Abstract
This paper presents a comprehensive study of the theory of entangled two-photon emission/absorption (E2P-EA) between a many-level cascade donor and a many-level acceptor (which could be quantum dots or molecules) using second-order perturbation theory and where the donor-acceptor pair is in a homogeneous but dispersive medium. To understand the mechanism of E2P-EA, we analyze how dipole orientation, radiative lifetime, energy detuning between intermediate states, separation distance, and entanglement time impact the E2P-EA rate. Our study shows that there are quantum interference effects in the E2P-EA rate expression that lead to oscillations in the rate as a function of entanglement time. Furthermore, we find that the E2P-EA rate for a representative system consisting of two quantum dots can be comparable to one-photon emission/absorption (OP-EA) when donor and acceptor are within a few nm. However, the E2P-EA rate falls off much more quickly with separation distance than does OP-EA.
| Original language | English (US) |
|---|---|
| Article number | 074103 |
| Journal | Journal of Chemical Physics |
| Volume | 159 |
| Issue number | 7 |
| DOIs | |
| State | Published - Aug 21 2023 |
Funding
This research was supported by NSF under Grant No. CHE-2055565. We thank K. Nasiri Avanaki for useful discussions.
ASJC Scopus subject areas
- General Physics and Astronomy
- Physical and Theoretical Chemistry