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

Eremchev, Ivan Yu; Tarasevich, Aleksandr O; Kniazeva, Maria A; Li, Jun; Naumov, Andrei V; Scheblykin, Ivan G · Nano Lett · 2023

basic_science · Level V

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Abstract

Time-resolved analysis of photon cross-correlation function <i>g</i><sup>(2)</sup>(τ) is applied to photoluminescence (PL) of individual submicrometer size MAPbI<sub>3</sub> 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 10<sup>13</sup>-10<sup>16</sup> cm<sup>-3</sup>. 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 <i>g</i><sup>(2)</sup>(0) for unambiguous identification of charge rerecombination processes in semiconductors considering the actual number of charge carries and defects states per particle is demonstrated.