Efficiency of energy funneling in the photosystem II supercomplex of higher plants

The investigation of energy transfer properties in photosynthetic multi-protein networks gives insight into their underlying design principles.Here, we discuss excitonic energy transfer mechanisms of the photosystem II (PS-II) C$_2$S$_2$M$_2$ supercomplex, which is the largest isolated functional unit of the photosynthetic apparatus of higher plants.Despite the lack of a decisive energy gradient in C$_2$S$_2$M$_2$, we show that the energy transfer is directed by relaxation to low energy states. C$_2$S$_2$M$_2$ is not organized to form pathways with strict energetic downhill transfer, which has direct consequences on the transfer efficiency, transfer pathways and transfer limiting steps. The exciton dynamics is sensitive to small structural changes, which, for instance, are induced by the reorganization of vibrational coordinates. In order to incorporate the reorganization process in our numerical simulations, we go beyond rate equations and use the hierarchically coupled equation of motion approach (HEOM). While transfer from the peripherical antenna to the proteins in proximity to the reaction center occurs on a faster time scale, the final step of the energy transfer to the RC core is rather slow, and thus the limiting step in the transfer chain. Our findings suggest that the structure of the PS-II supercomplex guarantees photoprotection rather than optimized efficiency.Comment: 23 pages, 6 figure

Nonlinear optics in the fractional quantum Hall regime

Engineering strong interactions between optical photons is a great challenge for quantum science. Envisioned applications range from the realization of photonic gates for quantum information processing to synthesis of photonic quantum materials for investigation of strongly-correlated driven-dissipative systems. Polaritonics, based on the strong coupling of photons to atomic or electronic excitations in an optical resonator, has emerged as a promising approach to implement those tasks. Recent experiments demonstrated the onset of quantum correlations in the exciton-polariton system, showing that strong polariton blockade could be achieved if interactions were an order of magnitude stronger. Here, we report time resolved four-wave mixing experiments on a two-dimensional electron system embedded in an optical cavity, demonstrating that polariton-polariton interactions are strongly enhanced when the electrons are initially in a fractional quantum Hall state. Our experiments indicate that in addition to strong correlations in the electronic ground state, exciton-electron interactions leading to the formation of polaron polaritons play a key role in enhancing the nonlinear optical response. Besides potential applications in realization of strongly interacting photonic systems, our findings suggest that nonlinear optical measurements could provide information about fractional quantum Hall states that is not accessible in linear optical response

Bright single photon emission from a quantum dot in a circular Bragg grating microcavity

Bright single photon emission from single quantum dots in suspended circular Bragg grating microcavities is demonstrated. This geometry has been designed to achieve efficient (> 50 %) single photon extraction into a near-Gaussian shaped far-field pattern, modest (~10x) Purcell enhancement of the radiative rate, and a spectral bandwidth of a few nanometers. Measurements of fabricated devices show progress towards these goals, with collection efficiencies as high as ~10% demonstrated with moderate spectral bandwidth and rate enhancement. Photon correlation measurements are performed under above-bandgap excitation (pump wavelength = 780 nm to 820 nm) and confirm the single photon character of the collected emission. While the measured sources are all antibunched and dominantly composed of single photons, the multi-photon probability varies significantly. Devices exhibiting tradeoffs between collection efficiency, Purcell enhancement, and multi-photon probability are explored and the results are interpreted with the help of finite-difference time-domain simulations. Below-bandgap excitation resonant with higher states of the quantum dot and/or cavity (pump wavelength = 860 nm to 900 nm) shows a near-complete suppression of multi-photon events and may circumvent some of the aforementioned tradeoffs.Comment: 11 pages, 12 figure

Interplay between excitation kinetics and reaction-center dynamics in purple bacteria

Photosynthesis is arguably the fundamental process of Life, since it enables energy from the Sun to enter the food-chain on Earth. It is a remarkable non-equilibrium process in which photons are converted to many-body excitations which traverse a complex biomolecular membrane, getting captured and fueling chemical reactions within a reaction-center in order to produce nutrients. The precise nature of these dynamical processes -- which lie at the interface between quantum and classical behaviour, and involve both noise and coordination -- are still being explored. Here we focus on a striking recent empirical finding concerning an illumination-driven transition in the biomolecular membrane architecture of {\it Rsp. Photometricum} purple bacteria. Using stochastic realisations to describe a hopping rate model for excitation transfer, we show numerically and analytically that this surprising shift in preferred architectures can be traced to the interplay between the excitation kinetics and the reaction center dynamics. The net effect is that the bacteria profit from efficient metabolism at low illumination intensities while using dissipation to avoid an oversupply of energy at high illumination intensities.Comment: 21 pages, 13 figures, accepted for publication in New Journal of Physic

Optical signatures of quantum delocalization over extended domains in photosynthetic membranes

The prospect of coherent dynamics and excitonic delocalization across several light-harvesting structures in photosynthetic membranes is of considerable interest, but challenging to explore experimentally. Here we demonstrate theoretically that the excitonic delocalization across extended domains involving several light-harvesting complexes can lead to unambiguous signatures in the optical response, specifically, linear absorption spectra. We characterize, under experimentally established conditions of molecular assembly and protein-induced inhomogeneities, the optical absorption in these arrays from polarized and unpolarized excitation, and demonstrate that it can be used as a diagnostic tool to determine the coherent coupling among iso-energetic light-harvesting structures. The knowledge of these couplings would then provide further insight into the dynamical properties of transfer, such as facilitating the accurate determination of F\"orster rates.Comment: 4 figures and Supplementary information with 7 figures. To appear in Journal of physical chemistry A, 201