictitious non-interacting electrons to move with exactly the same probability density as true interacting electrons. This has intriguing implications for…
We identify peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory that are crucial for time-resolved electron scattering in a model one-dimensional system. These structures are…
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…
Ehrenfest dynamics is a useful approximation for ab initio mixed quantum-classical molecular dynamics that can treat electronically nonadiabatic effects. Although a severe approximation to the exact solution of the molecular time-dependent…
A theory of electronic friction is developed using the exact factorization of the electron-nuclear wavefunction. No assumption is made regarding the electronic bath, which can be made of independent or interacting electrons, and the nuclei…
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…
Mixed quantum-classical methods, such as surface hopping and Ehrenfest dynamics, have proven useful for describing molecular processes involving multiple electronic states. These methods require propagating many independent trajectories,…
We describe a novel approach to subsystem decoherence without the usual tracing-out of the environment. The subsystem of focus is described entirely by a pure state evolving non-unitarily along a single classical trajectory of its…
Nuclear quantum effects and non-Born--Oppenheimer effects play a vital role in many chemical and biological processes, motivating the incorporation of such effects into dynamical simulations. In real-time nuclear--electronic orbital…
A generalized formalism of the so-called non-adiabatic quantum molecular dynamics is presented, which applies for atomic many-body systems in external laser fields. The theory treats the nuclear dynamics and electronic transitions…
We discuss nuclear dynamics at molecule-metal interfaces including non-equilibrium molecular junctions. Starting from the many-body states (pseudoparticle) formulation of the molecule-metal system in the molecular vibronic basis, we…
We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with…
Non-adiabatic molecular phenomena, arising from the breakdown of the Born-Oppenheimer approximation, govern the fate of virtually all photo-physical and photochemical processes and limit the quantum efficiency of molecules and other…
We derive an accurate molecular orbital based expression for the coherent time evolution of a two-electron wave function in a quantum dot molecule where the electrons interact with each other, with external time dependent electromagnetic…
Crossing a quantum critical point in finite time challenges the adiabatic condition due to the closing of the energy gap, which ultimately results in the formation of excitations. Such non-adiabatic excitations are typically deemed…