Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Nonlinear valley phonon scattering under the strong coupling regime

Nature Materials volume 20, pages 1210–1215 (2021)Cite this article

Subjects

Abstract

Research efforts of cavity quantum electrodynamics have focused on the manipulation of matter hybridized with photons under the strong coupling regime1,2,3. This has led to striking discoveries including polariton condensation2 and single-photon nonlinearity3, where the phonon scattering plays a critical role1,2,3,4,5,6,7,8,9. However, resolving the phonon scattering remains challenging for its non-radiative complexity. Here we demonstrate nonlinear phonon scattering in monolayer MoS2 that is strongly coupled to a plasmonic cavity mode. By hybridizing excitons and cavity photons, the phonon scattering is equipped with valley degree of freedom and boosted with superlinear enhancement to a stimulated regime, as revealed by Raman spectroscopy and our theoretical model. The valley polarization is drastically enhanced and sustained throughout the stimulated regime, suggesting a coherent scattering process enabled by the strong coupling. Our findings clarify the feasibility of valley–cavity-based systems for lighting, imaging, optical information processing and manipulating quantum correlations in cavity quantum electrodynamics2,3,10,11,12,13,14,15,16,17.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Schematics of demonstrating phonon scattering under the strong coupling regime.
Fig. 2: Determination of the strong coupling regime in a MoS2 monolayer embedded in plasmonic cavities.
Fig. 3: Direct observation of phonon scattering under the strong coupling regime.
Fig. 4: Uncovering stimulated phonon scattering by polariton-resonance excitation.

Similar content being viewed by others

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

References

  1. Sanvitto, D. & Kéna-Cohen, S. The road towards polaritonic devices. Nat. Mater. 15, 1061–1073 (2016).

    Article  CAS  Google Scholar 

  2. Deng, H., Haug, H. & Yamamoto, Y. Exciton-polariton Bose-Einstein condensation. Rev. Mod. Phys. 82, 1489–1537 (2010).

    Article  CAS  Google Scholar 

  3. Lodahl, P., Mahmoodian, S. & Stobbe, S. Interfacing single photons and single quantum dots with photonic nanostructures. Rev. Mod. Phys. 87, 347–400 (2015).

    Article  CAS  Google Scholar 

  4. Kasprzak, J., Solnyshkov, D. D., André, R., Dang, L. S. & Malpuech, G. Formation of an exciton polariton condensate: thermodynamic versus kinetic regimes. Phys. Rev. Lett. 101, 146404 (2008).

    Article  CAS  Google Scholar 

  5. Müller, K. et al. Ultrafast polariton-phonon dynamics of strongly coupled quantum dot-nanocavity systems. Phys. Rev. X 5, 031006 (2015).

    Google Scholar 

  6. Seidelmann, T. et al. Phonon-induced enhancement of photon entanglement in quantum dot-cavity systems. Phys. Rev. Lett. 123, 137401 (2019).

    Article  CAS  Google Scholar 

  7. Gonzalez-Ballestero, C., Feist, J., Gonzalo Badía, E., Moreno, E. & Garcia-Vidal, F. J. Uncoupled dark states can inherit polaritonic properties. Phys. Rev. Lett. 117, 156402 (2016).

    Article  Google Scholar 

  8. Skopelitis, P., Cherotchenko, E. D., Kavokin, A. V. & Posazhennikova, A. Interplay of phonon and exciton-mediated superconductivity in hybrid semiconductor-superconductor structures. Phys. Rev. Lett. 120, 107001 (2018).

    Article  CAS  Google Scholar 

  9. Thomas, A. et al. Exploring superconductivity under strong coupling with the vacuum electromagnetic field. Preprint at https://arxiv.org/abs/1911.01459 (2019).

  10. Chen, Y.-J., Cain, J. D., Stanev, T. K., Dravid, V. P. & Stern, N. P. Valley-polarized exciton-polaritons in a monolayer semiconductor. Nat. Photon. 11, 431–435 (2017).

