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Interlayer electronic coupling on demand in a 2D magnetic semiconductor

Abstract

When monolayers of two-dimensional (2D) materials are stacked into van der Waals structures, interlayer electronic coupling can introduce entirely new properties, as exemplified by recent discoveries of moiré bands that host highly correlated electronic states and quantum dot-like interlayer exciton lattices. Here we show the magnetic control of interlayer electronic coupling, as manifested in tunable excitonic transitions, in an A-type antiferromagnetic 2D semiconductor CrSBr. Excitonic transitions in bilayers and above can be drastically changed when the magnetic order is switched from the layered antiferromagnetic ground state to a field-induced ferromagnetic state, an effect attributed to the spin-allowed interlayer hybridization of electron and hole orbitals in the latter, as revealed by Green’s function–Bethe–Salpeter equation (GW-BSE) calculations. Our work uncovers a magnetic approach to engineer electronic and excitonic effects in layered magnetic semiconductors.

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Fig. 1: Structure and optical properties of CrSBr.
Fig. 2: Excitons coupled to magnetic order.
Fig. 3: Magnetic order-dependent band structure and excitonic transitions.
Fig. 4: Magnetic order-dependent excitons in four-layer CrSBr.

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All relevant data are available in the main text, in the Supporting Information, or from the authors. These include all panels in Figs. 14 in the main text, Supplementary Figs. 19 in the Supporting Information and optimized atomic coordinates used in electronic structure calculations. There is no restriction on data availability.

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Acknowledgements

The temperature-dependent PL measurements were supported by the US Air Force Office of Scientific Research grant no. FA9550-18-1-0020 (to X.-Y.Z. and X.R.). Magneto-optical spectroscopy measurements are mainly supported by the US Department of Energy (DoE), Basic Energy Sciences (BES) under award no. DE-SC0018171. Synthesis, structural characterization and polarization-resolved PL measurements of CrSBr is supported by the Center on Programmable Quantum Materials, an Energy Frontier Research Center funded by the DoE, Office of Science, BES, under award no. DE-SC0019443 (to X.-Y.Z., X.X. and X.R.). Computational resources were provided by Hyak at UW. J.F. and K.X. acknowledge the Graduate Fellowship from Clean Energy Institute funded by the State of Washington. T.C. acknowledges support from the Micron Foundation. X.-Y.Z. acknowledges partial support for laser equipment by the Vannevar Bush Faculty Fellowship through the Office of Naval Research grant no. N00014-18-1-2080.

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X.-Y.Z., X.X., K.L. and N.P.W. conceived this work. Bulk crystals were synthesized and characterized by A.H.D. and E.J.T. with supervision by X.R. and C.D. Sample preparation was carried out by K.L. and A.H.D., assisted by N.P.W. and J.C. Temperature-dependent measurements were performed by K.L. with supervision from X.-Y.Z. Field-dependent and polarization-dependent measurements were performed by N.P.W. and J.C. with supervision from X.X. The vector magnet was operated by J.F., K.X., S.S. and T.C. performed first-principles calculations that interpreted the results. The manuscript was prepared by N.P.W., K.L., J.C., K.X., T.C., X.X. and X.-Y.Z. in consultation with all other authors. All authors read and commented on the manuscript.

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Correspondence to Ting Cao, Xavier Roy, Xiaodong Xu or Xiaoyang Zhu.

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Peer review information Nature Materials thanks Libai Huang, Sufei Shi and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Figs. 1–9, Method and Data.

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Wilson, N.P., Lee, K., Cenker, J. et al. Interlayer electronic coupling on demand in a 2D magnetic semiconductor. Nat. Mater. 20, 1657–1662 (2021). https://doi.org/10.1038/s41563-021-01070-8

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