Resonant excitation transfer: A quantum electrodynamical study

Andrews, Davıd L.; Sherborne, Brad

doi:10.1063/1.451910

Cited by 98 publications

(80 citation statements)

References 15 publications

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“…In its QED formulation, this emerges as a second-order perturbational process mediated by intermolecular propagation of a virtual photon [8][9][10][11][12][13][14]. The advantage of such a quantum electrodynamical treatment is that it extends the traditional F~Srster theory of short-range (near-zone) dipole-dipole radiationless transfer to arbitrary A-B separations R, thus establishing a continuous connection with long-range (far-zone) radiative transfer.…”

Section: A* +B--a+b* (13)mentioning

confidence: 99%

“…For example, two species (A and B) initially in their ground electronic states can together be promoted to by the incident photon annihilated at A (B) is transferred to another molecule B (A) through a virtual photon [1][2][3][4][5][6][7]. Virtual photon coupling is a common feature of all bimolecular photophysical processes, other examples being resonance intermolecular transfer of excitation energy [8][9][10][11][12][13][14], bimolecular Raman scattering [15], bimolecular three-photon absorption [16], etc. Within such a classification, resonance energy transfer,…”

Section: Introductionmentioning

confidence: 99%

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Quantum electrodynamics of bimolecular multiphoton processes in the condensed phase

Juzeliūnas¹,

Andrews²

1995

Chemical Physics

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Bimolecular photophysics is an area that accommodates a wide range of pairwise interactions of molecules with radiation, including cooperative absorption and emission, and bimolecular scattering. In this paper a QED theory is developed to deal with bimolecular multiphoton processes without recourse to the usual dilute medium approximation. The theory is fully microscopic, taking explicit account of effects due to any surrounding molecular medium. To this end, the concept of medium-dressed photons (bath polaritons) has been adopted, extending both to the real incoming and outgoing photons and also to the virtual photons that carry an energy mismatch between participating molecules. Modifications of the bimolecular rates resulting from the influence of the medium originate in two ways. One, associated with the real photons, brings in the refractive indexes at the appropriate photon frequencies. All terms constituting the transition matrix element are subject to introduction of the same refractive factor for each absorbed or emitted photon. Another medium effect, due to the virtual photons, appears through the electromagnetic coupling tensor which experiences, inter alia, changes due to screening and local field factors. Here the refractive effects in each term relate to the appropriate mismatch frequencies. These frequencies generally lie in a different spectral region to the real photons, and may equally be situated in either transparent or absorbing areas. In the latter absorbing case, an exponential decay factor emerges in the coupling tensor, regularising the long-range R -2 contribution. That solves the problem of potentially infinite ensemble rates which arises in the dilute medium approximation.

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Section: A* +B--a+b* (13)mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Quantum electrodynamics of bimolecular multiphoton processes in the condensed phase

Juzeliūnas¹,

Andrews²

1995

Chemical Physics

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“…What are commonly called 'radiative' and 'radiationless' energy transfer are simply asymptotes of a unified electrodynamic mechanism. [11][12][13][14][15][16][17] In the case of electric dipole-allowed transitions the two distance regimes are characterized by an inverse-square dependence on distance in the wave-zone, inverse sixth power in the near-field. Over intermediate distances additional terms arise, giving rise to an overall distance dependence as exhibited in Fig.…”

Section: Introductionmentioning

confidence: 99%

On the conveyance of angular momentum in electronic energy transfer

Andrews

2010

Phys. Chem. Chem. Phys.

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When electronic excitation transfer occurs, it is of considerable interest to establish whether angular momentum can also be conveyed in the process. The question is prompted by a consideration that when the participating chromophores are atoms, ions, or molecular systems having high local symmetry, the electronic excited states that are involved are generally characterized not only by energy, but by angular momentum properties. Moreover, it is known that electron spin can be communicated between quantum dot exciton states. Resolving the general issue entails an electrodynamic representation exploiting irreducible tensor methods, the analysis being illustrated by application to energy transfer associated with a variety of multipolar transitions. The results exhibit novel connections between an angular momentum content of the electromagnetic coupling and a strongly varying distance dependence. It is concluded that the communication of angular momentum does not in general map unambiguously between a donor and energy acceptor.

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“…It is now known [2][3][4][5][6][7] that the Förster interaction is the short-range limit of a more general result given by a unified transfer theory -a theory that is valid over any distance, and which includes additional terms with inverse fourth power and inverse square dependences on separation. At large donor-acceptor separations, it emerges that the energy transfer is a radiative process involving the distinct emission and subsequent absorption of a photon.…”

Section: Introductionmentioning

confidence: 99%