Pseudo-particle approach for charge-transferring molecule-surface collisions

TL;DR

This paper introduces a pseudo-particle method based on a generalized Anderson-Newns model to analyze charge transfer and electron emission during molecule-surface collisions, capturing resonant and Auger processes simultaneously.

Contribution

It develops a novel pseudo-particle framework combined with non-equilibrium Green functions to model complex charge transfer phenomena in molecule-surface interactions.

Findings

Resonant tunneling significantly reduces Auger contributions to electron emission.

The model predicts electron spectra and secondary emission coefficients accurately.

Both charge transfer channels are effectively treated on equal footing.

Abstract

Based on a semi-empirical generalized Anderson-Newns model we construct a pseudo-particle description for electron emission due to de-excitation of metastable molecules at surfaces. The pseudo-particle approach allows us to treat resonant charge-transfer and Auger processes on an equal footing, as it is necessary when both channels are open. This is for instance the case when a metastable nitrogen molecule hits a diamond surface. Using non-equilibrium Green functions and physically motivated approximations to the self-energies of the Dyson equations we derive a system of rate equations for the probabilities with which the metastable molecule, the molecular ground state, and the negative ion can be found in the course of the scattering event. From the rate equations we also obtain the spectrum of the emitted electron and the secondary electron emission coefficient. Our numerical results indicate the resonant tunneling process undermining the source of the Auger channel which therefore contributes only a few percent to the secondary electron emission.