Highly pure single photon emission from single perovskite QDs

Chenglian Zhu^a^,^b, Malwina Marczak^a^,^b, Leon Feld^a^,^b, Simon C. Boehme^a^,^b, Caterina Bernasconi^a^,^b, Anastasiia Moskalenko^a^,^b, Ihor Cherniukh^a^,^b, Dmitry Dirin^a^,^b, Maryna I. Bodnarchuk^a^,^b, Maksym V. Kovalenko^a^,^b, Gabriele Raino^a^,^b

^aInstitute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland

^bLaboratory for Thin Films and Photovoltaics, Empa Swiss Federal Laboratories for Materials Science and Technology, 8600 Dübendorf, Suiza, Dübendorf, Switzerland

Proceedings of International Conference on Emerging Light Emitting Materials (EMLEM22)

Aspects of Emergent Light Emitters:

Limasol, Cyprus, 2022 October 3rd - 5th

Organizers: Maksym Kovalenko, Maryna Bodnarchuk and Grigorios Itskos

Oral, Chenglian Zhu, presentation 006
DOI: https://doi.org/10.29363/nanoge.emlem.2022.006
Publication date: 15th July 2022

Attaining pure single-photon emission is key for many quantum technologies,^[1] from optical quantum computing^[2] to quantum key distribution^[3] and quantum imaging.^[4] The past 20 years have seen the development of several solid-state quantum emitters, but most of them require highly sophisticated techniques (e.g., ultra-high vacuum growth methods and cryostats for low-temperature operation). The system complexity may be significantly reduced by employing quantum emitters capable of working at room temperature. Lead-halide perovskite APbX₃ (A=Cs or organic cation; X=Cl, Br, I) quantum dots (QDs) are one of the desired materials, of particular interest due to their low-cost synthesis, solution processability, tunability of the emission wavelength via size and composition, narrow-band emission, short radiative lifetime (~ns at RT) as well as high photoluminescence quantum yield (QY).^[5,6] Here, we present a systematic study across ∼ 170 photostable single CsPbX₃(X: Br and I) colloidal QDs of different sizes and compositions, unveiling that increasing quantum confinement is an effective strategy for maximizing single-photon purity due to the suppressed biexciton quantum yield. Leveraging the latter, we achieve 98% single-photon purity (g⁽²⁾(0) as low as 2%) from a cavity-free, non-resonantly excited single 6.6 nm CsPbI₃ QDs, showcasing the great potential of CsPbX₃ QDs as room-temperature highly pure single-photon sources for quantum technologies.

References:

[1] Aharonovich, I., Englund, D. & Toth, M. Solid-state single-photon emitters. Nature Photonics 10, 631-641 (2016).

[2] Wang, H.; Qin, J.; Ding, X.; Chen, M.-C.; Chen, S.; You, X.; He, Y.-M.; Jiang, X.; You, L.; Wang, Z. Boson sampling with 20 input photons and a 60-mode interferometer in a 1 0 14-dimensional hilbert space. Phys. Rev. Lett. 2019, 123 (25), 250503.

[3] Brassard, G.; Lütkenhaus, N.; Mor, T.; Sanders, B. C. Limitations on practical quantum cryptography. Phys. Rev. Lett. 2000, 85 (6), 1330.

[4] Tenne, R.; Rossman, U.; Rephael, B.; Israel, Y.; Krupinski-Ptaszek, A.; Lapkiewicz, R.; Silberberg, Y.; Oron, D. Super-resolution enhancement by quantum image scanning microscopy. Nature Photonics 2019, 13 (2), 116-122.

[5] Protesescu, L.; Yakunin, S.; Bodnarchuk, M. I.; Krieg, F.; Caputo, R.; Hendon, C. H.; Yang, R. X.; Walsh, A.; Kovalenko, M. V. Nanocrystals of cesium lead halide perovskites (CsPbX3, X= Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut. Nano Lett. 2015, 15, 3692-3696 (2015).

[6] Krieg, F.; Sercel, P. C.; Burian, M.; Andrusiv, H.; Bodnarchuk, M. I.; Stöferle, T.; Mahrt, R. F.; Naumenko, D.; Amenitsch, H.; Rainò, G. Monodisperse long-chain sulfobetaine-capped CsPbBr3 nanocrystals and their superfluorescent assemblies. ACS central science 7, 135-144 (2020).

Acknowledgements:

This project was funded by the Swiss National Science Foundation (SNSF Grant No. 200021_192308, “Q-Light- Engineered Quantum Light Sources with Nanocrystal Assemblies”). The project was also partially supported by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the Grant Agreement No. 899141 (PoLLoC), by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, and by SNSF Grant No. 200021_188404 (“Novel inorganic light emitters: synthesis, spectroscopy and applications”).

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