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Investigations that probe defects one at a time offer a unique opportunity toobserve properties and dynamics that are washed out of ensemble measurements.Here we present confocal fluorescence measurements of individual defects inAl-doped ZnO nanoparticles and undoped ZnO sputtered films that are excitedwith sub-bandgap energy light. Photon correlation measurements yield bothantibunching and bunching, indicative of single-photon emission from isolateddefects that possess a metastable shelving state. The single-photon emission isin the range 560 - 720 nm and typically exhibits two broad spectral peaksseparated by approximately 150 meV. The excited state lifetimes range from 1 -13 ns, consistent with the finite-size and surface effects of nanoparticles andsmall grains. We also observe discrete jumps in the fluorescence intensitybetween a bright state and a dark state. The dwell times in each state areexponentially distributed and the average dwell time in the bright (dark) statedoes (may) depend on the power of the exciting laser. Taken together, ourmeasurements demonstrate the utility of a single-molecule approach tosemiconductor defect studies and highlight ZnO as a potential host material forsingle-defect based applications.

A single-molecule approach to ZnO defect studies: single photons and single defects