I investigate energy transfer in a donor-acceptor pair beyond weak system-bath coupling. I identify a transition from coherent to incoherent dynamics with increasing temperature, due to multiphonon effects not captured by a standard weak-coupling treatment. The crossover temperature has a marked dependence on the degree of spatial correlation between fluctuations experienced at the two system s...

We show how both the subwavelength confinement associated with surface plasmons and the one-dimensional character of plasmonic waveguides can be exploited to enhance the coupling between quantum emitters. Resonance energy transfer and the phenomenon of superradiance are investigated in three different waveguiding schemes (wires, wedges, and channels) by means of the Finite Element Method. We al...

Based on Spin-Forbidden Resonance Energy Transfer Angel A. Martı́,† Cindy A. Puckett,‡ Joanne Dyer,† Nathan Stevens,† Steffen Jockusch,† Jingyue Ju,|,⊥ Jacqueline K. Barton,‡ and Nicholas J. Turro*,†,⊥ Department of Chemistry and Department of Chemical Engineering, Columbia UniVersity, New York, New York 10027, DiVision of Chemistry and Chemical Engineering, California Institute of Technology, P...

Photosynthetic proteins have evolved over billions of years so as to undergo optimal energy transfer to the sites of charge separation. On the basis of spectroscopically detected quantum coherences, it has been suggested that this energy transfer is partially wavelike. This conclusion depends critically on the assignment of the coherences to the evolution of excitonic superpositions. We demonst...

We extend the exchange fluctuation theorem for energy exchange between thermal quantum systems beyond the assumption of molecular chaos, and describe the nonequilibrium exchange dynamics of correlated quantum states. The relation quantifies how the tendency for systems to equilibrate is modified in high-correlation environments. In addition, a more abstract approach leads us to a "correlation f...

Recent theoretical studies show that decoherence process can enhance transport efficiency in quantum systems. This effect is known as environment-assisted quantum transport (ENAQT). The role of ENAQT in optimal quantum transport is well investigated; however, it is less known how robust ENAQT is with respect to variations in the system or its environment characteristic. Toward answering this qu...

The optimized mean-trajectory (OMT) approximation is a semiclassical method for computing vibrational response functions from action-quantized classical trajectories connected by discrete transitions representing radiation-matter interactions. Here we apply this method to an anharmonic chromophore coupled to a harmonic bath. A forward-backward trajectory implementation of the OMT method is desc...

Both S(1) and T(1) energy transfer rates (porphyrin → cluster) increase from mono- to di- to tetracarboxylate[tetraphenyl-(zinc)porphyrin] adducts with [Pd(3)(dppm)(3)(CO)](2+) clusters.

The synthesis, structure, and photophysical properties of a new family of trinuclear CuRe(2) chromophore-quencher complexes having the general form [Cu(pyacac)(2)(Re(bpy')(CO)(3))(2)](OTf)(2) (where pyacac = 3-(4-pyridyl)-acetylacetonate and bpy' = 4,4'-5,5'-tetramethyl-2,2'-bipyridine (tmb, 1), 4,4'-dimethyl-2,2'-bipyridine (dmb, 2), 2,2'-bipyridine (bpy, 3), 4,4'-dichloro-2,2'-bipyridine (dcl...

proton transfer (pt) and methyl group transfer (mgt) occurring in small biomimetic systems, formamide-formamidic acid (fa-fi), and n-formyl-n-methylformamide-(e)-methyl n-formylformimidate (nmfa-nmfi) are investigated in the gas phase and in single-walled carbon nanotubes by using the density functional theory and the oniom approach. it is shown that pt reaction is disfavoured in single-walled ...