Related papers: Non-adiabatic quantum molecular dynamics: Ionizati…
Electron-electron interactions and correlations form the basis of difficulties encountered in the theoretical solution of problems dealing with multi-electron systems. Accurate treatment of the electron-electron problem is likely to unravel…
We consider quantum dynamics for which the strict adiabatic approximation fails but which do not escape too far from the adiabatic limit. To treat these systems we introduce a generalisation of the time dependent wave operator theory which…
We introduce a novel computational framework for excited-states molecular quantum dynamics simulations driven by quantum computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method…
The adiabatic approximation is a natural approach for the description of phenomena induced by low frequency laser radiation because the ratio of the laser frequency to the characteristic frequency of an atom or a molecule is a small…
Continuum or discrete polarizable models for the study of optoelectronic processes in embedded subsystems rely mostly on the restriction of the surrounding electronic dielectric response to its low frequency limit. Such a description hinges…
The limits of linear electrodynamics are reviewed, and possible directions of nonlinear extension are explored. The central theme is that the qualitative character of the empirical successes of quantum electrodynamics must be used as a…
We present a general multi-component density functional theory in which electrons and nuclei are treated completely quantum mechanically, without the use of a Born-Oppenheimer approximation. The two fundamental quantities in terms of which…
In this paper we calculate and visualize the dynamics of an ensemble of electrons trapping in an electrostatic wave of slowly increasing amplitude, illustrating that, despite disordering of particles in angle during the trapping transition…
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…
We build on the concept of eigenvector continuation to develop an efficient multi-state method for the rigorous and smooth interpolation of a small training set of many-body wavefunctions through chemical space at mean-field cost. The…
We prove that for a combined system of classical and quantum particles, it is possible to write a dynamics for the classical particles that incorporates in a natural way the Boltzmann equilibrium population for the quantum subsystem. In…
Starting with the exact factorization of the molecular wavefunction, this paper presents the results from the numerical implementation in nonadiabatic molecular dynamics of the recently proposed bohmion method. Within the context of quantum…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
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…
The adiabatic theorem is an important concept in quantum mechanics, it tells that a quantum system subjected to gradually changing external conditions remains to the same instantaneous eigenstate of its Hamiltonian as it initially in. In…
We consider an implementation of the adiabatic spin dynamics approach in a tight-binding description of the electronic structure. The adiabatic approximation for spin-degrees of freedom assumes that the faster electronic degrees of freedom…
Non-equilibrium thermodynamics can provide strong advantages when compared to more standard equilibrium situations. Here, we present a general framework to study its application to concrete problems, which is valid also beyond the…
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…
A multiscale QM/classical approach is presented, that is able to model the optical properties of complex nanostructures composed of a molecular system adsorbed on metal nanoparticles. The latter are described by a combined…
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…