Hydrogen atom collisions with a semiconductor efficiently promote electrons to the conduction band

The Born-Oppenheimer approximation is the keystone of modern computational chemistry and there is wide interest in understanding under what conditions it remains valid. Hydrogen atom scattering from insulator, semi-metal and metal surfaces has helped provide such information. The approximation is adequate for insulators and for metals it fails, but not severely. Here we present hydrogen atom scattering from a semiconductor surface: Ge(111)c(2 x 8). Experiments show bimodal energy-loss distributions revealing two channels. Molecular dynamics trajectories within the Born-Oppenheimer approximation reproduce one channel quantitatively. The second channel transfers much more energy and is absent in simulations. It grows with hydrogen atom incidence energy and exhibits an energy-loss onset equal to the Ge surface bandgap. This leads us to conclude that hydrogen atom collisions at the surface of a semiconductor are capable of promoting electrons from the valence to the conduction band with high efficiency. Our current understanding fails to explain these observations.

Automated summary

The Born-Oppenheimer approximation is crucial in computational chemistry, but its validity under different conditions is still a topic of interest. Scattering experiments with hydrogen atoms on various surfaces have shed light on this matter. In this study, hydrogen atom scattering from a semiconductor surface revealed two channels, with one being accurately described by the Born-Oppenheimer approximation and the other showing a higher energy transfer that was not captured in simulations.