Natural and artificial light harvesting processes have recently gained new interest. Signatures of long lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate,
as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton-vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.
We show that the influence of the shared phonon bath considered in H. Hossein-Nejad and G. D. Scholes, New J. Phys. 12, 065045 (2010) on the exciton transfer in a two-molecule system can be reproduced by that of an independent bath model.
In a network of interacting quantum systems achieving fast coherent energy transfer is a challenging task. While quantum systems are susceptible to a wide range of environmental factors, in many physical settings their interactions with quantized vib
rations, or phonons, of a supporting structure are the most prevalent. This leads to noise and decoherence in the network, ultimately impacting the energy-transfer process. In this work, we introduce a novel type of coherent energy-transfer mechanism for quantum systems, where phonon interactions are able to actually enhance the energy transfer. Here, a shared phonon interacts with the systems and dynamically adjusts their resonances, providing remarkable directionality combined with quantum speed- up. We call this mechanism phonon-induced dynamic resonance energy transfer and show that it enables long-range coherent energy transport even in highly disordered systems.
Considering a multi-pathway structure in a light-harvesting complex of photosynthesis, we investigate the role of energy-level mismatches between antenna molecules in transferring the absorbed energy to a reaction center. We find a condition in which
the antenna molecules faithfully play their roles: Their effective absorption ratios are larger than those of the receiver molecule directly coupled to the reaction center. In the absence of energy-level mismatches and dephasing noise, there arises quantum destructive interference between multiple paths that restricts the energy transfer. On the other hand, the destructive interference diminishes as asymmetrically biasing the energy-level mismatches and/or introducing quantum noise of dephasing for the antenna molecules, so that the transfer efficiency is greatly enhanced to near unity. Remarkably, the near-unity efficiency can be achieved at a wide range of asymmetric energy-level mismatches. Temporal characteristics are also optimized at the energy-level mismatches where the transfer efficiency is near unity. We discuss these effects, in particular, for the Fenna-Matthews-Olson complex.
We propose an operational quasiprobability function for qudits, enabling a comparison between quantum and hidden-variable theories. We show that the quasiprobability function becomes positive semidefinite if consecutive measurement results are descri
bed by a hidden-variable model with locality and noninvasive measurability assumed. Otherwise, it is negative valued. The negativity depends on the observables to be measured as well as a given state, as the quasiprobability function is operationally defined. We also propose a marginal quasiprobability function and show that it plays the role of an entanglement witness for two qudits. In addition, we discuss an optical experiment of a polarization qubit to demonstrate its nonclassicality in terms of the quasiprobability function.
