Semiconductor nanocrystals (NCs) have bright, narrow, and tunable emission across the visible and infrared. However, fundamental insight into NC photophysics is incomplete. At single-particle scales, NCs undergo fluorescence intermittency whereby photon emission switches between ON and OFF states with erratic kinetics. The range of timescales relevant to the excitonic lifecyle adds to the challenge of spectroscopically distinguishing between proposed mechanisms. Here, we demonstrate all-optical modulation of blinking statistics and discover that sub-bandgap light perturbs ON-times of NCs in a timescale-free manner. On the ensemble scale, NCs possess advantages when sensitizing spin-triplet states of surface-bound molecules for excitonic upconversion. In the energy transfer step, it remains unclear whether correlated transfer is outpaced by sequential electron transfer. Using tailored NC synthesis, we observe rich spectroscopic dynamics including the pervasive role of surface states.
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