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Surface scattering

Mysterious energy losses

Nature Chemistry volume 15, pages 301–302 (2023)Cite this article

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The adiabatic approximation is often applied to describe the scattering of molecules or atoms from solid surfaces. Now, unusual energy loss has been observed during the scattering of hyperthermal hydrogen atoms from a single crystalline Ge(111) surface — suggesting the existence of a non-adiabatic mechanism involving electronic interband transitions in the Ge that are induced by the hydrogen atoms.

Introduced by Born and Oppenheimer more than 100 years ago, the adiabatic approximation is regularly applied to describe scattering and reactions of molecules or atoms at solid surfaces. It assumes that the electronic system stays in the lowest-energy ground state while the reactants interact1, and it is plausible because nuclear motion is slow on the electronic timescale of excitation and relaxation. The approximation allows intuitive models of potential energy surfaces or landscapes — including activation barriers or energy minima — and it is the implicit prerequisite of standard molecular dynamics (MD) calculations. In many surface-scattering processes, electronic excitations can be neglected and the validity of the adiabatic approximation has been successfully demonstrated. However, there is also clear experimental evidence that electrons are excited in rapid surface reactions or scattering events via the observation of chemiluminescence, exo-electron emission into vacuum, internal hot-charge-carrier chemicurrents, or in scattering cross-sections that cannot be described with adiabatic models2.

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Fig. 1: Energy transfer during scattering of hyperthermal H atoms from Ge(111)c(2 × 8).

References

  1. Born, M. & Oppenheimer, R. Ann. Phys. 389, 457–484 (1927).

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  2. Lundqvist, B. I. et al. Handbook of Surface Science Vol. 3 (eds Hasselbrink, E. & Lundqvist, B. I) 429 (Elsevier, 2008).

  3. Krüger, K. et al. Nat. Chem. https://doi.org/10.1038/s41557-022-01085-x (2022).

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  1. Experimental Physics, University of Duisburg-Essen, Duisburg, Germany

    Hermann Nienhaus

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  1. Hermann Nienhaus
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Correspondence to Hermann Nienhaus.

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Nienhaus, H. Mysterious energy losses. Nat. Chem. 15, 301–302 (2023). https://doi.org/10.1038/s41557-023-01145-w

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