Electronic Structure for Multielectronic Molecules Near a Metal Surface

Abstract

We analyze a model problem representing a multi-electronic molecule sitting on a metal surface. Working with a reduced configuration interaction Hamiltonian, we show that one can extract very accurate ground state wavefunctions as compared with the numerical renormalization group theory (NRG) -- even in the limit of weak metal-molecule coupling strength but strong intramolecular electron-electron repulsion. Moreover, we extract what appear to be meaningful excitation energies as well. Our findings should lay the groundwork for future {\em ab initio} studies of charge transfer processes and bond making/breaking processes on metal surfaces.

References in corpus (5)

• Continuous-time Monte Carlo methods for quantum impurity models
• The numerical renormalization group method for quantum impurity systems
• Delta Self-Consistent Field as a method to obtain potential energy surfaces of excited molecules on surfaces
• Truncated Configuration Interaction expansions as solvers for correlated quantum impurity models and dynamical mean field theory
• PyCDFT: A Python package for constrained density functional theory