Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources
Colloidal perovskite quantum dots (PQDs) emerge 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 SP purity in all-inorganic...
| Main Authors: | , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2024
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| Online Access: | https://hdl.handle.net/10356/175431 |
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| author | Wang, Bo Lim, Melvin Jia Wei Loh, Siow Mean Mayengbam, Rishikanta Ye, Senyun Feng, Minjun He, Huajun Liang, Xiao Cai, Rui Zhang, Qiannan Kwek, Leong Chuan Demir, Hilmi Volkan Mhaisalkar, Subodh Gautam Blundell, Steven A. Sum, Tze Chien |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Wang, Bo Lim, Melvin Jia Wei Loh, Siow Mean Mayengbam, Rishikanta Ye, Senyun Feng, Minjun He, Huajun Liang, Xiao Cai, Rui Zhang, Qiannan Kwek, Leong Chuan Demir, Hilmi Volkan Mhaisalkar, Subodh Gautam Blundell, Steven A. Sum, Tze Chien |
| author_sort | Wang, Bo |
| collection | NTU |
| description | Colloidal perovskite quantum dots (PQDs) emerge 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 SP purity in all-inorganic CsPbBr3 QDs. However, this also increases 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 low g^((2) ) (0)<0.07±0.03 and nearly blinking-free behaviour (ON-state fraction >95%) in 11 nm FAPbBr3 QDs is 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 mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k⋅p approaches point towards 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. |
| first_indexed | 2025-02-19T03:50:47Z |
| format | Journal Article |
| id | ntu-10356/175431 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-02-19T03:50:47Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1754312024-04-29T15:37:14Z Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources Wang, Bo Lim, Melvin Jia Wei Loh, Siow Mean Mayengbam, Rishikanta Ye, Senyun Feng, Minjun He, Huajun Liang, Xiao Cai, Rui Zhang, Qiannan Kwek, Leong Chuan Demir, Hilmi Volkan Mhaisalkar, Subodh Gautam Blundell, Steven A. Sum, Tze Chien School of Physical and Mathematical Sciences School of Electrical and Electronic Engineering School of Materials Science and Engineering LUMINOUS! Centre of Excellence for Semiconductor Lighting & Displays The Photonics Institute Physics Colloidal perovskite quantum dots Weak confinement Transient absorption spectroscopy Single photon sources Blinking behavior Colloidal perovskite quantum dots (PQDs) emerge 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 SP purity in all-inorganic CsPbBr3 QDs. However, this also increases 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 low g^((2) ) (0)<0.07±0.03 and nearly blinking-free behaviour (ON-state fraction >95%) in 11 nm FAPbBr3 QDs is 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 mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k⋅p approaches point towards 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. Ministry of Education (MOE) Nanyang Technological University National Research Foundation (NRF) Submitted/Accepted version This research/project is supported by Nanyang Technological University under its NTUitive Gap Fund (NGF-2022-11-018) and LUX Photonics Consortium Industry-IHL Collaboration Seed grant award (2022LUX02P01), the Ministry of Education under its AcRF Tier 2 grant (MOE-T2EP50120-0004); and the National Research Foundation (NRF) Singapore under its NRF Investigatorship (NRF-NRFI2018-04) and the Competitive Research Programme (NRF-CRP25-2020-0004). T.C.S also acknowledges the support from the Institute for Digital Molecular Analytics and Science (IDMxS) under the Singapore Ministry of Education Research Centres of Excellence scheme. S.A.B. and S.M.L. are grateful to the French CEA’s program PTC-Matériaux et Procédés for support, and to DARI-TGCC for computing resources under project AD010914220. The computational work for this article was also partially performed on resources of the National Supercomputing Centre (NSCC), Singapore (https://www.nscc.sg). H.V.D. and X.L. acknowledge the support received from Singapore Agency for Science, Technology and Research (A*STAR) MTC program (Grant No. M21J9b0085). H.V.D. also gratefully acknowledges support from TUBA. 2024-04-24T05:51:01Z 2024-04-24T05:51:01Z 2024 Journal Article Wang, B., Lim, M. J. W., 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. & Sum, T. C. (2024). Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources. ACS Nano, 18(16), 10807-10817. https://dx.doi.org/10.1021/acsnano.3c12311 1936-0851 https://hdl.handle.net/10356/175431 10.1021/acsnano.3c12311 16 18 10807 10817 en NGF-2022-11-018 2022LUX02P01 MOE-T2EP50120-0004 NRF-NRFI2018-04 NRF-CRP25-2020-0004 AD010914220 M21J9b0085 ACS Nano 10.21979/N9/ZOTDKX © 2024 American Chemical Society. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1021/acsnano.3c12311. application/pdf application/pdf |
| spellingShingle | Physics Colloidal perovskite quantum dots Weak confinement Transient absorption spectroscopy Single photon sources Blinking behavior Wang, Bo Lim, Melvin Jia Wei Loh, Siow Mean Mayengbam, Rishikanta Ye, Senyun Feng, Minjun He, Huajun Liang, Xiao Cai, Rui Zhang, Qiannan Kwek, Leong Chuan Demir, Hilmi Volkan Mhaisalkar, Subodh Gautam Blundell, Steven A. Sum, Tze Chien Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources |
| title | Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources |
| title_full | Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources |
| title_fullStr | Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources |
| title_full_unstemmed | Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources |
| title_short | Weakly confined organic–inorganic halide perovskite quantum dots as high-purity room-temperature single photon sources |
| title_sort | weakly confined organic inorganic halide perovskite quantum dots as high purity room temperature single photon sources |
| topic | Physics Colloidal perovskite quantum dots Weak confinement Transient absorption spectroscopy Single photon sources Blinking behavior |
| url | https://hdl.handle.net/10356/175431 |
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