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Room-temperature electrically switchable spin–valley coupling in a van der Waals ferroelectric halide perovskite with persistent spin helix

Nature Photonics volume 16, pages 529–537 (2022)Cite this article

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Abstract

Spintronic devices, by harnessing the spin degree of freedom, are expected to outperform charge-based devices in terms of energy efficiency and speed of operation. The use of an electric field to control spin at room temperature has been pursued for decades. A major hurdle that has contributed to the slow progress in this regard is the dilemma between effective control and strong spin relaxation. For example, in a Rashba/Dresselhaus material with strong spin–orbit coupling, although the internal magnetic field could be substantial enough to effectively control spin precession, often, the spin-relaxation time becomes extremely short as a consequence of Dyakonov–Perel scattering. To address this, a persistent spin helix has been proposed in systems with SU(2) symmetry. Here we show the discovery of the persistent spin helix in an organic–inorganic hybrid ferroelectric halide perovskite whose layered nature makes it intrinsically like a quantum well. We demonstrate that the spin-polarized band structure is switchable at room temperature via an intrinsic ferroelectric field. We reveal valley–spin coupling through a circular photogalvanic effect in single-crystalline bulk crystals. The favoured short spin helix wavelength (three orders of magnitude shorter than in III–V materials), room-temperature operation and non-volatility make the hybrid perovskite an ideal platform for understanding symmetry-tuned spin dynamics, towards designing practical spintronic materials and devices that can resolve the control-relaxation dilemma.

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Fig. 1: The proposal of natural multilayer quantum-well-like bulk crystals with persistent spin helix.
Fig. 2: Theoretically calculated spin and effective magnetic field structures of (4,4-DFPD)2PbI4 predicted to host the persistent spin helix.
Fig. 3: Structural and optical properties of (4,4-DFPD)2PbI4.
Fig. 4: Light helicity-dependent photocurrent.
Fig. 5: Room-temperature ferroelectrically switchable CPGE.

Data availability

The data supporting the findings of this study are available within the paper.

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Codes are available upon reasonable request from the corresponding authors.

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Acknowledgements

This work is supported by the US ARO under grant no. W911NF-21-1-0013 (J.S. and R.S.), the US AFOSR under award no. FA9550-18-1-0116 (J.S.), the US AFOSR under award no. FA9550-YR-1-XYZQ (Y.P.), the New York State’s Empire State Development’s Division of Science, Technology and Innovation through Focus Center contract no. C180117 (L.Z., J.S., Z.L. and T.M.L.) and the US National Science Foundation under award nos. 1706815 (J.S.), 2031692 (J.S.) and 1916652 (R.S. and J.S.).

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Author notes

  1. These authors contributed equally: Lifu Zhang, Jie Jiang, Christian Multunas.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, Troy, NY, USA

    Lifu Zhang, Jie Jiang, Christian Multunas, Zhizhong Chen, Yang Hu, Saloni Pendse, Ru Jia, Mani Chandra, Ravishankar Sundararaman & Jian Shi

  2. Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute, Troy, NY, USA

    Christian Multunas, Zonghuan Lu & Toh-Ming Lu

  3. State Key Lab of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, People’s Republic of China

    Chen Ming & Yi-Yang Sun

  4. Department of Chemistry and Biochemistry, University of California, Santa Cruz, CA, USA

    Yuan Ping

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Contributions

J.S., R.S., Y.P. and L.Z. conceived and developed the idea. L.Z., Y.H., J.J. and J.S. planned the experiments. L.Z. and J.J. prepared samples and devices. L.Z. and J.J. performed optical and PL experiments. L.Z. performed ferroelectric polarization tests and SEM studies. L.Z. and J.J. performed CPGE measurements. C. Multunas, M.C., R.S., Y.P., C. Ming and Y.-Y.S. performed DFT calculations. Y.H. performed XRD and Z.L. performed EBSD. L.Z. processed the raw data. L.Z., C. Multunas, Y.P., R.S. and J.S. analysed and interpreted the results. L.Z. prepared the initial manuscript draft and J.S. revised it. All authors were involved in the discussion of data analysis and the writing of the manuscript. J.S., R.S. and Y.P. supervised the project.

Corresponding authors

Correspondence to Yuan Ping, Ravishankar Sundararaman or Jian Shi.

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Nature Photonics thanks Jean Luc Pelouard and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Zhang, L., Jiang, J., Multunas, C. et al. Room-temperature electrically switchable spin–valley coupling in a van der Waals ferroelectric halide perovskite with persistent spin helix. Nat. Photon. 16, 529–537 (2022). https://doi.org/10.1038/s41566-022-01016-9

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