    Article  CAS  Google Scholar 

  11. Dufferwiel, S. et al. Valley addressable exciton-polaritons in atomically thin semiconductors. Nat. Photon. 11, 497–501 (2017).

    Article  CAS  Google Scholar 

  12. Sun, Z. et al. Optical control of room-temperature valley polaritons. Nat. Photon. 11, 491–496 (2017).

    Article  CAS  Google Scholar 

  13. Chervy, T. et al. Room temperature chiral coupling of valley excitons with spin-momentum locked surface plasmons. ACS Photon. 5, 1281–1287 (2018).

    Article  CAS  Google Scholar 

  14. Lundt, N. et al. Optical valley Hall effect for highly valley-coherent exciton-polaritons in an atomically thin semiconductor. Nat. Nanotechnol. 14, 770–775 (2019).

    Article  CAS  Google Scholar 

  15. Zhu, H. et al. Observation of chiral phonons. Science 359, 579–582 (2018).

    Article  CAS  Google Scholar 

  16. Miller, B. et al. Tuning the Fröhlich exciton-phonon scattering in monolayer MoS2. Nat. Commun. 10, 807 (2019).

    Article  Google Scholar 

  17. Luo, Y. et al. Deterministic coupling of site-controlled quantum emitters in monolayer WSe2 to plasmonic nanocavities. Nat. Nanotechnol. 13, 1137–1142 (2018).

    Article  CAS  Google Scholar 

  18. Liu, W. et al. Strong exciton–plasmon coupling in MoS2 coupled with plasmonic lattice. Nano Lett. 16, 1262–1269 (2016).

    Article  CAS  Google Scholar 

  19. Chikkaraddy, R. et al. Single-molecule strong coupling at room temperature in plasmonic nanocavities. Nature 535, 127–130 (2016).

    Article  CAS  Google Scholar 

  20. Mak, K. F. & Shan, J. Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides. Nat. Photon. 10, 216–226 (2016).

    Article  CAS  Google Scholar 

  21. Carvalho, B. R. et al. Intervalley scattering by acoustic phonons in two-dimensional MoS2 revealed by double-resonance Raman spectroscopy. Nat. Commun. 8, 14670 (2017).

    Article  Google Scholar 

  22. Xu, X., Yao, W., Xiao, D. & Heinz, T. Spin and pseudospins in layered transition metal dichalcogenides. Nat. Phys. 10, 343–350 (2014).

    Article  CAS  Google Scholar 

  23. Zhang, X. et al. Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material. Chem. Soc. Rev. 44, 2757–2785 (2015).

    Article  CAS  Google Scholar 

  24. Drapcho, S. G. et al. Apparent breakdown of Raman selection rule at valley exciton resonances in monolayer MoS2. Phys. Rev. B 95, 165417 (2017).

    Article  Google Scholar 

  25. Lombardi, A. et al. Pulsed molecular optomechanics in plasmonic nanocavities: from nonlinear vibrational instabilities to bond-breaking. Phys. Rev. X 8, 011016 (2018).

    CAS  Google Scholar 

  26. Schmidt, M. K., Esteban, R., González-Tudela, A., Giedke, G. & Aizpurua, J. Quantum mechanical description of Raman scattering from molecules in plasmonic cavities. ACS Nano 10, 6291–6298 (2016).

    Article  CAS  Google Scholar 

  27. Fainstein, A. & Jusserand, B. Cavity-polariton mediated resonant Raman scattering. Phys. Rev. Lett. 78, 1576–1579 (1997).

    Article  CAS  Google Scholar 

  28. Shalabney, A. et al. Enhanced Raman scattering from vibro-polariton hybrid states. Angew. Chem. Int. Ed. 54, 7971–7975 (2015).

    Article  CAS  Google Scholar 

  29. Chen, S.-Y., Zheng, C., Fuhrer, M. S. & Yan, J. Helicity resolved Raman scattering of MoS2, MoSe2, WS2 and WSe2 atomic layers. Nano Lett. 15, 2526–2532 (2015).

