Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 11, Pages 3181-3188Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b00902
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- U.S. National Science Foundation [CHE-1760537]
- Office of the Provost
- Northwestern University Information Technology
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Inspired by the unique nonclassical character of two-photon interactions induced by entangled photons, we develop a new comprehensive Forster-type formulation for entangled-two-photon resonance energy transfer (E2PRET) mediated by inhomogeneous, dispersive, and absorptive media with any spacedependent and frequency-dependent dielectric function and with any size of donor/ acceptor. In our theoretical framework, two uncoupled particles are jointly excited by the temporally entangled field associated with two virtual photons that are produced by three-level radiative cascade decay in a donor particle. The temporal entanglement leads to frequency anticorrelation in the virtual photon's field, and vanishing of one of the time-ordered excitation pathways. The underlying mechanism leads to more than 3 orders of magnitude enhancement in the E2P-RET rate compared with the uncorrelated photon case. With the power of our new formulation, we propose a way to characterize E2P-RET through an effective rate coefficient K-E2p, introduced here. This coefficient shows how energy transfer can be enhanced or suppressed depending on rate parameters in the radiative cascade, and by varying the donor-acceptor frequency differences.
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