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Title: Zero-field quantum beats and spin decoherence mechanisms in CsPbBr₃ perovskite nanocrystals
Authors: Cai, Rui
Wadgaonkar, Indrajit
Lim, Melvin Jia Wei
Dal Forno, Stefano
Giovanni, David
Feng, Minjun
Ye, Senyun
Battiato, Marco
Sum, Tze Chien
Keywords: Science::Physics
Issue Date: 2023
Source: Cai, R., Wadgaonkar, I., Lim, M. J. W., Dal Forno, S., Giovanni, D., Feng, M., Ye, S., Battiato, M. & Sum, T. C. (2023). Zero-field quantum beats and spin decoherence mechanisms in CsPbBr₃ perovskite nanocrystals. Nature Communications, 14(1), 2472-.
Project: MOE2019-T2-1-006 
Journal: Nature Communications 
Abstract: Coherent optical manipulation of exciton states provides a fascinating approach for quantum gating and ultrafast switching. However, their coherence time for incumbent semiconductors is highly susceptible to thermal decoherence and inhomogeneous broadening effects. Here, we uncover zero-field exciton quantum beating and anomalous temperature dependence of the exciton spin lifetimes in CsPbBr3 perovskite nanocrystals (NCs) ensembles. The quantum beating between two exciton fine-structure splitting (FSS) levels enables coherent ultrafast optical control of the excitonic degree of freedom. From the anomalous temperature dependence, we identify and fully parametrize all the regimes of exciton spin depolarization, finding that approaching room temperature, it is dominated by a motional narrowing process governed by the exciton multilevel coherence. Importantly, our results present an unambiguous full physical picture of the complex interplay of the underlying spin decoherence mechanisms. These intrinsic exciton FSS states in perovskite NCs present fresh opportunities for spin-based photonic quantum technologies.
ISSN: 2041-1723
DOI: 10.1038/s41467-023-37721-4
DOI (Related Dataset): 10.21979/N9/GEBAP3
Schools: School of Physical and Mathematical Sciences 
Interdisciplinary Graduate School (IGS) 
Research Centres: Energy Research Institute @ NTU (ERI@N) 
Rights: © 2023 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit licenses/by/4.0/.
Fulltext Permission: open
Fulltext Availability: With Fulltext
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