Evidence for a polariton-mediated biexciton transition in single-walled carbon nanotubes
Strong coupling of excitonic resonances with a cavity gives rise to exciton-polaritons which possess a modified energy landscape compared to the uncoupled emitter. However, due to the femtosecond lifetime of the so-called bright polariton states and transient changes of the cavity reflectivity under...
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| Hauptverfasser: | , , , , |
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| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
4 May 2022
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| In: |
ACS photonics
Year: 2022, Jahrgang: 9, Heft: 5, Pages: 1567-1576 |
| ISSN: | 2330-4022 |
| DOI: | 10.1021/acsphotonics.1c01590 |
| Online-Zugang: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acsphotonics.1c01590
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| Verfasserangaben: | Jan M. Lüttgens, Zhuoran Kuang, Nicolas F. Zorn, Tiago Buckup, and Jana Zaumseil |
| Zusammenfassung: | Strong coupling of excitonic resonances with a cavity gives rise to exciton-polaritons which possess a modified energy landscape compared to the uncoupled emitter. However, due to the femtosecond lifetime of the so-called bright polariton states and transient changes of the cavity reflectivity under excitation, it is challenging to directly measure the polariton excited state dynamics. Here, near-infrared pump-probe spectroscopy is used to investigate the ultrafast dynamics of exciton-polaritons based on strongly coupled (6,5) single-walled carbon nanotubes in metal-clad microcavities. We present a protocol for fitting the reflectivity-associated response of the cavity using genetic algorithm-assisted transfer-matrix simulations. With this approach, we are able to identify an absorptive exciton-polariton feature in the transient transmission data. This feature appears instantaneously under resonant excitation of the upper polariton but is delayed for off-resonant excitation. The observed transition energy and detuning dependence point toward a direct upper polariton-to-biexciton transition. Our results provide direct evidence for exciton-polariton intrinsic transitions beyond the bright polariton lifetime in strongly coupled microcavities. |
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| Beschreibung: | Gesehen am 13.07.2022 |
| Beschreibung: | Online Resource |
| ISSN: | 2330-4022 |
| DOI: | 10.1021/acsphotonics.1c01590 |