Abstract
Inspired by the unique nonclassical character of two-photon interactions induced by entangled photons, we develop a new comprehensive Förster-type formulation for entangled-two-photon resonance energy transfer (E2P-RET) mediated by inhomogeneous, dispersive, and absorptive media with any space-dependent 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 KE2P, 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.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 3181-3188 |
| Number of pages | 8 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 10 |
| Issue number | 11 |
| DOIs | |
| State | Published - Jun 6 2019 |
Funding
This work was supported by the U.S. National Science Foundation under Grant No. CHE-1760537. This research was supported in part through the computational resources and staff contributions provided for the Quest high performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology.
ASJC Scopus subject areas
- General Materials Science
- Physical and Theoretical Chemistry