1. Combined Coherent-States/Density-Functional-Theory Dynamics ACS PRF# AC6 Jorge A. Morales Department of Chemistry and Biochemistry Texas Tech University PO Box 41061, Lubbock, TX , USA
The vast realm of the coherent states (CS) theory can provide a convenient framework for the direct simulation of chemical reactions. Specifically, CS sets furnish adequate over-complete sets to represent wave functions and to express the quantum dynamical equations of a molecular system in a classical-like format. In this project, we are merging such a CS approach to chemical dynamics with density functional theory capabilities to benefit from their adequate description of electron correlation effects at low computational cost. In the resulting methodology, nuclei are described by a product of narrow, frozen Gaussian wave packets, which is separable into translational, rotational, and vibrational quasi-classical CS, whereas electrons are described by a single-determinantal Thouless CS in a Kohn-Sham fashion. This approach improves some features of the celebrated Car-Parrinello method by providing: an ab initio CS Lagrangian, a quasi-classical CS analysis of dynamical properties at final time, and a non-redundant representation of an electronic single-determinantal state. This methodology is being implemented into the CSTechG program package.
Figure: Four snapshots of the time-dependent charge density in H+ + C2H2 at ELab = 30 eV