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Light-Harvesting Efficiency Cannot Depend on Optical Coherence in the Absence of Orientational Order.
Rouse, Dominic M; Kushwaha, Adesh; Tomasi, Stefano; Lovett, Brendon W; Gauger, Erik M; Kassal, Ivan.
Afiliación
  • Rouse DM; School of Physics and Astronomy, University of Glasgow, Glasgow G12 8QQ, United Kingdom.
  • Kushwaha A; Department of Physics and Astronomy, University of Manchester, Manchester M13 9PL, United Kingdom.
  • Tomasi S; School of Chemistry and University of Sydney Nano Institute, University of Sydney, Sydney, NSW 2006, Australia.
  • Lovett BW; School of Chemistry and University of Sydney Nano Institute, University of Sydney, Sydney, NSW 2006, Australia.
  • Gauger EM; SUPA, School of Physics and Astronomy, University of St Andrews, St Andrews KY16 9SS, United Kingdom.
  • Kassal I; SUPA, Institute of Photonics and Quantum Sciences, Heriot-Watt University, Edinburgh EH14 4AS, United Kingdom.
J Phys Chem Lett ; 15(1): 254-261, 2024 Jan 11.
Article en En | MEDLINE | ID: mdl-38165172
ABSTRACT
The coherence of light has been proposed as a quantum-mechanical control for enhancing light-harvesting efficiency. In particular, optical coherence can be manipulated by changing either the polarization state or the spectral phase of the light. Here, we show that, in weak light, light-harvesting efficiency cannot be controlled using any form of optical coherence in molecular light-harvesting systems and, more broadly, those comprising orientationally disordered subunits and operating on longer-than-ultrafast time scales. Under those conditions, optical coherence does not affect the light-harvesting efficiency, meaning that it cannot be used for control. Specifically, polarization-state control is lost in disordered samples or when the molecules reorient on the time scales of light harvesting, and spectral-phase control is lost when the efficiency is time-averaged over a period longer than the optical coherence time. In practice, efficiency is always averaged over long times, meaning that coherent optical control is only possible through polarization and only in systems with orientational order.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2024 Tipo del documento: Article País de afiliación: Reino Unido Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2024 Tipo del documento: Article País de afiliación: Reino Unido Pais de publicación: Estados Unidos