TY - JOUR
T1 - Monitoring polariton dynamics in the LHCII photosynthetic antenna in a microcavity by two-photon coincidence counting
AU - Zhang, Zhedong
AU - Saurabh, Prasoon
AU - Dorfman, Konstantin E.
AU - Debnath, Arunangshu
AU - Mukamel, Shaul
PY - 2018/2/21
Y1 - 2018/2/21
N2 - The relaxation dynamics of light-harvesting complex II in an optical cavity is explored theoretically by multidimensional photon coincidence counting spectroscopy. This technique reveals the dynamics in both single (e) and double (f) excitation bands. We study how the polariton dynamics are affected by coupling to photon modes and molecular vibrations described by a realistic spectral density at 77 K. Without the cavity, the e- and f-band energy transfer pathways are not clearly resolved due to the line broadening caused by fast exciton dephasing. The strong coupling to cavity photons results in well-resolved polariton modes. The hybrid nature of polaritons slows down their energy transfer rates.
AB - The relaxation dynamics of light-harvesting complex II in an optical cavity is explored theoretically by multidimensional photon coincidence counting spectroscopy. This technique reveals the dynamics in both single (e) and double (f) excitation bands. We study how the polariton dynamics are affected by coupling to photon modes and molecular vibrations described by a realistic spectral density at 77 K. Without the cavity, the e- and f-band energy transfer pathways are not clearly resolved due to the line broadening caused by fast exciton dephasing. The strong coupling to cavity photons results in well-resolved polariton modes. The hybrid nature of polaritons slows down their energy transfer rates.
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U2 - 10.1063/1.5004432
DO - 10.1063/1.5004432
M3 - RGC 21 - Publication in refereed journal
C2 - 29471638
SN - 0021-9606
VL - 148
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 7
M1 - 074302
ER -