Ab initio Gutzwiller method: first application to plutonium

Ab-initio Gutzwiller method: first application to Plutonium

Using a density matrix approach to Gutzwiller method, we present a formalism to treat ab-initio multiband Tight-Binding Hamiltonians including local Coulomb interaction in a solid, like, for e.g., the degenerate Hubbard model. We first derive the main results of our method: starting from the density matrix of the non-interacting state, we build a multi-configurational variational wave function....

Application of wavefunction-based ab initio methods to extended systems

The quantum-mechanical problems of solving the electronic Hamiltonian of realistic system on an ab initio level is mainly tackled with the density functional approach, which relies on the ground-state density of the system and avoids the calculation of the many-body wavefunction of the system. However, the present DFT-based approaches are not amenable to systematic improvements. Therefore, it i...

Development of a Non-Adiabatic Ab Initio Molecular Dynamics Method and its Application to Photodynamical Processes

A fewest switches trajectory surface hopping algorithm based on linear response time-dependent density functional theory is developed and implemented into the plane wave ab initio molecular dynamics package CPMD. A scheme to calculate non-adiabatic couplings using a multi determinantal approximation of the excited state wavefunction is introduced. The method is applied to the study of the photo...

Just How Ab Initio Is Ab Initio Quantum Chemistry?

Quantum Mechanics has been the most spectacularly successful theory in the history of science. As is often mentioned the accuracy to which the gyromagnetic ratio of the electron can be calculated is a staggering nine decimal places. Quantum Mechanics has revolutionized the study of radiation and matter since its inception just over one hundred years ago. The impact of the theory has been felt i...

First ultraviolet absorption band of methane: An ab initio study