Discriminatory Resonance Energy Transfer Mediated by a Third Molecule

Salam, A.

doi:10.1021/acs.jpca.0c11053

Cited by 5 publications

(2 citation statements)

References 52 publications

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“…(10). Here, we would like to emphasize that the investigation on the TC model can provide an alternative point of view on the theory of resonance energy transfer based on molecular quantum electrodynamics [64][65][66][67][68] because resonance energy transfer is associated with the dyadic Green's functions [33,36,38] in the GSDs.…”

Section: Discussionmentioning

confidence: 99%

Tavis-Cummings model revisited: A perspective from macroscopic quantum electrodynamics

Chuang

Lee²,

Hsu³

2022

Front. Phys.

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The Tavis-Cummings (TC) model has been widely used to investigate the collective coupling effect in hybrid light-matter systems; however, the TC model neglects the effect of a dielectric environment (the spectral structure of photonic bath), and it remains unclear whether the TC model can adequately depict the light-matter interaction in a non-homogeneous, dispersive, and absorbing medium. To clarify the ambiguity, in this work, we first connect the macroscopic quantum electrodynamics and the TC model with dissipation. Based on the relationship between these two theoretical frameworks, we develop a guideline that allows us to examine the applicability of the TC model with dissipation. The guideline states that if 1) the generalized spectral densities are independent of the positions of molecules and 2) the generalized spectral densities resemble a Lorentzian function, then the hybrid light-matter system can be properly described by the TC model with dissipation. In order to demonstrate how to use the guideline, we examine the position dependence and the lineshape of the generalized spectral densities in three representative systems, including a silver Fabry-Pérot cavity, a silver surface, and an aluminum spherical cavity. We find that only the aluminum spherical cavity meets the two conditions, i.e., position independence and Lorentzian lineshape, required for the utilization of the dissipative TC model. Our results indicate that the use of the TC model with dissipation to study the collective coupling effect should be done with care, providing an important perspective on resonance energy transfer and polariton chemistry.

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Section: Discussionmentioning

confidence: 99%

Tavis-Cummings model revisited: A perspective from macroscopic quantum electrodynamics

Chuang

Lee²,

Hsu³

2022

Front. Phys.

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“…We then consider the donor-acceptor pair first immersed inside a chiral medium with known handedness. In the limit of a very dilute gas the surrounding medium is rather modelled by its individual constituents [20][21][22][23][24][25][26][27]. We therefore consider lastly the discrimination in the presence of a single additional chiral molecule [28], called mediator.…”

Section: Introductionmentioning

confidence: 99%

Discriminatory resonance energy transfer mediated by a chiral environment

Franz,

Yoshi Buhmann,

Salam

2024

New J. Phys.

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In this study, we delve into the crucial influence of and enhancement by chiral environments on the discriminatory capabilities of RET. Firstly, we scrutinize the impact of a macroscopic chiral medium enveloping the interacting molecules; secondly, we probe the effect of a chiral mediating molecule in close proximity to the system.Importantly, our findings demonstrate that chiral environments not only modulate pre-existing discriminatory effects but also introduce novel mechanisms for discrimination. Central to our research is the application of an innovative model for chiral local-field corrections, which unveils a remarkable distance-dependent inversion of the discrimination dynamics. Our study extends beyond the confines of any specific molecular system, offering a comprehensive discussion of these diverse effects, thereby providing insights with broader implications.Finally, we present a comparative analysis across all studied systems, illustrating our insights by employing 3-methyl-cyclopentanone as an example molecule.

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Two bridge-particle-mediated RET between chiral molecules

Salam

2022

The Journal of Chemical Physics

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The problem of resonance energy transfer between a pair of chiral molecules mediated by two electrically polarizable bridging particles is solved using molecular QED theory. In this framework a single virtual photon propagates between any two-coupled entities and is responsible for the conveyance of excitation energy from emitter to absorber. Electric dipole and quadrupole, and magnetic dipole couplings linear in the Maxwell fields are employed for donor and acceptor, while each mediator scatters two virtual photons and responds quadratically to the electric displacement field via its electric dipole polarizability. This enables fourth-order diagrammatic perturbation theory to be used to compute the probability amplitude for the process. Individual multipole moment contributions to the Fermi golden rule rate are then extracted for oriented and isotropic systems. Discriminatory transfer rates arise when either the donor or the acceptor are electric-magnetic dipole and the other has a pure multipole moment, or when both are chiral, with mixed electric dipole-quadrupole contributions vanishing in the fluid phase. The bridge-mediated transfer rate is found to be a maximum for a collinear geometry. Moreover, a multi-level model of the mediator is necessary for energy migration. Asymptotically limiting rates for arbitrary and collinear geometries are also obtained for one centre purely electric dipolar and the other purely quadrupolar, or both donor and absorber purely quadrupolar. Understanding is gained of radiationless and radiative transfer mechanisms between chiral moieties in a dielectric medium.

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Discriminatory Resonance Energy Transfer Mediated by a Third Molecule

Cited by 5 publications

References 52 publications

Tavis-Cummings model revisited: A perspective from macroscopic quantum electrodynamics

Tavis-Cummings model revisited: A perspective from macroscopic quantum electrodynamics

Discriminatory resonance energy transfer mediated by a chiral environment

Two bridge-particle-mediated RET between chiral molecules

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