Energy transfer in N-component nanosystems enhanced by pulse-driven vibronic many-body entanglement

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.