Predicting the effect that an interacting environment has on the properties of molecules is vital. Typically, however, the electronic properties of molecules are solved in isolation via closed-system eigenvalue equations (e.g Kohn-Sham). Resulting states are discrete and have an infinite lifetime.<br/>In this work, the interacting environment is included with the Nonequilibrium Green's function method (NEGF). NEGF is widely accepted in physics as the most consistent method for solving quantum mechanical systems including environmental interactions. The notion of an interacting environment is exemplified on a single benzene molecule placed in water ice. The interaction strength of the benzene molecules with the ice environment are varied. Fig. 1 shows the density of electronic states for an isolated benzene molecule. Fig 2 shows increased interaction. As expected the benzene electrons stay within the benzene carbon atoms in Fig 1. When coupling is increased the electronic states spread out into the ice, the electrons are no longer pure benzene electrons and their lifetime becomes finite. Shifts and broadening of states in energy are observed, too. NEGF results of similar applications indicate that the speed of chemical reactions critically depends on this type of environmental state broadening.

Modeling molecules in an interacting environment

255th National Meeting (2018)

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