Theory for polariton-assisted remote energy transfer

Du, Matthew; Martínez-Martínez, Luis A.; Ribeiro, Raphael F.; Hu, Zixuan; Menon, Vinod M.; Yuen-Zhou, Joel

doi:10.1039/c8sc00171e

Cited by 209 publications

(194 citation statements)

References 93 publications

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“…are the projections of the product normal modes on the oscillator of the N -th product; these scalings are the same as those obtained in our studies on polariton assisted energy transfer (PARET) [37].…”

Section: Theoretical Frameworksupporting

confidence: 64%

Resonant catalysis of thermally activated chemical reactions with vibrational polaritons

Campos-González-Angulo

2019

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Interaction between light and matter results in new quantum states whose energetics can modify chemical kinetics. In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number $$N$$ N of molecular transitions couple to each resonant cavity mode, yielding two hybrid light–matter (polariton) modes and a reservoir of $$N-1$$ N − 1 dark states whose chemical dynamics are essentially those of the bare molecules. This fact is seemingly in opposition to the recently reported modification of thermally activated ground electronic state reactions under VSC. Here we provide a VSC Marcus–Levich–Jortner electron transfer model that potentially addresses this paradox: although entropy favors the transit through dark-state channels, the chemical kinetics can be dictated by a few polaritonic channels with smaller activation energies. The effects of catalytic VSC are maximal at light–matter resonance, in agreement with experimental observations.

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Section: Theoretical Frameworksupporting

confidence: 64%

Resonant catalysis of thermally activated chemical reactions with vibrational polaritons

Campos-González-Angulo

2019

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“…[134,[154][155][156][157] VSC/ESC Controlled chemical reactivity with spatially-separated donor and acceptor molecules. [158,159] ESC Cavity-enhanced energy and charge transport with molecular ensembles.…”

Section: A Recent Experimental Progressmentioning

confidence: 99%

“…Among these results, the development of the Holstein-Tavis-Cummings (HTC) model of vibronic polaritons [75,134] has been particularly useful, as it has been successfully used to explain features in the optical signals of organic microcavities that were notoriously confusing, such as the apparent breakdown of reciprocity in the oscillator strengths in absorption and emission strengths over specific frequencies [88,195]. Further predictions of the HTC model regarding the nature of the lower polariton manifold were later confirmed using variational techniques [196,197], and applied in subsequent work on singlet fission [198] and long-range energy transfer [158].…”

Section: B Recent Theoretical Progressmentioning

confidence: 99%

Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

259

248

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This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared cavities. Using a microscopic quantum electrodynamics formulation, we discuss the competition between the collective cooperative dipolar response of a molecular ensemble and local dynamical processes that molecules typically undergo, including chemical reactions. We highlight some of the observable consequences of this competition between local and collective effects in linear transmission spectroscopy, including the formal equivalence between quantum mechanical theory and the classical transfer matrix method, under specific conditions of molecular density and indistinguishability. We also overview recent experimental and theoretical developments on strong and ultrastrong coupling with electronic and vibrational transitions, with a special focus on cavity-modified chemistry and infrared spectroscopy under vibrational strong coupling. We finally suggest several opportunities for further studies that may lead to novel applications in chemical and electromagnetic sensing, energy conversion, optoelectronics, quantum control and quantum technology.

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“…6 Theoretical considerations suggest that non-radiative processes that can couple light-matter polaritons especially in a dissipative fashion can play a role in the modification of the energy transfer. [19][20][21] The fundamental mechanism of energy transfer mediated by strongly confined light modes has also been experimentally tackled in nano-optical systems such as between two nanoemitters attached to microspheres. 22 Moreover, high finesse microcavities Figure 1.…”

Section: Introductionmentioning

confidence: 99%

Energy transfer and correlations in cavity-embedded donor-acceptor configurations

Reitz

Mineo

Genes

2018

Sci Rep

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The rate of energy transfer in donor-acceptor systems can be manipulated via the common interaction with the confined electromagnetic modes of a micro-cavity. We analyze the competition between the near-field short range dipole-dipole energy exchange processes and the cavity mediated long-range interactions in a simplified model consisting of effective two-level quantum emitters that could be relevant for molecules in experiments under cryogenic conditions. We find that free-space collective incoherent interactions, typically associated with sub- and superradiance, can modify the traditional resonant energy transfer scaling with distance. The same holds true for cavity-mediated collective incoherent interactions in a weak-coupling but strong-cooperativity regime. In the strong coupling regime, we elucidate the effect of pumping into cavity polaritons and analytically identify an optimal energy flow regime characterized by equal donor/acceptor Hopfield coefficients in the middle polariton. Finally we quantify the build-up of quantum correlations in the donor-acceptor system via the two-qubit concurrence as a measure of entanglement.

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Theory for polariton-assisted remote energy transfer

Abstract: A comprehensive theory is presented to mechanistically elucidate the long-range energy transfer between molecules strongly coupled to electromagnetic fields.

Cited by 209 publications

References 93 publications

Resonant catalysis of thermally activated chemical reactions with vibrational polaritons

Resonant catalysis of thermally activated chemical reactions with vibrational polaritons

Molecular polaritons for controlling chemistry with quantum optics

Energy transfer and correlations in cavity-embedded donor-acceptor configurations

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