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

ACS Nano. 2024 Apr 23;18(16):10807-10817. doi: 10.1021/acsnano.3c12311. Epub 2024 Apr 10.

Authors

Bo Wang¹, Jia Wei Melvin Lim¹, Siow Mean Loh², Rishikanta Mayengbam¹, Senyun Ye¹, Minjun Feng¹, Huajun He¹, Xiao Liang³, Rui Cai¹, Qiannan Zhang¹, Leong-Chuan Kwek^{4

5}, Hilmi Volkan Demir^{1

3

6}, Subodh G Mhaisalkar^{7

8}, Steven A Blundell², Tze Chien Sum¹

Affiliations

¹ Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore.
² Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, F-38000 Grenoble, France.
³ LUMINOUS! Center of Excellence for Semiconductor Lighting and Displays, The Photonics Institute, School of Electrical and Electronic Engineering, Nanyang Technological University, Singapore 639798, Singapore.
⁴ Centre for Quantum Technologies, National University of Singapore, Singapore 117543, on Singapore.
⁵ National Institute of Education, Nanyang Technological University, 1 Nanyang Walk Singapore 637616, Singapore.
⁶ UNAM─Institute of Materials Science and Nanotechnology, The National Nanotechnology Research Center, Department of Electrical and Electronics Engineering, Department of Physics, Bilkent University, Bilkent, Ankara 06800, Turkey.
⁷ School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
⁸ SKKU Institute of Energy Science and Technology (SIEST), Sungkyunkwan University, 2066 Seobu-ro, Jangan-gu, Suwon-si, Gyeonggi-do 440-746, Korea.

PMID: 38598660
DOI: 10.1021/acsnano.3c12311

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.

Keywords: Blinking behavior; Colloidal perovskite quantum dots; Single photon sources; Transient absorption spectroscopy; Weak confinement.