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Compact spin-valley-locked perovskite emission

Nature Materials volume 22, pages 1065–1070 (2023)Cite this article

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Abstract

Circularly polarized light sources with free-space directional emission play a key role in chiroptics1, spintronics2, valleytronics3 and asymmetric photocatalysis4. However, conventional approaches fail to simultaneously realize pure circular polarization, high directionality and large emission angles in a compact emitter. Metal-halide perovskite semiconductors are promising light emitters5,6,7,8, but the absence of an intrinsic spin-locking mechanism results in poor emission chirality. Further, device integration has undermined the efficiency and directionality of perovskite chiral emitters. Here we realize compact spin-valley-locked perovskite emitting metasurfaces where spin-dependent geometric phases are imparted into bound states in the continuum via Brillouin zone folding, and thus, photons with different spins are selectively addressed to opposite valleys. Employing this approach, chiral purity of 0.91 and emission angle of 41.0° are simultaneously achieved, with a beam divergence angle of 1.6°. With this approach, we envisage the realization of chiral light-emitting diodes, as well as the on-chip generation of entangled photon pairs.

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Fig. 1: Spin-valley-locked emission in perovskite metasurfaces.
Fig. 2: Spontaneous emission properties of perovskite metasurfaces.
Fig. 3: Spin-valley-locked lasing measured in perovskite metasurfaces.
Fig. 4: Perovskite lasing with tunable valleys and polarizations.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request. The raw data are available via the repository at https://figshare.com/articles/dataset/Raw_data_for_NM22061931A/22226455.

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Acknowledgements

We thank Prof. L. Jiang for the constructive discussions on perovskite assembly. Q.X. gratefully acknowledges funding support from the National Natural Science Foundation of China (no. 12020101003 and no. 92250301) and strong support from the State Key Laboratory of Low-Dimensional Quantum Physics at Tsinghua University. R.S. gratefully acknowledges funding support from the Nanyang Technological University via a Nanyang Assistant Professorship start-up grant and the Singapore Ministry of Education via the AcRF Tier 3 programme ‘Geometrical Quantum Materials’ (MOE2018-T3-1-002). Y.C. acknowledges support from the National Natural Science Foundation of China (no. 62275241). Y. Hou acknowledges support from the National University of Singapore (NUS) Presidential Young Professorship (A-0009174-03-00 and A-0009174-02-00). Y. Hou also acknowledges financial support from SERIS, which is a research institute supported by NUS, the National Research Foundation Singapore (NRF), the Energy Market Authority of Singapore (EMA) and the Singapore Economic Development Board (EDB). C.-W.Q. acknowledges financial support from the National Research Foundation, Prime Minister’s Office, Singapore, under Competitive Research Program Award NRF-CRP22-2019-0006. C.-W.Q. is also supported by a grant (R-261-518-004-720|A-0005947-16-00) from the Advanced Research and Technology Innovation Centre (ARTIC), NUS. Y. Huang acknowledges financial support from the Knut and Alice Wallenberg Foundation (KAW).

Author information

Author notes

  1. Yang Chen

    Present address: Chinese Academy of Sciences Key Laboratory of Mechanical Behavior and Design of Materials, Department of Precision Machinery and Precision Instrumentation, University of Science and Technology of China, Hefei, People’s Republic of China

  2. Jiangang Feng

    Present address: Department of Electrical and Computer Engineering, National University of Singapore, Singapore, Singapore

  3. These authors contributed equally: Yang Chen, Jiangang Feng, Yuqing Huang.

Authors and Affiliations

  1. Department of Electrical and Computer Engineering, National University of Singapore, Singapore, Singapore

    Yang Chen, Weijin Chen & Cheng-Wei Qiu

  2. Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, Singapore

    Jiangang Feng, Yuqing Huang & Rui Su

  3. Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, Sweden

    Yuqing Huang

  4. Beijing Academy of Quantum Information Sciences, Beijing, People’s Republic of China

    Sanjib Ghosh & Qihua Xiong

  5. Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, Singapore

    Yi Hou

  6. Solar Energy Research Institute of Singapore (SERIS), National University of Singapore, Singapore, Singapore

    Yi Hou

  7. State Key Laboratory of Low-Dimensional Quantum Physics and Department of Physics, Tsinghua University, Beijing, People’s Republic of China

    Qihua Xiong

  8. Frontier Science Center for Quantum Information, Beijing, People’s Republic of China

    Qihua Xiong

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Contributions

Y.C., Q.X. and C.-W.Q. conceived the idea. Y.C. designed the metasurfaces and conducted the simulations, and J.F. designed the experiments. J.F. and Q.X. oversaw and conducted the nanofabrication, perovskite assembly and optical spectroscopy measurements. Y. Huang developed the theoretical model and analysis. R.S. and Y. Hou provided support on sample synthesis and optical measurements. W.C. and S.G. provided support on simulation. Y.C. and J.F. analysed the data. Y.C., J.F., Y. Huang, Q.X. and C.-W.Q. drafted the paper with inputs from all the authors. Q.X. and C.-W.Q. supervised the project.

Corresponding authors

Correspondence to Jiangang Feng, Qihua Xiong or Cheng-Wei Qiu.

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Nature Materials thanks Makhsud Saidaminov and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Sections 1–8, Figs. 1–13 and Table 1.

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Chen, Y., Feng, J., Huang, Y. et al. Compact spin-valley-locked perovskite emission. Nat. Mater. 22, 1065–1070 (2023). https://doi.org/10.1038/s41563-023-01531-2

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