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Halide perovskites enable polaritonic XY spin Hamiltonian at room temperature

Nature Materials volume 21, pages 761–766 (2022)Cite this article

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Abstract

Exciton polaritons, the part-light and part-matter quasiparticles in semiconductor optical cavities, are promising for exploring Bose–Einstein condensation, non-equilibrium many-body physics and analogue simulation at elevated temperatures. However, a room-temperature polaritonic platform on par with the GaAs quantum wells grown by molecular beam epitaxy at low temperatures remains elusive. The operation of such a platform calls for long-lifetime, strongly interacting excitons in a stringent material system with large yet nanoscale-thin geometry and homogeneous properties. Here, we address this challenge by adopting a method based on the solution synthesis of excitonic halide perovskites grown under nanoconfinement. Such nanoconfinement growth facilitates the synthesis of smooth and homogeneous single-crystalline large crystals enabling the demonstration of XY Hamiltonian lattices with sizes up to 10 × 10. With this demonstration, we further establish perovskites as a promising platform for room temperature polaritonic physics and pave the way for the realization of robust mode-disorder-free polaritonic devices at room temperature.

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Fig. 1: Synthesis and characterization of single-crystalline excitonic halide perovskites in DBR nanocavities.
Fig. 2: Room-temperature demonstration of polariton XY Hamiltonian square 2 × 2 lattices.
Fig. 3: Extended polariton lattices.

Data availability

The authors declare that the main data supporting the findings of this study are available within the paper. Extra data are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

We thank P. James Schuck and F. Xue for reading the manuscript and valuable comments and A. Gao from SVOTEK Inc. for assisting with the high-quality DBR mirror coating. W.B. and K.P. acknowledge support from the Office of Naval Research (award no. N00014-21-1-2099) and National Science Foundation (award no. OIA-2044049). W.B. thanks the CAREER support from the National Science Foundation (award no. DMR-2143041). X.Z. and R.T. thank the support by the Gordon and Betty Moore Foundation (award no. 5722) and the Ernest S. Kuh Endowed Chair Professorship. S.K.-C. and L.H. acknowledge funding from the Canada Research Chairs programme and the Army Research Office (W911NF1810149). The work of Q.L. and G.R.F. was supported by the US Department of Energy, Office of Science, Basic Energy Science, Chemical Sciences, Geosciences, and Biosciences Division. Use of the Center for Nanoscale Materials, a US Department of Energy Office of Science User Facility, was supported by the US Department of Energy, Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357.

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Author notes

  1. These authors contributed equally: Renjie Tao, Kai Peng

Authors and Affiliations

  1. Nanoscale Science and Engineering Center, University of California, Berkeley, CA, USA

    Renjie Tao & Xiang Zhang

  2. Department of Electrical and Computer Engineering, University of Nebraska-Lincoln, Lincoln, NE, USA

    Kai Peng & Wei Bao

  3. Department of Engineering Physics, École Polytechnique de Montréal, Montréal, Quebec, Canada

    Louis Haeberlé & Stéphane Kéna-Cohen

  4. Department of Chemistry, University of California, Berkeley, CA, USA

    Quanwei Li & Graham R. Fleming

  5. Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA

    Dafei Jin

  6. Faculty of Science and Faculty of Engineering, The University of Hong Kong, Hong Kong, China

    Xiang Zhang

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Contributions

W.B., X.Z., R.T. and K.P. initiated the project and conceived the experiments. R.T. fabricated the microcavities and grew and characterized the perovskite materials. K.P. performed all optical measurements except lifetime characterizations. Q.L. and G.R.F. performed the PL lifetime experiments. S.K.-C., D.J. and L.H. provided valuable insight and suggestions. W.B. and X.Z. supervised the whole project. R.T., K.P. and W.B. prepared the initial draught of the manuscript. K.P., W.B., R.T. and X.Z. led the efforts in revising the manuscript with the other authors’ participation.

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Correspondence to Xiang Zhang or Wei Bao.

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Nature Materials thanks Natalia Berloff, Hui Deng and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–27 and text.

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Source Data Fig. 1

Raw data for plot and fitting in Fig. 1.

Source Data Fig. 2

Raw data for plot and fitting in Fig. 2a.

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Tao, R., Peng, K., Haeberlé, L. et al. Halide perovskites enable polaritonic XY spin Hamiltonian at room temperature. Nat. Mater. 21, 761–766 (2022). https://doi.org/10.1038/s41563-022-01276-4

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