First-Principles Study of Hot Electron Dynamics on Silicon Quantum Dot-Molecule System*

Controlling hot carriers in nanomaterials is an active area of research, central to various optoelectronic applications. In our previous work¹, a short-lived hot electron transfer from a hydrogen-terminated Si(111) surface to the cyanidin molecule was observed during hot electron relaxation within the conduction manifold of the silicon, followed by interfacial electron transfer of picosecond timescale. We expand this study onto a silicon quantum dot attached to a cyanidin molecule to investigate the extent to which these observations change. Hot electron dynamics are investigated using first-principles simulation based on fewest switches surface hopping method combined with first-principles molecular dynamics and GW calculation.

(1) L. Li, Y. Kanai, J. Phys. Chem. Lett. 7, 1495 (2016).