When Blinking Helps: Suppressed Biexciton Emission in Lead Halide Perovskite Quantum Dots
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arXiv
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| Autores principales: | , , , , |
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| Formato: | Preprint |
| Publicado: |
2026
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| _version_ | 1866915794125848576 |
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| author | Olejniczak, Adam Ryu, Jehyeok Di Stasio, Francesco Rakovich, Yury Krivenkov, Victor |
| author_facet | Olejniczak, Adam Ryu, Jehyeok Di Stasio, Francesco Rakovich, Yury Krivenkov, Victor |
| contents | 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 $g^{(2)}(τ)$ 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2602_11385 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | When Blinking Helps: Suppressed Biexciton Emission in Lead Halide Perovskite Quantum Dots Olejniczak, Adam Ryu, Jehyeok Di Stasio, Francesco Rakovich, Yury Krivenkov, Victor Mesoscale and Nanoscale Physics 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 $g^{(2)}(τ)$ 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. |
| title | When Blinking Helps: Suppressed Biexciton Emission in Lead Halide Perovskite Quantum Dots |
| topic | Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2602.11385 |