Monitoring polariton dynamics in the LHCII photosynthetic antenna in a microcavity by two-photon coincidence counting

Abstract

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.

Entangled photon assisted multidimensional nonlinear optics of exciton–polaritons

“…multi-mode Brownian oscillators and one over-damped oscillator. The number of multimode Brownian oscillators (N b ), the respective spectral shift parameters (λ 0 , λ j ¼ υ j ϒ j , where υ j and ϒ j are the jth oscillator frequencies and Huang-Rhys parameters, respectively), and the damping parameter γ 0 , γ j that are required to optimally describe the equilibrium spectral density function have been obtained via a systematic spectral fitting procedure in the work of Novoderezhkin et al 32,43 The numerical values corresponding to those parameters are enlisted in Appendix B.…”

“…The values of the cavity mode frequencies, ω I c Àω III c are chosen to be in resonance with the lower energy, the central region, and the higher energy region of the spectral bands of the bare exciton. 32 Moreover, within a set, each column is characterized by different values for the entanglement times given as T I b ¼ 100 fs, T II b ¼ 200 fs, T III b ¼ 500 fs while the rows account for the variations of the coupling strengths. In other words, in the simulation, each representative parameter combinations {ω I c , g I c } to {ω III c , g III c } is studied for three further variations of the biphoton entanglement times and has been presented along each column, i.e., making an assignment {ω I c , g I c , T I b } for a particular set.…”

“…Toward this aim, the cavity mediated control of the coherent excitonic transport properties in the quantum aggregates remains a coveted goal. [24][25][26][27][28][29][30][31][32] This communication aims to leverage the static tunability of the cavity to generate the exciton-polariton sideband modes and investigate the emergent mode correlation dynamics in the presence of phonon induced dissipation using the entangled biphoton sources (Fig. 1).…”

Optimization of selective two-photon absorption in cavity polaritons

“…Nevertheless, recent years have seen the rapid rise of theoretical investigations, as well as first proof-of-concept experiments that challenge this convention, and investigate how quantum properties of light can be applied or exploited beneficially in spectroscopic applications [4][5][6][7][8] . This includes the use of photon correlation measurements to analyse the light fields emitted by a sample [9][10][11][12][13] in single-molecule spectroscopy [14][15][16] , or to exploit coincidence measurements to detect particular spectral features in the sample [17][18][19][20] , as well as the generation of photonic entanglement in fluorescent proteins 21 .…”

Geometry Effects on Light‐Harvesting Complex's Light Absorption and Energy Transfer in Purple Bacteria

“…Quantum coherence phenomenon between the excitation migration pathways has also been demonstrated using 2D Fourier transform electronic spectroscopy . A novel time‐resolved and frequency‐resolved spectroscopic probe has been recently proposed for monitoring the exciton relaxation in LHCII antenna . The light‐induced infrared difference spectroscopy of the LHC has also been investigated .…”