Electronic structure calculations in arbitrary electrostatic environments
Abstract
Modeling of electronic structure of molecules in electrostatic environments is of considerable relevance for surface-enhanced spectroscopy and molecular electronics. We have developed and implemented a novel approach to the molecular electronic structure in arbitrary electrostatic environments that is compatible with standard quantum chemical methods and can be applied to medium-sized and large molecules. The scheme denoted CheESE (chemistry in electrostatic environments) is based on the description of molecular electronic structure subject to a boundary condition on the system/environment interface. Thus, it is particularly suited to study molecules on metallic surfaces. The proposed model is capable of describing both electrostatic effects near nanostructured metallic surfaces and image-charge effects. We present an implementation of the CheESE model as a library module and show example applications to neutral and negatively charged molecules.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jan 09, 2012
- Source ID
- 10.1063/1.3670417
Entities
People
- Alán Aspuru-Guzik
- Dmitrij Rappoport
- Elizabeth M. Y. Lee
- Mark A. Watson
- Roberto Olivares-amaya
Organizations
- Defense Advanced Research Projects Agency
- Harvard University
- National Science Foundation