When Blinking Helps: Suppressed Biexciton Emission in Lead Halide Perovskite Quantum Dots

TL;DR

This study uncovers a novel blinking regime in lead halide perovskite quantum dots where dark states enhance single-photon purity by suppressing biexciton emission through a self-trapped-exciton mechanism, challenging conventional blinking models.

Contribution

It introduces a new understanding of blinking behavior in PQDs, demonstrating that dark states can improve single-photon purity via STE-mediated suppression of biexcitons.

Findings

Dark states exhibit higher single-photon purity than bright states.

Biexciton emission is suppressed by a factor of ~10 in dark states.

Single-photon purity improves with $g^{(2)}_0$ decreasing from 0.155 to 0.120.

Abstract

Blinking and multiphoton emission in metal halide perovskite quantum dots (PQDs) limit their use as single-photon quantum emitters. Conventional models distinguish between trion-related A-type blinking and defect-assisted BC-type blinking, both expected to degrade single-photon purity in a dark state. Here, time-resolved spectroscopy on individual PQDs reveals a qualitatively different regime in which low emitting dark states exhibit higher single-photon purity than bright states. For those PQDs state-resolved $g^{(2)}(\tau)$ analysis shows that the exciton photoluminescence quantum yield decreases by a factor of $\sim 8$, while the biexciton one is suppressed by a factor of $\sim 10$. This leads to a moderate improvement of single-photon purity with $g^{(2)}_0$ decreased from 0.155 to 0.120. In contrast, PQDs with fluorescence lifetime--intensity distribution patterns characteristic for A-type blinking, display the expected increase of $g^{(2)}_0$ in charged, trion-dominated states. To explain the observed improvement of single-photon purity of low-emitting dark states, we propose a self-trapped-exciton (STE) mechanism that selectively blocks biexciton formation by diverting hot excitons into long-lived, weakly emissive STE configurations. This STE-mediated blinking channel explains why certain low-emitting states improve, rather than degrade, single-photon purity and suggests a lattice-driven route to perovskite quantum emitters with intrinsically suppressed multiphoton events.