Resonance energy flow dynamics of coherently delocalized excitons in biological and macromolecular systems: Recent theoretical advances and open issues

Abstract

Recent experimental and theoretical studies suggest that biological photosynthetic complexes utilize the quantum coherence in a positive manner for efficient and robust flow of electronic excitation energy. Clear and quantitative understanding of such suggestion is important for identifying the design principles behind efficient flow of excitons coherently delocalized over multiple chromophores in condensed environments. Adaptation of such principles for synthetic macromolecular systems has also significant implication for the development of novel photovoltaic systems. Advanced theories of resonance energy transfer are presented, which can address these issues. Applications to photosynthetic light harvesting complex systems and organic materials demonstrate the capabilities of new theoretical approaches and future challenges. C 2012 John Wiley & Sons, Ltd.

Generalised Marcus theory for multi-molecular delocalised charge transfer

“…The gMT electronic coupling factor |V αβ | 2 = | j,k c αj c * βk V jk | 2 includes a coherent sum involving electronic amplitudes in each of the donor and acceptor aggregates, allowing both constructive and destructive interference to affect the transfer rate. If the interferences is constructive, leading to enhanced transfer rates, we call the effect supertransfer, and if it is destructive, subtransfer, borrowing terminology from the similar problem of MC-FRET [28].…”

Time-resolved energy transfer from single chloride-terminated nanocrystals to graphene

“…Resonant energy transfer occurs via dipole coupling to the two-dimensional plane of graphene with a z -4 distance rate dependence. 6,[19][20][21] and n-butylamine ligands (0.6 nm in length), which maintain the solubility of the nanocrystals.…”

Impact of environmentally induced fluctuations on quantum mechanically mixed electronic and vibrational pigment states in photosynthetic energy transfer and 2D electronic spectra

“…[11][12][13][14][15][16] It has generally been assumed that electronic coherence decays sufficiently rapidly that it does not affect the nature of electronic energy transfer in photosynthetic light harvesting systems. Nevertheless, these recent experiments have attributed long-lived quantum beats to an electronic origin.…”