RESUMO
The processing of energy by transfer and redistribution, plays a key role in the evolution of dynamical systems. At the ultrasmall and ultrafast scale of nanosystems, quantum coherence could in principle also play a role and has been reported in many pulse-driven nanosystems (e.g. quantum dots and even the microscopic Light-Harvesting Complex II (LHC-II) aggregate). Typical theoretical analyses cannot easily be scaled to describe these general N-component nanosystems; they do not treat the pulse dynamically; and they approximate memory effects. Here our aim is to shed light on what new physics might arise beyond these approximations. We adopt a purposely minimal model such that the time-dependence of the pulse is included explicitly in the Hamiltonian. This simple model generates complex dynamics: specifically, pulses of intermediate duration generate highly entangled vibronic (i.e. electronic-vibrational) states that spread multiple excitons - and hence energy - maximally within the system. Subsequent pulses can then act on such entangled states to efficiently channel subsequent energy capture. The underlying pulse-generated vibronic entanglement increases in strength and robustness as N increases.
RESUMO
Light-harvesting bacteria Rhodospirillum photometricum were recently found to adopt strikingly different architectures depending on illumination conditions. We present analytic and numerical calculations which explain this observation by quantifying a dynamical interplay between excitation transfer kinetics and reaction center cycling. High light-intensity membranes exploit dissipation as a photoprotective mechanism, thereby safeguarding a steady supply of chemical energy, while low light-intensity membranes efficiently process unused illumination intensity by channeling it to open reaction centers. More generally, our analysis elucidates and quantifies the trade-offs in natural network design for solar energy conversion.
