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Pressure tuning of minibands in MoS2/WSe2 heterostructures revealed by moiré phonons

Nature Nanotechnology volume 18, pages 1147–1153 (2023)Cite this article

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Abstract

Moiré superlattices of two-dimensional heterostructures arose as a new platform to investigate emergent behaviour in quantum solids with unprecedented tunability. To glean insights into the physics of these systems, it is paramount to discover new probes of the moiré potential and moiré minibands, as well as their dependence on external tuning parameters. Hydrostatic pressure is a powerful control parameter, since it allows to continuously and reversibly enhance the moiré potential. Here we use high pressure to tune the minibands in a rotationally aligned MoS2/WSe2 moiré heterostructure, and show that their evolution can be probed via moiré phonons. The latter are Raman-inactive phonons from the individual layers that are activated by the moiré potential. Moiré phonons manifest themselves as satellite Raman peaks arising exclusively from the heterostructure region, increasing in intensity and frequency under applied pressure. Further theoretical analysis reveals that their scattering rate is directly connected to the moiré potential strength. By comparing the experimental and calculated pressure-induced enhancement, we obtain numerical estimates for the moiré potential amplitude and its pressure dependence. The present work establishes moiré phonons as a sensitive probe of the moiré potential as well as the electronic structures of moiré systems.

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Fig. 1: High-pressure Raman experiments on a 0°-MoS2/WSe2 moiré heterostructure.
Fig. 2: Moiré phonons in a 0°-MoS2/WSe2 moiré heterostructure.
Fig. 3: Origin of moiré phonons in a 0°-MoS2/WSe2 heterostructure.
Fig. 4: Miniband evolution with pressure revealed by moiré phonons.

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Data availability

The datasets generated in the the current study are available via Zenodo at https://zenodo.org/record/7872421 (ref. 63). Source data are provided with this paper.

Code availability

DFT calculations were conducted with the SIESTA code (https://gitlab.com/siesta-project/siesta), which is released under the terms of the GPL open-source license. The proprietary Vienna ab initio simulation package code was used under license no. 5-488 (available at https://www.vasp.at/) for the periodic DFT phonon calculations together with the Phonopy software. Phonopy is an open-source package for phonon calculations at harmonic and quasi-harmonic levels, which is released under the terms of the BSD license and is available at https://phonopy.github.io/phonopy. An implementation of the zone-folding computation is available from the corresponding authors upon reasonable request.

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Acknowledgements

L.G.P.M., J.-H.P. and J.K. acknowledge support from the MURI project by the US Army Research Office (ARO) under grant no. W911NF-18-1-0431. D.A.R.-T. acknowledges funding from PAPIIT-DGAPA-UNAM grant IA106523, and CONACyT grant 1564464. R.C. acknowledges support from the National Science Foundation under grant no. 1751739 and the STC Center for Integrated Quantum Materials, NSF, grant no. DMR-1231319. L.G.P.M. and J.K. acknowledge support from CNPq under the program Ciência sem Fronteiras (206251/2014-9). L.G.C. acknowledges support from CNPq through grant 309537/2019-3. M.S.C.M. and M.J.S.M. acknowledge financial support from CNPq, FAPEMIG and INCT-Nanocarbono. M.J.S.M. acknowledges support from the Universidade Federal de Ouro Preto (UFOP). We also acknowledge computational support from CESUP-UFRGS. This work was performed in part at the Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF award no. 1541959.

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Author notes

  1. These authors contributed equally: Luiz G. Pimenta Martins, David A. Ruiz-Tijerina.

Authors and Affiliations

  1. Physics Department, Massachusetts Institute of Technology, Cambridge, MA, USA

    Luiz G. Pimenta Martins, Connor A. Occhialini, Qian Song & Riccardo Comin

  2. Departamento de Física Química, Instituto de Física, Universidad Nacional Autónoma de México, Ciudad de México, Mexico

    David A. Ruiz-Tijerina

  3. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA

    Ji-Hoon Park, Ang-Yu Lu & Jing Kong

  4. Instituto de Física, Universidade Federal Fluminense, Niterói, Brazil

    Pedro Venezuela

  5. Departamento de Física, Universidade Federal de Minas Gerais, Belo Horizonte, Brazil

    Luiz G. Cançado & Mário S. C. Mazzoni

  6. Departamento de Física, Universidade Federal de Ouro Preto, Ouro Preto, Brazil

    Matheus J. S. Matos

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Contributions

L.G.P.M., J.K. and R.C. conceived the project. J.K. and R.C. supervised the project. D.A.R.-T. proposed the effective model for the pressure-dependent moiré potential, and carried out the zone-folding analysis and Raman rate computations. L.G.P.M., J.-H.P., Q.S. and A.-Y.L. prepared the TMD samples on a silicon substrate. L.G.P.M. and C.A.O. carried out the high-pressure Raman and PL experiments, and they analysed the experimental data. D.A.R.-T., L.G.P.M. and L.G.C. developed the proposed scattering mechanisms for moiré phonons. M.J.S.M., M.S.C.M. and P.V. carried out the DFT calculations. L.G.P.M., D.A.R.-T., J.K. and R.C. wrote the manuscript. All authors contributed to the scientific discussions and data interpretation.

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Correspondence to Luiz G. Pimenta Martins, Jing Kong or Riccardo Comin.

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Extended data

Extended Data Fig. 1 Raman frequencies as a function of pressure, measured both in the heterostructure and in the individual layers.

a A’1 of MoS2. b E’ of MoS2. c nearly-degenerate E’ and A’1 modes of WSe2.

Extended Data Fig. 2 Raman spectra of WSe2, MoS2, and MoS2/WSe2 at increasing pressures, zoomed-in the M3 peak spectral region.

The MoS2 M3 moiré phonon Raman peak is downshifted with respect to the MoS2 E’ peak. Its intensity increases with increasing pressure. The pressure is indicated at the top right corner of each panel.

Extended Data Fig. 3 Optical image of loaded sample inside of the DAC.

Regions 1, 2 and 3, corresponding to WSe2 monolayer, MoS2 monolayer and a rotationally-aligned MoS2/WSe2 heterostructure, respectively. During the loading process, the other two MoS2/WSe2 heterostructures, indicated by the red arrows, got partially damaged. Image taken with a 650 nm edge filter to enhance the optical contrast.

Supplementary information

Supplementary Information

Supplementary Sections 1–5, Figs. 1–5 and discussion.

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Source data

Source Data Fig. 1

Unprocessed Raman data shown in Fig. 1d,e.

Source Data Fig. 2

Experimental and fitting data points for Fig. 2a–d, and unprocessed polarized Raman data shown in Fig. 2e.

Source Data Fig. 4

Experimental and fitting data points for Fig. 4a,b.

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Pimenta Martins, L.G., Ruiz-Tijerina, D.A., Occhialini, C.A. et al. Pressure tuning of minibands in MoS2/WSe2 heterostructures revealed by moiré phonons. Nat. Nanotechnol. 18, 1147–1153 (2023). https://doi.org/10.1038/s41565-023-01413-3

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