Correlated photons inspire abundance of metrology-related platforms, which benefit from quantum (anti-) correlations and outperform their classical counterparts. While these mainly focus on entanglement, the role of photon exchange phase and degree of distinguishability has not been widely used in quantum applications. Using an interferometric setup, we theoretically show that, when a two-photon wave function is coupled to matter, it is encoded with “which pathway?” information even at low-degree of entanglement. An interferometric protocol, which enables phase-sensitive discrimination between microscopic interaction histories (pathways), is developed. We find that quantum light interferometry facilitates utterly different set of time delay variables, which are unbound by uncertainty to the inverse bandwidth of the wave packet. We illustrate our findings on an exciton model system and demonstrate how to probe intraband dephasing in the time domain without temporally resolved detection. The unusual scaling of multiphoton coincidence signals with the applied pump intensity is discussed.
Nonlinear quantum interferometric spectroscopy with entangled photon pairs
We develop closed expressions for a time-resolved photon counting signal induced by an entangled photon pair in an interferometric spectroscopy setup. Superoperator expressions in Liouville-space are derived that can account for relaxation and dephasing induced by coupling to a bath. Interferometric setups mix matter and light variables non-trivially, which complicates their interpretation. We provide an intuitive modular framework for this setup that simplifies its description. Based on the separation between the detection stage and the light–matter interaction processes, we show that the pair entanglement time and the interferometric time-variables control the observed physics time scale. Only a few processes contribute in the limiting case of small entanglement time with respect to the sample response, and specific contributions can be singled out.
- Award ID(s):
- 1953045
- Publication Date:
- NSF-PAR ID:
- 10363458
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 156
- Issue:
- 9
- Page Range or eLocation-ID:
- Article No. 094202
- ISSN:
- 0021-9606
- Publisher:
- American Institute of Physics
- Sponsoring Org:
- National Science Foundation
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