Detection of Single Charge Trapping Defects in Semiconductor Particles by Evaluating Photon Antibunching in Delayed...

Time-resolved analysis of photon cross-correlation function g⁽²⁾(τ) is applied to photoluminescence (PL) of individual submicrometer size MAPbI₃ perovskite crystals. Surprisingly, an antibunching effect in the long-living tail of PL is observed, while the prompt PL obeys the photon statistics typical for a classical emitter. We propose that antibunched photons from the PL decay tail originate from radiative recombination of detrapped charge carriers which were initially captured by a very limited number (down to one) of shallow defect states. The concentration of these trapping sites is estimated to be in the range 10¹³-10¹⁶ cm^-3. In principle, photon correlations can be also caused by highly nonlinear Auger recombination processes; however, in our case it requires unrealistically large Auger recombination coefficients. The potential of the time-resolved g⁽²⁾(0) for unambiguous identification of charge rerecombination processes in semiconductors considering the actual number of charge carries and defects states per particle is demonstrated.