TY - JOUR
T1 - Resonant Confinement of an Excitonic Polariton and Ultraefficient Light Harvest in Artificial Photosynthesis
AU - Chen, Yong Cong
AU - Song, Bo
AU - Leggett, Anthony J.
AU - Ao, Ping
AU - Zhu, Xiaomei
N1 - Publisher Copyright:
© 2019 American Physical Society.
PY - 2019/6/27
Y1 - 2019/6/27
N2 - We uncover a novel phenomenon from a recent artificial light-harvesting experiment [P.-Z. Chen et al., Angew. Chem., Int. Ed. Engl. 55, 2759 (2016)ACIEAY0570-083310.1002/anie.201510503] on organic nanocrystals of self-assembled difluoroboron chromophores. A resonant confinement of a polariton under strong photon-exciton coupling is predicted to exist within the microcavity of the crystal's own natural boundaries. Moreover, the radiative energy of a localized exciton falls into the spectrum of confinement. Hence, in the experiment, the spontaneous emission of an excited pigment would undergo a two-step process. It should first decay to an excitonic polariton trapped by the cavity resonance. The intermediate polariton could then funnel the energy directly to a doped acceptor, leading to the over 90% transfer efficiency observed at less than 1/1000 acceptor/donor ratio. The proposed mechanism is supported by parameter-free analyses entirely based on experiment data. Our finding may imply possible polariton-mediated pathways for energy transfers in biological photosynthesis.
AB - We uncover a novel phenomenon from a recent artificial light-harvesting experiment [P.-Z. Chen et al., Angew. Chem., Int. Ed. Engl. 55, 2759 (2016)ACIEAY0570-083310.1002/anie.201510503] on organic nanocrystals of self-assembled difluoroboron chromophores. A resonant confinement of a polariton under strong photon-exciton coupling is predicted to exist within the microcavity of the crystal's own natural boundaries. Moreover, the radiative energy of a localized exciton falls into the spectrum of confinement. Hence, in the experiment, the spontaneous emission of an excited pigment would undergo a two-step process. It should first decay to an excitonic polariton trapped by the cavity resonance. The intermediate polariton could then funnel the energy directly to a doped acceptor, leading to the over 90% transfer efficiency observed at less than 1/1000 acceptor/donor ratio. The proposed mechanism is supported by parameter-free analyses entirely based on experiment data. Our finding may imply possible polariton-mediated pathways for energy transfers in biological photosynthesis.
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U2 - 10.1103/PhysRevLett.122.257402
DO - 10.1103/PhysRevLett.122.257402
M3 - Article
C2 - 31347870
AN - SCOPUS:85069907117
SN - 0031-9007
VL - 122
JO - Physical review letters
JF - Physical review letters
IS - 25
M1 - 257402
ER -