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Tunable interaction between excitons and hybridized magnons in a layered semiconductor

Nature Nanotechnology volume 18, pages 23–28 (2023)Cite this article

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Abstract

The interaction between distinct excitations in solids is of both fundamental interest and technological importance. One such interaction is the coupling between an exciton, a Coulomb bound electron–hole pair, and a magnon, a collective spin excitation. The recent emergence of van der Waals magnetic semiconductors1 provides a platform to explore these exciton–magnon interactions and their fundamental properties, such as strong correlation2, as well as their photospintronic and quantum transduction3 applications. Here we demonstrate the precise control of coherent exciton–magnon interactions in the layered magnetic semiconductor CrSBr. We varied the direction of an applied magnetic field relative to the crystal axes, and thus the rotational symmetry of the magnetic system4. Thereby, we tuned not only the exciton coupling to the bright magnon, but also to an optically dark mode via magnon–magnon hybridization. We further modulated the exciton–magnon coupling and the associated magnon dispersion curves through the application of uniaxial strain. At a critical strain, a dispersionless dark magnon band emerged. Our results demonstrate an unprecedented level of control of the opto–mechanical–magnonic coupling, and a step towards the predictable and controllable implementation of hybrid quantum magnonics5,6,7,8,9,10,11.

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Fig. 1: Magnetic field tuning of exciton–magnon coupling.
Fig. 2: Coherent coupling between the bright and dark magnon modes.
Fig. 3: Control of exciton-hybridized magnon coupling via a symmetry-breaking magnetic field.
Fig. 4: Strain tuning the exciton–magnon coupling.

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Data availability

The datasets generated during and/or analysed during this study are provided with this paper. All other data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was mainly supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (DE-SC0012509). Sample fabrication and optical measurements are partially supported by AFOSR FA9550-19-1-0390 and FA9550-21-1-0460. Synthesis of the CrSBr crystals is supported as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under award DE-SC0019443. D.G.C. was supported by the NSF MRSEC on Precision-Assembled Quantum Materials (DMR-2011738). This research was supported by an appointment to the Intelligence Community Postdoctoral Research Fellowship Program at the University of Washington, administered by the Oak Ridge Institute for Science and Education through an interagency agreement between the US Department of Energy and the Office of the Director of National Intelligence.

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Author notes

  1. These authors contributed equally: Geoffrey M. Diederich, John Cenker, Yafei Ren.

Authors and Affiliations

  1. Intelligence Community Postdoctoral Research Fellowship Program, University of Washington, Seattle, WA, USA

    Geoffrey M. Diederich

  2. Department of Physics, University of Washington, Seattle, WA, USA

    Geoffrey M. Diederich, John Cenker, Jordan Fonseca, Di Xiao & Xiaodong Xu

  3. Department of Materials Science and Engineering, University of Washington, Seattle, WA, USA

    Yafei Ren, Ting Cao, Di Xiao & Xiaodong Xu

  4. Department of Chemistry, Columbia University, New York, NY, USA

    Daniel G. Chica, Youn Jue Bae, Xiaoyang Zhu & Xavier Roy

Authors
  1. Geoffrey M. Diederich
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Contributions

X.X. and D.X. conceived the project. G.M.D. performed the measurements with help from J.C., J.F. and Y.J.B. J.C. designed the strain technique and fabricated the samples. G.M.D., J.C., Y.R., X.Z., T.C., D.X. and X.X. analysed the data and interpreted the results. Y.R., T.C. and D.X. built the model and performed the simulations. D.G.C. and X.R. grew the CrSBr crystals. G.M.D., J.C., Y.R., D.X. and X.X. wrote the manuscript with input from all the authors. All the authors discussed the results.

Corresponding authors

Correspondence to Di Xiao or Xiaodong Xu.

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Extended data

Extended Data Fig. 1 Comparison of measurements.

Magnetic field dependent magnon spectra obtained by Fourier transformation of a, transient reflectivity and b, TR-MOKE data.

Extended Data Fig. 2 Raw transient reflectivity data at θab = 0°.

a, Magnetic field dependence of the transient reflectivity signal. b, Slice from the raw data taken from a at µoH = 0.3 T. c, The same data in (b) after subtraction of the electronic decay signal.

Extended Data Fig. 3 Raw transient reflectivity data with θab = 2°.

a, Magnetic field dependence of the transient reflectivity signal. b, Fourier transform of (a). c, Slice taken from a along µoH = 0.53 T, that is at the center of the avoided crossing.

Extended Data Fig. 4 Raw transient reflectivity data with respect to θab.

a, Intensity plot of transient reflectivity signal as a function of magnetic field and pump-probe delay at θab = 3°. b, and c, are the same as (a) but with θab = 6° and 9°, respectively. d-f, Time resolved line traces at three selected magnetic field strengths for each θab value.

Extended Data Fig. 5 Angular dependence of magnon coupling.

a-c, Magnon spectra measured at fixed µoH while varying θab. Note that limitations of the experimental apparatus put upper bounds on the accessible field angles. d-f, Simulations of the magnon spectra at fixed µoH while varying θab over the full range of angles. Here the dashed lines show the magnon center frequency and the colored dots show the amplitude.

Extended Data Fig. 6 Raw transient reflectivity data at high strains.

a, Magnetic field dependence of the transient reflectivity signal at a strain larger than the stain induced AFM to FM transition. There is a shift in the data with field, but the lack of any oscillatory signal implies that the crystal is in the FM state at all fields. b, Fourier transform of (a). c, Slice taken from (a) at µoH = 0 T.

Extended Data Fig. 7 Calibration of the strain device.

a, Strain calibration curves for increasing (blue) and decreasing (orange) piezo voltages. Inset shows a picture of the CrSBr flake measured in this study with gold evaporated on top. b, Shift of the P3 Raman peakz with increasing piezo voltage. c, The same peak shown in (b) at 0% (blue) and 1.9% (black) strain.

Supplementary information

Supplementary Information

Additional information on data processing, strain calibration and the theoretical framework.

Source data

Source Data Fig. 1

Raw transient reflectivity data for Fig. 1.

Source Data Fig. 2

Raw transient reflectivity data for Fig. 2.

Source Data Fig. 3

Raw transient reflectivity data and fitting results for Fig. 3.

Source Data Fig. 4

Raw transient reflectivity data and fitting results for Fig. 4.

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Diederich, G.M., Cenker, J., Ren, Y. et al. Tunable interaction between excitons and hybridized magnons in a layered semiconductor. Nat. Nanotechnol. 18, 23–28 (2023). https://doi.org/10.1038/s41565-022-01259-1

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