Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources

Bo Wang; Jia Wei Melvin Lim; Siow Mean Loh; Rishikanta Mayengbam; Senyun Ye; Minjun Feng; Huajun He; Xiao Liang; Rui Cai; Qiannan Zhang; Leong Chuan Kwek; Hilmi Volkan Demir; Subodh G. Mhaisalkar; Steven A. Blundell; Tze Chien Sum

doi:10.1021/acsnano.3c12311

Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources

Bo Wang, Jia Wei Melvin Lim, Siow Mean Loh, Rishikanta Mayengbam, Senyun Ye, Minjun Feng, Huajun He, Xiao Liang, Rui Cai, Qiannan Zhang, Leong Chuan Kwek, Hilmi Volkan Demir, Subodh G. Mhaisalkar, Steven A. Blundell, Tze Chien Sum^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

4 Citations (Scopus)

Abstract

Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr₃ QDs. However, this also increases the fluorescence intermittency. Achieving high SP purity and blinking mitigation simultaneously remains a significant challenge. Here, we transcend this limitation with room-temperature synthesized weakly confined hybrid organic-inorganic perovskite (HOIP) QDs. Superior single photon purity with a low g⁽²⁾(0) < 0.07 ± 0.03 and a nearly blinking-free behavior (ON-state fraction >95%) in 11 nm FAPbBr₃ QDs are achieved at room temperature, attributed to their long exciton lifetimes (τ_X) and short biexciton lifetimes (τ_XX). The significance of the organic A-cation is further validated using the mixed-cation FA_xCs_1-xPbBr₃. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k·p approaches point toward the modulation of the dielectric constants by the organic cations. Importantly, our findings provide valuable insights into an additional lever for engineering facile-synthesized room-temperature PQD single photon sources.

Original language	English
Pages (from-to)	10807-10817
Number of pages	11
Journal	ACS Nano
Volume	18
Issue number	16
DOIs	https://doi.org/10.1021/acsnano.3c12311
Publication status	Published - Apr 23 2024
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2024 American Chemical Society.

ASJC Scopus Subject Areas

General Materials Science
General Engineering
General Physics and Astronomy

Keywords

Blinking behavior
Colloidal perovskite quantum dots
Single photon sources
Transient absorption spectroscopy
Weak confinement

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10.1021/acsnano.3c12311

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Wang, B., Lim, J. W. M., Loh, S. M., Mayengbam, R., Ye, S., Feng, M., He, H., Liang, X., Cai, R., Zhang, Q., Kwek, L. C., Demir, H. V., Mhaisalkar, S. G., Blundell, S. A., & Chien Sum, T. (2024). Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources. ACS Nano, 18(16), 10807-10817. https://doi.org/10.1021/acsnano.3c12311

@article{0935460af4a84ff3b9591660421bb13e,

title = "Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources",

abstract = "Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr3 QDs. However, this also increases the fluorescence intermittency. Achieving high SP purity and blinking mitigation simultaneously remains a significant challenge. Here, we transcend this limitation with room-temperature synthesized weakly confined hybrid organic-inorganic perovskite (HOIP) QDs. Superior single photon purity with a low g(2)(0) < 0.07 ± 0.03 and a nearly blinking-free behavior (ON-state fraction >95%) in 11 nm FAPbBr3 QDs are achieved at room temperature, attributed to their long exciton lifetimes (τX) and short biexciton lifetimes (τXX). The significance of the organic A-cation is further validated using the mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k·p approaches point toward the modulation of the dielectric constants by the organic cations. Importantly, our findings provide valuable insights into an additional lever for engineering facile-synthesized room-temperature PQD single photon sources.",

keywords = "Blinking behavior, Colloidal perovskite quantum dots, Single photon sources, Transient absorption spectroscopy, Weak confinement",

author = "Bo Wang and Lim, {Jia Wei Melvin} and Loh, {Siow Mean} and Rishikanta Mayengbam and Senyun Ye and Minjun Feng and Huajun He and Xiao Liang and Rui Cai and Qiannan Zhang and Kwek, {Leong Chuan} and Demir, {Hilmi Volkan} and Mhaisalkar, {Subodh G.} and Blundell, {Steven A.} and {Chien Sum}, Tze",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

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doi = "10.1021/acsnano.3c12311",

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T1 - Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources

AU - Wang, Bo

AU - Lim, Jia Wei Melvin

AU - Loh, Siow Mean

AU - Mayengbam, Rishikanta

AU - Ye, Senyun

AU - Feng, Minjun

AU - He, Huajun

AU - Liang, Xiao

AU - Cai, Rui

AU - Zhang, Qiannan

AU - Kwek, Leong Chuan

AU - Demir, Hilmi Volkan

AU - Mhaisalkar, Subodh G.

AU - Blundell, Steven A.

AU - Chien Sum, Tze

PY - 2024/4/23

Y1 - 2024/4/23

N2 - Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr3 QDs. However, this also increases the fluorescence intermittency. Achieving high SP purity and blinking mitigation simultaneously remains a significant challenge. Here, we transcend this limitation with room-temperature synthesized weakly confined hybrid organic-inorganic perovskite (HOIP) QDs. Superior single photon purity with a low g(2)(0) < 0.07 ± 0.03 and a nearly blinking-free behavior (ON-state fraction >95%) in 11 nm FAPbBr3 QDs are achieved at room temperature, attributed to their long exciton lifetimes (τX) and short biexciton lifetimes (τXX). The significance of the organic A-cation is further validated using the mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k·p approaches point toward the modulation of the dielectric constants by the organic cations. Importantly, our findings provide valuable insights into an additional lever for engineering facile-synthesized room-temperature PQD single photon sources.

AB - Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr3 QDs. However, this also increases the fluorescence intermittency. Achieving high SP purity and blinking mitigation simultaneously remains a significant challenge. Here, we transcend this limitation with room-temperature synthesized weakly confined hybrid organic-inorganic perovskite (HOIP) QDs. Superior single photon purity with a low g(2)(0) < 0.07 ± 0.03 and a nearly blinking-free behavior (ON-state fraction >95%) in 11 nm FAPbBr3 QDs are achieved at room temperature, attributed to their long exciton lifetimes (τX) and short biexciton lifetimes (τXX). The significance of the organic A-cation is further validated using the mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k·p approaches point toward the modulation of the dielectric constants by the organic cations. Importantly, our findings provide valuable insights into an additional lever for engineering facile-synthesized room-temperature PQD single photon sources.

KW - Blinking behavior

KW - Colloidal perovskite quantum dots

KW - Single photon sources

KW - Transient absorption spectroscopy

KW - Weak confinement

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SN - 1936-0851

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EP - 10817

JO - ACS Nano

JF - ACS Nano

IS - 16

ER -

Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources

Abstract

Bibliographical note

ASJC Scopus Subject Areas

Keywords

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