Chemical bonding in excited states: Energy transfer and charge redistribution from a real space perspective

J Comput Chem. 2017 May 15;38(13):957-970. doi: 10.1002/jcc.24769. Epub 2017 Mar 7.

Abstract

This work provides a novel interpretation of elementary processes of photophysical relevance from the standpoint of the electron density using simple model reactions. These include excited states of H2 taken as a prototype for a covalent bond, excimer formation of He2 to analyze non-covalent interactions, charge transfer by an avoided crossing of electronic states in LiF and conical interesections involved in the intramolecular scrambling in C2 H4 . The changes of the atomic and interaction energy components along the potential energy profiles are described by the interacting quantum atoms approach and the quantum theory of atoms in molecules. Additionally, the topological analysis of one- and two-electron density functions is used to explore basic reaction mechanisms involving excited and degenerate states in connection with the virial theorem. This real space approach allows to describe these processes in a unified way, showing its versatility and utility in the study of chemical systems in excited states. © 2017 Wiley Periodicals, Inc.

Keywords: conical intersections; electron density analysis; energy transfer; excited states; interacting quantum atoms.

Publication types

  • Research Support, Non-U.S. Gov't