    Article  CAS  Google Scholar 

  30. Zhang, R. et al. Chemical mapping of a single molecule by plasmon-enhanced Raman scattering. Nature 498, 82–86 (2013).

    Article  CAS  Google Scholar 

  31. Li, J. F. et al. Surface analysis using shell-isolated nanoparticle-enhanced Raman spectroscopy. Nat. Protoc. 8, 52–65 (2013).

    Article  CAS  Google Scholar 

  32. Eilers, P. H. C. A perfect smoother. Anal. Chem. 75, 3631–3636 (2003).

    Article  CAS  Google Scholar 

  33. Palik, E. D. Handbook of Optical Constants of Solids II (Academic Press, 1991).

  34. Cadiz, F. et al. Excitonic linewidth approaching the homogeneous limit in MoS2-based van der Waals heterostructures. Phys. Rev. X 7, 021026 (2017).

    Google Scholar 

  35. Kleemann, M. E. et al. Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature. Nat. Commun. 8, 1296 (2017).

    Article  Google Scholar 

  36. Qin, J. et al. Revealing strong plasmon-exciton coupling between nanogap resonators and two-dimensional semiconductors at ambient conditions. Phys. Rev. Lett. 124, 063902 (2020).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the King Abdullah University of Science and Technology Office of Sponsored Research award OSR-2016-CRG5-2996, National Science Foundation MRI grant 1725335 and the Ernest S. Kuh Endowed Chair Professorship. X.L. also acknowledges support from the National Natural Science Foundation of China (grant nos 12074297 and 62005202). J.-F.L. acknowledges support from National Natural Science Foundation of China (grant no. 21925404) and National Key Research and Development Program of China (2019YFA0705400). Y.-H.L. acknowledges support from the Ministry of Science and Technology (MoST 109-2124-M-007-001-MY3; 108-2112-M-007-006-MY3; 107-2923-M-007-002-MY3), the Frontier Research Center on Fundamental and Applied Sciences of Matters and the Center for Quantum Technology of National Tsing-Hua University.

Author information

Author notes

  1. These authors contributed equally: Xiaoze Liu, Jun Yi.

Authors and Affiliations

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

    Xiaoze Liu, Jun Yi, Sui Yang, Peiyao Zhang, Yuan Wang & Xiang Zhang

  2. School of Physics and Technology, Wuhan University, Wuhan, China

    Xiaoze Liu

  3. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China

    Jun Yi, Yue-Jiao Zhang, Jian-Feng Li & Zhong-Qun Tian

  4. Department of Materials Science and Engineering, National Tsing-Hua University, Hsinchu, Taiwan, Republic of China

    Erh-Chen Lin & Yi-Hsien Lee

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

    Xiang Zhang

Authors
  1. Xiaoze Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jun Yi
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Sui Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Erh-Chen Lin
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Yue-Jiao Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Peiyao Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Jian-Feng Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Yuan Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Yi-Hsien Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Zhong-Qun Tian
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Xiang Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

X.L. and J.Y. conceived the ideas and designed the experiments. X.L., J.Y. and S.Y. conducted the experiments. J.Y. performed finite element methods simulations and the theoretical modelling. E.-C.L. and Y.-H.L synthesized the CVD monolayer MoS2 sample. Y.-J.Z. and J.-F.L. synthesized the shell-isolated nanoparticles. X.Z. supervised the research. X.L. and J.Y. analysed the data and wrote the manuscript. All authors contributed to data interpretation and editing the manuscript.

Corresponding author

Correspondence to Xiang Zhang.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

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

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Notes 1 and 2, Figs. 1–19, Table 1 and references.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liu, X., Yi, J., Yang, S. et al. Nonlinear valley phonon scattering under the strong coupling regime. Nat. Mater. 20, 1210–1215 (2021). https://doi.org/10.1038/s41563-021-00972-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41563-021-00972-x

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing