On the nature of two-photon transitions for a collection of molecules in a Fabry–Perot cavity
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- University of Pennsylvania, Philadelphia, PA (United States)
- University of Pennsylvania, Philadelphia, PA (United States); Department of Chemistry and Biochemistry, Notre Dame, IN (United States)
- Arizona State University, Tempe, AZ (United States); Arizona State University, Mesa, AZ (United States)
- University of Pennsylvania, Philadelphia, PA (United States); Tel Aviv University (Israel)
Here, we investigate the effect of a cavity on nonlinear two-photon transitions of a molecular system and we analyze how such an effect depends on the cavity quality factor, the field enhancement, and the possibility of dephasing. We find that the molecular response to strong light fields in a cavity with a variable quality factor can be understood as arising from a balance between (i) the ability of the cavity to enhance the field of an external probe and promote multiphoton transitions more easily and (ii) the fact that the strict selection rules on multiphoton transitions in a cavity support only one resonant frequency within the excitation range. Although our simulations use a classical level description of the radiation field (i.e., we solve Maxwell–Bloch or Maxwell–Liouville equations within the Ehrenfest approximation for the field–molecule interaction), based on experience with this level of approximation in the past studies of plasmonic and polaritonic systems, we believe that our results are valid over a wide range of external probing.
- Research Organization:
- University of Pennsylvania, Philadelphia, PA (United States)
- Sponsoring Organization:
- Air Force Office of Scientific Research (AFOSR); U.S. National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- SC0019397
- OSTI ID:
- 2510486
- Journal Information:
- Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 160; ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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