A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels
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Upon adsorption of a molecule onto a surface, the molecular energy levels (MELs) broaden and change their alignment. This phenomenon directly affects electron transfer across the interface and is, therefore, a fundamental observable that influences electrochemical device performance. Here, we propose a rigorous parameter-free framework, built upon the theoretical construct of Green's functions, for studying the interface between a molecule and a bulk surface and its effect on MELs. The method extends beyond the usual wide-band limit approximation, and its generality allows its use with any level of electronic structure theory. We demonstrate its ability to predict the broadening and shifting of MELs as a function of intramolecular coupling, molecule/surface coupling, and the surface density of states for a molecule with two MELs adsorbed on a one-dimensional model metal surface. The new approach could help provide guidelines for the design and experimental characterization of electrochemical devices with optimal electron transport.
Originalsprog | Engelsk |
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Tidsskrift | Nano Letters |
Vol/bind | 22 |
Udgave nummer | 24 |
Sider (fra-til) | 9854–9860 |
Antal sider | 7 |
ISSN | 1530-6984 |
DOI | |
Status | Udgivet - 2022 |
ID: 332197572