Speaker
Description
Nonadiabatic energy dissipation is known to play a crucial role in
hyperthermal scattering at surfaces, leading to electron-hole pair ex-
citation and highly inelastic scattering. For projectiles with unpaired
spins, such as hydrogen atoms, hybridisation with the metal surface re-
sults in strong non-adiabatic effects driven by a phase transition in its
spin-polarisation. It is known that traditional mean-field descriptions
of the resultant nonadiabatic dynamics using methods like MDEF and
Ehrenfest dynamics break down in the presence of the transition, lead-
ing to divergent energy transfer rates and unphysical stopping powers
at the location of the spin transition [Box et al. J. Phys. Chem. Lett.
15, 51 (2024); Lindenblatt et al. Phys. Rev. Lett. 97 (2006)].
Here, we model H/Cu(111) and H/Ag(111) scattering in the pres-
ence of on-site correlation in the adsorbate state using the Newns-
Anderson Hamiltonian. We go beyond previous works by simulat-
ing the dynamics using stochastic trajectory surface hopping methods
that capture the coupling between the nuclear and electronic degrees
of freedom beyond the mean-field. We systematically classify scat-
tering regimes and assess the applicability of mean-field and beyond
mean-field methods for predicting the nonadiabatic energy loss in these
regimes.