Breaking the Phonon Bottleneck for Holes in Semiconductor Quantum Dots

Size dependent hole dynamics are measured in colloidal CdSe quantum dots for a specific state-to-state excitonic transition. These experiments show that the hole energy loss rate increases for smaller quantum dots, contradicting known relaxation mechanisms for holes. These experiments reveal a new mechanism for hole relaxation in colloidal quantum dots which circumvents the expected phonon bottleneck for holes. The data are consistent with a nonadiabatic surface channel as the dominant pathway for hole relaxation in colloidal semiconductor quantum dots.