Thomas Wellens

Efficient and coherent excitation transfer across disordered molecular networks

We show that finite-size, disordered molecular networks can mediate highly efficient, coherent excitation transfer which is robust against ambient dephasing and associated with strong multisite entanglement. Such optimal, random molecular conformations may explain efficient energy transfer in the photosynthetic Fenna-Matthews-Olson complex.

Optimal networks for excitonic energy transport

We investigate coherent and incoherent excitation transfer in a random network with dipole–dipole interactions as a model system describing energy transport, e.g., in photosynthetic light-harvesting complexes or gases of cold Rydberg atoms. For this purpose, we introduce and compare two different measures (the maximum output probability and the average transfer time) for the efficiency of transport from the input to the output site. We especially focus on optimal configurations which maximize the transfer efficiency and the impact of dephasing noise on the transport dynamics. For most configurations of the random network, the transfer efficiency increases when adding noise, giving rise to essentially classical transport. These noise-assisted configurations are, however, systematically less efficient than the optimal configurations. The latter reach their highest efficiency for purely coherent dynamics, i.e. in the absence of noise.

Entanglement of 2×K quantum systems

We derive an analytical expression for the lower bound of the concurrence of mixed quantum states of composite 2×K systems. In contrast to other, implicitly defined entanglement measures, the numerical evaluation of our bound is straightforward. We explicitly evaluate its tightness for general mixed states of 2 × 3 systems, and identify a large class of states where our expression gives the exact value of the concurrence.

Nonlinear coherent transport of waves in disordered media.

We present a diagrammatic theory for coherent backscattering from disordered dilute media in the nonlinear regime. We show that the coherent backscattering enhancement factor is strongly affected by the nonlinearity, and we corroborate these results by numerical simulations. Our theory can be applied to several physical scenarios such as scattering of light in a nonlinear Kerr medium or propagation of matter waves in disordered potentials.

Coherent Backscattering of Bose-Einstein Condensates in Two-Dimensional Disorder Potentials

We study quantum transport of an interacting Bose-Einstein condensate in a two-dimensional disorder potential. In the limit of a vanishing atom-atom interaction, a sharp cone in the angle-resolved density of the scattered matter wave is observed, arising from constructive interference between amplitudes propagating along reversed scattering paths. Weak interaction transforms this coherent backscattering peak into a pronounced dip, indicating destructive instead of constructive interference. We reproduce this result, obtained from the numerical integration of the Gross-Pitaevskii equation, by a diagrammatic theory of weak localization in the presence of nonlinearity.

Partial nonlinear reciprocity breaking through ultrafast dynamics in a random photonic medium.

We demonstrate that ultrafast nonlinear dynamics gives rise to reciprocity breaking in a random photonic medium. Reciprocity breaking is observed via the suppression of coherent backscattering, a manifestation of weak localization of light. The effect is observed in a pump-probe configuration where the pump induces an ultrafast step change of the refractive index during the dwell time of the probe light in the material. The dynamical suppression of coherent backscattering is reproduced well by a multiple scattering Monte Carlo simulation. Ultrafast reciprocity breaking provides a distinct mechanism in nonlinear optical media, which opens up avenues for the active manipulation of mesoscopic transport, random lasers, and photon localization.

The optimization topography of exciton transport

Stunningly large exciton transfer rates in the light harvesting complex of photosynthesis, together with recent experimental 2D spectroscopic data, have spurred a vivid debate on the possible quantum origin of such efficiency. Here we show that configurations of a random molecular network that optimize constructive quantum interference from input to output site yield systematically shorter transfer times than classical transport induced by ambient dephasing noise.

Transport and Entanglement

Publisher Summary This chapter reviews the essential ingredients of quantum transport in disordered systems, and introduces measures of quantum coherence and entanglement in multisite systems. It explains excitation transport in Fenna–Matthews–Olsen (FMO)-like structures under strictly coherent conditions as well as in presence of a dephasing environment. The statistical treatment of excitation transport across a molecular network mimicking the FMO light-harvesting complex shows the potential of quantum coherence to enhance transport, on transient timescales. The transfer probability thus achieved can reach 100%—a value unachievable by classically diffusive, unbiased transport. Furthermore, because such quantum transfer is brought about by constructive multipath interference along intermediate sites of the molecular complex, coherent quantum transport is certainly faster than classically diffusive transport for comparable inter-site coupling strengths. Taking both transfer probability and transfer time together, coherence thus defines levels of quantum efficiency unreached by a classical transport process on the same network. The quantum coherence holds the potential to steer quantum transport efficiencies in engineered devices as abundant in semiconductor technology.

Centrosymmetry enhances quantum transport in disordered molecular networks

For more than 50 years we have known that photosynthetic systems harvest solar energy with almost unit quantum efficiency. However, recent experimental evidence of quantum coherence during the excitonic energy transport in photosynthetic organisms challenges our understanding of this fundamental biological function. Currently, and despite numerous efforts, the causal connection between coherence and efficiency is still a matter of debate. We show, through extensive simulations of quantum coherent transport on networks, that three dimensional structures characterized by centro-symmetric Hamiltonians are statistically more efficient than random arrangements. Moreover, a strong correlation of centro-symmetry with quantum efficiency is also observed under the coherent transport dynamics induced by experimentally estimated electronic Hamiltonians of the Fenna–Mathew–Olson complex of sulfur bacteria and of the cryptophyte PC645 complex of marine algae. The application of a genetic algorithm results in a set of optimized Hamiltonians only when seeded from the experimentally estimated Hamiltonian. These results suggest that what appears to be geometrically disordered complexes may well exhibit an inherent hidden symmetry which enhances the energy transport between chromophores. We are confident that our results will motivate research to explore the properties of nearly centro-symmetric Hamiltonians in realistic environments, and to unveil the role of symmetries for quantum effects in biology. The unravelling of such symmetries may open novel perspectives and suggest new design principles in the development of artificial devices.

Improving triplet-triplet-annihilation based upconversion systems by tuning their topological structure

Materials capable to perform upconversion of light transform the photon spectrum and can be used to increase the efficiency of solar cells by upconverting sub-bandgap photons, increasing the density of photons able to generate an electron-hole pair in the cell. Incoherent solar radiation suffices to activate upconverters based on sensitized triplet-triplet annihilation, which makes them particularly suited for this task. This process requires two molecular species, sensitizers absorbing low energy photons, and emitters generating higher frequency photons. Successful implementations exist in solutions and solids. However, solid upconverters exhibit lower efficiency than those in solution, which poses a serious problem for real applications. In the present work, we suggest a new strategy to increase the efficiency of sensitized upconverters that exploits the solid nature of the material. We show that an upconversion model system with molecules distributed as clusters outperforms a system with a random distribution of molecules, as used in current upconverters. Our simulations reveal a high potential for improvement of upconverter systems by exploring different structural configurations of the molecules. The implementation of advanced structures can push the performance of solid upconverters further towards the theoretical limit and a step closer to technological application of low power upconversion.