相关论文: Electronic non-adiabatic states

An accurate theory describing adiabatic following of the dark, nonabsorbing state in the three-level system is developed. An analytical solution for the wave function of the particle experiencing Raman excitation is found as an expansion in…

This work presents an alternative, general, and in-principle exact extension of electronic Kohn-Sham density functional theory (KS-DFT) to the fully quantum-mechanical molecular problem. Unlike in existing multi-component or…

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…

Vibrational energies and wave functions of the triplet state of the H3+ ion have been determined. In the calculations, the ground and first excited triplet electronic states are included as well as the non-Born-Oppenheimer coupling between…

We present a universal expression for the electronic friction as felt by a set of classical nuclear degrees of freedom (DoF's) coupled to a manifold of quantum electronic DoF's; no assumptions are made regarding the nature of the electronic…

An adiabatic-connection fluctuation-dissipation theorem approach based on a range separation of electron-electron interactions is proposed. It involves a rigorous combination of short-range density functional and long-range random phase…

We study non--adiabatic transitions in scattering theory for the time dependent molecular Schroedinger equation in the Born--Oppenheimer limit. We assume the electron Hamiltonian has finitely many levels and consider the propagation of…

Modern density functional theory (DFT) calculations employ the Kohn-Sham (KS) system of non-interacting electrons as a reference, with all complications buried in the exchange-correlation energy (Exc). The adiabatic connection formula gives…

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…

Variational wave functions are very useful for describing the panoply of ground states found in interacting many-electron systems. Some particular trial states are "adiabatically" linked to a reference state, from which they borrow the…

Trajectory-based mixed quantum-classical approaches to coupled electron-nuclear dynamics suffer from well-studied problems such as the lack of (or incorrect account for) decoherence in the trajectory surface hopping method and the inability…

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…

We present a novel theory and implementation for computing coupled electronic and quantal nuclear subsystems on a single potential energy surface, moving beyond the standard Born-Oppenheimer (BO) separation of nuclei and electrons. We…

We evaluate all the electron-phonon couplings derived from the one-body electronic interactions, in both the adiabatic and extreme non-adiabatic limit, for a dimer with a non-degenerate orbital built from atomic wave functions of Gaussian…

A non-adiabatic nuclear wavepacket dynamics simulation of the H$_2$O$^+$ de-excitation process is performed based on electronic structure calculations using the variational quantum eigensolver. The adiabatic potential energy surfaces and…

The Exact Factorization (XF) of molecular wavefunctions can be viewed as an 'electronic wavepacket' framework for quantum dynamics. It is an appealing alternative to the conventional non-adiabatic dynamics, unfolding in the space of coupled…

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…

We investigate the exact wavefunction as a single product of electronic and nuclear wavefunction for a model conical intersection system. Exact factorized spiky potentials and nodeless nuclear wavefunctions are found. The exact factorized…

We show that the time dependent single electron, nuclear density matrix of an interacting electronic system coupled to nuclear degrees of freedom can be exactly reproduced by that of an electronic system with arbitrarily specified…

Using an accurate semi-analytic wavefunction for two electron atoms, we construct the external potential for varying strength of electron-electron (e-e) interaction. Using this potential we explicitly calculate the energy of their positive…