Ultrafast stimulated emission microscopy of single nanocrystals

Single-molecule detection is a powerful method used to distinguish different species and follow time trajectories within the ensemble average. However, such detection capability requires efficient emitters and is prone to photobleaching, and the slow, nanosecond spontaneous emission process only reports on the lowest excited state. We demonstrate direct detection of stimulated emission from individual colloidal nanocrystals at room temperature while simultaneously recording the depleted spontaneous emission, enabling us to trace the carrier population through the entire photocycle. By capturing the femtosecond evolution of the stimulated emission signal, together with the nanosecond fluorescence, we can disentangle the ultrafast charge trajectories in the excited state and determine the populations that experience stimulated emission, spontaneous emission, and excited-state absorption processes.