Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons
Abstract Anti-Stokes photoluminescence (PL) is light emission at a higher photon energy than the excitation, with applications in optical cooling, bioimaging, lasing, and quantum optics. Here, we show how plasmonic nano-cavities activate anti-Stokes PL in WSe2 monolayers through resonant excitation...
| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-09-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-41401-8 |
| _version_ | 1797558741110882304 |
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| author | Niclas S. Mueller Rakesh Arul Gyeongwon Kang Ashley P. Saunders Amalya C. Johnson Ana Sánchez-Iglesias Shu Hu Lukas A. Jakob Jonathan Bar-David Bart de Nijs Luis M. Liz-Marzán Fang Liu Jeremy J. Baumberg |
| author_facet | Niclas S. Mueller Rakesh Arul Gyeongwon Kang Ashley P. Saunders Amalya C. Johnson Ana Sánchez-Iglesias Shu Hu Lukas A. Jakob Jonathan Bar-David Bart de Nijs Luis M. Liz-Marzán Fang Liu Jeremy J. Baumberg |
| author_sort | Niclas S. Mueller |
| collection | DOAJ |
| description | Abstract Anti-Stokes photoluminescence (PL) is light emission at a higher photon energy than the excitation, with applications in optical cooling, bioimaging, lasing, and quantum optics. Here, we show how plasmonic nano-cavities activate anti-Stokes PL in WSe2 monolayers through resonant excitation of a dark exciton at room temperature. The optical near-fields of the plasmonic cavities excite the out-of-plane transition dipole of the dark exciton, leading to light emission from the bright exciton at higher energy. Through statistical measurements on hundreds of plasmonic cavities, we show that coupling to the dark exciton leads to a near hundred-fold enhancement of the upconverted PL intensity. This is further corroborated by experiments in which the laser excitation wavelength is tuned across the dark exciton. We show that a precise nanoparticle geometry is key for a consistent enhancement, with decahedral nanoparticle shapes providing an efficient PL upconversion. Finally, we demonstrate a selective and reversible switching of the upconverted PL via electrochemical gating. Our work introduces the dark exciton as an excitation channel for anti-Stokes PL in WSe2 and paves the way for large-area substrates providing nanoscale optical cooling, anti-Stokes lasing, and radiative engineering of excitons. |
| first_indexed | 2024-03-10T17:35:46Z |
| format | Article |
| id | doaj.art-aab44d4f4e754135a8d6c78e17541f33 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-10T17:35:46Z |
| publishDate | 2023-09-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-aab44d4f4e754135a8d6c78e17541f332023-11-20T09:52:33ZengNature PortfolioNature Communications2041-17232023-09-011411910.1038/s41467-023-41401-8Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitonsNiclas S. Mueller0Rakesh Arul1Gyeongwon Kang2Ashley P. Saunders3Amalya C. Johnson4Ana Sánchez-Iglesias5Shu Hu6Lukas A. Jakob7Jonathan Bar-David8Bart de Nijs9Luis M. Liz-Marzán10Fang Liu11Jeremy J. Baumberg12NanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeNanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeNanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeDepartment of Chemistry, Stanford UniversityDepartment of Materials Science and Engineering, Stanford UniversityCIC biomaGUNE, Basque Research and Technology Alliance (BRTA)NanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeNanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeNanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeNanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeCIC biomaGUNE, Basque Research and Technology Alliance (BRTA)Department of Chemistry, Stanford UniversityNanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of CambridgeAbstract Anti-Stokes photoluminescence (PL) is light emission at a higher photon energy than the excitation, with applications in optical cooling, bioimaging, lasing, and quantum optics. Here, we show how plasmonic nano-cavities activate anti-Stokes PL in WSe2 monolayers through resonant excitation of a dark exciton at room temperature. The optical near-fields of the plasmonic cavities excite the out-of-plane transition dipole of the dark exciton, leading to light emission from the bright exciton at higher energy. Through statistical measurements on hundreds of plasmonic cavities, we show that coupling to the dark exciton leads to a near hundred-fold enhancement of the upconverted PL intensity. This is further corroborated by experiments in which the laser excitation wavelength is tuned across the dark exciton. We show that a precise nanoparticle geometry is key for a consistent enhancement, with decahedral nanoparticle shapes providing an efficient PL upconversion. Finally, we demonstrate a selective and reversible switching of the upconverted PL via electrochemical gating. Our work introduces the dark exciton as an excitation channel for anti-Stokes PL in WSe2 and paves the way for large-area substrates providing nanoscale optical cooling, anti-Stokes lasing, and radiative engineering of excitons.https://doi.org/10.1038/s41467-023-41401-8 |
| spellingShingle | Niclas S. Mueller Rakesh Arul Gyeongwon Kang Ashley P. Saunders Amalya C. Johnson Ana Sánchez-Iglesias Shu Hu Lukas A. Jakob Jonathan Bar-David Bart de Nijs Luis M. Liz-Marzán Fang Liu Jeremy J. Baumberg Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons Nature Communications |
| title | Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons |
| title_full | Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons |
| title_fullStr | Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons |
| title_full_unstemmed | Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons |
| title_short | Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons |
| title_sort | photoluminescence upconversion in monolayer wse2 activated by plasmonic cavities through resonant excitation of dark excitons |
| url | https://doi.org/10.1038/s41467-023-41401-8 |
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