Evidence for a polariton-mediated biexciton transition in single-walled carbon nanotubes

• Verfasst von: Lüttgens, Jan [VerfasserIn]
• Verfasst von: Kuang, Zhuoran [VerfasserIn]
• Verfasst von: Zorn, Nicolas [VerfasserIn]
• Verfasst von: Buckup, Tiago [VerfasserIn]
• Verfasst von: Zaumseil, Jana [VerfasserIn]
• Titel: Evidence for a polariton-mediated biexciton transition in single-walled carbon nanotubes
• Verf.angabe: Jan M. Lüttgens, Zhuoran Kuang, Nicolas F. Zorn, Tiago Buckup, and Jana Zaumseil
• E-Jahr: 2022
• Jahr: 4 May 2022
• Umfang: 10 S.
• Fussnoten: Gesehen am 13.07.2022
• Titel Quelle: Enthalten in: American Chemical SocietyACS photonics
• Ort Quelle: Washington, DC : ACS, 2014
• Jahr Quelle: 2022
• Band/Heft Quelle: 9(2022), 5, Seite 1567-1576
• ISSN Quelle: 2330-4022
• DOI: doi:10.1021/acsphotonics.1c01590
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 1810091446

Abstract

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.