Ultrafast transition from coherent to incoherent polariton nonlinearities in a hybrid 1L-WS2/plasmon structure
Exciton polaritons based on atomically thin semiconductors are essential building blocks of quantum optoelectronic devices. Their properties are governed by an ultrafast and oscillatory energy transfer between their excitonic and photonic constituents, resulting in the formation of polaritonic quasiparticles with pronounced nonlinearities induced by the excitonic component. In metallic, plasmonic nanoresonators, dissipation phenomena limit the polariton lifetime to a few tens of femtoseconds, so short that the role of these polaritons for the nonlinear response of such hybrids is yet unexplored. Here we use ultrafast two-dimensional electronic spectroscopy (2DES) to uncover coherent polariton dynamics in a hybrid monolayer (1L) WS<sub>2</sub>/plasmonic nanostructure. With respect to an uncoupled WS<sub>2</sub> flake, we observe an over 20-fold, polarization-dependent enhancement of the optical nonlinearity and a rapid evolution of the 2DES spectra within ~70 fs. We relate these dynamics to a transition from coherent polaritons to incoherent excitations, unravel the microscopic origin of the optical nonlinearities and show the potential of coherent polaritons for ultrafast all-optical switching.
Authors
- Daniel C. Timmer (ORCID: https://orcid.org/0000-0001-7541-8047)
- Moritz Gittinger (ORCID: https://orcid.org/0009-0003-5164-3014)
- Daniel C. Lünemann (ORCID: https://orcid.org/0000-0003-2077-3062)
- Martin Silies (ORCID: https://orcid.org/0000-0002-3704-2066)
- Christoph Lienau (ORCID: https://orcid.org/0000-0003-3854-5025)
- Sven Stephan
- Alisson R. Cadore (ORCID: https://orcid.org/0000-0003-1081-0915)
- Bárbara L. T. Rosa (ORCID: https://orcid.org/0000-0001-9433-3532)
- Thomas Quenzel (ORCID: https://orcid.org/0000-0002-3455-7857)
- Antonietta De Sio (ORCID: https://orcid.org/0000-0003-2363-5634)
- Marten Richter (ORCID: https://orcid.org/0000-0003-4160-1008)
- Lara Greten (ORCID: https://orcid.org/0000-0001-9796-3257)
- Andrea C. Ferrari
- Giulio Cerullo
- Wenshan Li
- Andreas Knorr
- Giancarlo Soavi
Institutions
- Carl von Ossietzky Universität Oldenburg (DE)
- University of Cambridge (GB)
- Instituto de Óptica "Daza de Valdés" (ES)
- Istituto di Fotonica e Nanotecnologie (IT)
- Brazilian Center for Research in Energy and Materials (BR)
- Technische Universität Berlin (DE)
- Friedrich Schiller University Jena (DE)
- Politecnico di Milano (IT)
Publication Details
- Journal
- Nature Nanotechnology
- Published
- 2026-01-21
- DOI
- https://doi.org/10.1038/s41565-025-02054-4
- Citations
- 2
- Primary Topic
- Strong Light-Matter Interactions
- Type
- article
- Field-Weighted Citation Impact
- 62.78
Funders
- Niedersächsische Ministerium für Wissenschaft und Kultur
- Graphene Flagship
- Carl von Ossietzky Universität Oldenburg
- European Commission
- Deutsche Forschungsgemeinschaft
- Engineering and Physical Sciences Research Council