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Physics Letters A

Dark-state mechanism for the long-time transfer of excitations in a donor–acceptor system

Jing Lu, Lan Zhou, H. C. Fu

Published Mar 21, 2013• 2 citations
Publisher
DOI
10.1016/j.physleta.2013.03.024

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The rates of exciton transfer within dyads of perylene diimide and terrylene diimide connected by oligophenylene bridge units have been shown to deviate significantly from those of Förster's resonance energy transfer theory, according to single molecule spectroscopy experiments. The present work provides a detailed computational and theoretical study investigating the source of such discrepancy. Electronic spectroscopy data are calculated by time-dependent density function theory and then compared with experimental results. Electronic couplings between exciton donor and acceptor are estimated based on both transition density cube method and transition dipole approximation. These results confirm that the delocalization of exciton to the bridge parts contribute to significant enhancement of donor-acceptor electronic coupling. Mechanistic details of exciton transfer are examined by estimating the contributions of the bridge electronic states, vibrational modes of the dyads commonly coupled to both donor and acceptor, inelastic resonance energy transfer mechanism, and dark exciton states. These analyses suggest that the contribution of common vibrational modes serves as the main source of deviation from Förster's spectral overlap expression.
Abstract Abstractauthoren We theoretically investigate the energy transfer between concentrically arranged nanostructures by using a quantum‐entanglement measure. The model system is formed in double concentric circles of interacting two‐level systems, where the outer circle is the donor and the inner circle is the acceptor. We show that a rapid energy transfer can be achieved by utilizing a strongly entangled donor–acceptor state. First, we clarify that a selection rule exists in the energy‐transfer process; the energy transfer from the donor to the acceptor occurs only between the energy eigenstates having the same rotational symmetry. Next, in terms of the analysis of the degree of quantum entanglement, we clarify that the quantum entanglement is strongly formed between the donor and acceptor with higher rotational symmetry and the energy transfer process dominates in the donor–acceptor entangled state. Finally, we show that a rapid energy transfer can occur by efficiently exciting the entangled state with the help of thermal fluctuation at room temperature. From the aspect of device applications, this mechanism has the advantage over the conventional energy‐transfer process in natural photosynthetic systems because no spatial disorder and fluctuation are required. Application to photonic devices using the nanomaterial is also discussed.
Summary form only given. The migration of excitation energy within dielectric crystals doped with lanthanide ions is a rich area for the study of mechanisms involving both conventional pairwise resonance energy transfer and more complex many-body effects. Within the framework of molecular quantum electrodynamics, we present a delineation of systems undergoing simultaneous transfer from two pre-excited donor ions to a single ground-state acceptor, termed three-centre energy pooling. Calculations lead to the identification of two competing mechanisms of transfer co-existing in each system-one cooperative pathway where the excitation is transferred directly to the acceptor from both donors, alongside an accretive mechanism where the excitation energy of one donor is accrued by a second, with net transfer to the acceptor ensuing.