Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.152
Publication date: 16th December 2024
Generating and manipulating non-classical light in the form of a stream of single photons is central to a broad range of emerging quantum-light applications, from quantum computing to quantum sensing and quantum imaging. In this talk, I will present recent advances in using colloidal lead-halide perovskite quantum dots (QDs) towards this end, with advantageous attributes such as spectral tunability, solution-processability, and scalability.
Sharing results from single-particle spectroscopy and ab-initio molecular-dynamics simulations, I will argue that the pronounced exciton-phonon coupling in perovskite QDs[1] is key to understanding and manipulating (multi)excitons in these materials. To illustrate this point, I will elaborate on the strikingly different photophysics in individual perovskite QDs at cryogenic and room temperature. At cryogenic temperature, perovskite QDs behave as textbox semiconductors, capable of cavity-free coherent quantum-light emission and hosting phenomena such as single-photon superradiance[2] and superabsorption.[3] The latter two concepts have both been proposed theoretically early on but evaded experimental demonstration until very recently. At room temperature, on the other hand, coupling of the exciton to large-amplitude lattice vibrations in the QD core and at the QD surface leads to pronounced emission broadening[4] and localization of the exciton wavefunction.[5] While the latter inevitably accelerates thermally activated decoherence processes, it can auspiciously be leveraged to increase single-photon purity, up to 98% for cavity-free, nonresonantly excited single perovskite QDs at room temperature.[6]
References:
[1] C. Zhu, et al., Adv. Optical Mater. 2024, 12, 2301534.
[2] C. Zhu, et al., Nature 2024, 626, 535–541.
[3] S.C. Boehme, et al., under review.
[4] G. Rainò, et al., Nat. Commun. 2022, 13, 2587.
[5] L.G. Feld, at al., DOI: 10.48550/arXiv.2404.15920.
[6] C. Zhu, et al., Nano Lett. 2022, 22, 3751–3760.
The project was supported by the European Union's Horizon 2020 program, through a FET Open research and innovation action under Grant Agreement No. 899141 (PoLLoC). This work was also supported by the Weizmann-ETH Zürich Bridge Program, by the Air Force Office of Scientific Research under award number FA8655-21-1 7013, by the Swiss National Science Foundation (Grant No. 200021_192308, "Q-Light-Engineered Quantum Light Sources with Nanocrystal Assemblies") and by the European Research Council (grant agreement No. 819740, SCALE-HALO).
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