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Room-temperature coherent optical manipulation of hole spins in solution-grown perovskite quantum dots

Nature Nanotechnology volume 18, pages 124–130 (2023)Cite this article

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Abstract

Manipulation of solid-state spin coherence is an important paradigm for quantum information processing. Current systems either operate at very low temperatures or are difficult to scale up. Developing low-cost, scalable materials whose spins can be coherently manipulated at room temperature is thus highly attractive for a sustainable future of quantum information science. Here we report ambient-condition all-optical initialization, manipulation and readout of hole spins in an ensemble of solution-grown CsPbBr3 perovskite quantum dots with a single hole in each dot. The hole spins are initialized by sub-picosecond electron scavenging following circularly polarized femtosecond-pulse excitation. A transverse magnetic field induces spin precession, and a second off-resonance femtosecond-pulse coherently rotates hole spins via strong light–matter interaction. These operations accomplish near-complete quantum-state control, with a coherent rotation angle close to the π radian, of hole spins at room temperature.

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Fig. 1: System design and experimental set-up.
Fig. 2: Room-temperature hole spin precession in AQ-functionalized CsPbBr3 QDs.
Fig. 3: Ultrafast rotation using the OSE.
Fig. 4: Room-temperature hole spin manipulation in AQ-functionalized CsPbBr3 QDs.

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Data availability

All data are available in the main text or Supplementary Information and can be obtained upon request from the corresponding author. The data are also available via Figshare at https://figshare.com/articles/figure/Data_for_Room-temperature_coherent_optical_manipulation_of_hole_spins_in_solution-grown_perovskite_quantum_dots_/21378075. Source data are provided with this paper.

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Acknowledgements

K.W. acknowledges financial support from the Chinese Academy of Sciences (grant number YSBR-007), the Ministry of Science and Technology of China (grant number 2018YFA0208703), the National Natural Science Foundation of China (grant number 22173098) and the Dalian Institute of Chemical Physics (grant number DICP I202106).

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Authors and Affiliations

  1. State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, China

    Xuyang Lin, Yaoyao Han, Jingyi Zhu & Kaifeng Wu

  2. University of Chinese Academy of Sciences, Beijing, China

    Xuyang Lin, Yaoyao Han & Kaifeng Wu

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Contributions

K.W. conceived the idea and designed the project. X.L. and Y.H. synthesized the samples, performed the spectroscopy with the help of J.Z. and analysed the data. K.W. wrote the manuscript with input from all authors. X.L. and Y.H. contributed equally to this work.

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Correspondence to Kaifeng Wu.

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Lin, X., Han, Y., Zhu, J. et al. Room-temperature coherent optical manipulation of hole spins in solution-grown perovskite quantum dots. Nat. Nanotechnol. 18, 124–130 (2023). https://doi.org/10.1038/s41565-022-01279-x

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