Title :

Rapid and accurate simulation of electron dynamics across nanostructures

Abstract :

Accurate first-principles modeling of electron dynamics is a challenging area of research. To follow the dynamics of molecular electron density one has to solve the time-dependent electronic Schrödinger equation (TDSE). Straight-forward extensions of common quantum chemistry methods to the time-dependent domain reveal density functional theory (DFT), or even the coupled cluster theories to be extremely unsuited for this purpose. In a series of studies, we have demonstrated linear equations of motions to be one of the fundamental requirements to reliably model electonic wavepacket dynamics, or coherent controlled state-to-state excitation. To this end, we have developed one of the most effcient implementations of the time-dependent configuration-interaction (TDCI) methodology to solve the TDSE. Our
implementation has been successfully applied to follow the electron transport across molecular wires and nanostructures terminating in a small metal cluster or a model gold surface. When combined with imaginary time propagation, or other variational schemes TDCI can be utilized also to perform time-independent task of computing the bound states. The present talk will provide an overview of the TDCI methodology and summarize the results of some recent applications.

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