Kinetics of electron-phonon scattering in silicon resolved by Rydberg transitions of donors

Abstract

Rydberg states of atoms in vacuum are now well recognized as a resource for quantum technologies. Donors in semiconductors also display analogous states, which have been proposed for similar applications. While they benefit from permanent locations in their host crystals, electron-lattice coupling leads to much shorter excited-state lifetimes than for neutral atoms in vacuum. Here we provide a quantitative description of donor-phonon kinetics, creating a basis for engineering donor systems in realistic material stacks for quantum devices. Our theory incorporates both form factors for the Rydberg states, which given their large extents in real space provide strong selectivity in momentum space, and tabulated deformation potentials for all six phonon branches throughout the Brillouin zone. By confronting this framework with carefully controlled time-resolved free electron laser measurements, we show that the widely quoted position of the silicon conduction band minimum, $k_0$, is inconsistent with observed donor relaxation rates and that quantitative agreement is obtained for a value further from the X-point than commonly assumed. This stringent experiment-theory comparison establishes donor relaxation as a precision metrology for conduction band parameters and scattering processes in silicon, with consequences spanning from quantum devices to classical electronics.