On the nature of two-photon transitions for a collection of molecules in a Fabry–Perot cavity

Author:

Zhou Zeyu1ORCID,Chen Hsing-Ta12ORCID,Sukharev Maxim34ORCID,Subotnik Joseph E.1ORCID,Nitzan Abraham15ORCID

Affiliation:

1. Department of Chemistry, University of Pennsylvania 1 , 231 South 34th Street, Philadelphia, Pennsylvania 19104, USA

2. Department of Chemistry and Biochemistry 2 , 251 Nieuwland Science Hall, Notre Dame, Indiana 46556, USA

3. Department of Physics, Arizona State University 3 , Tempe, Arizona 85287, USA

4. College of Integrative Sciences and Arts, Arizona State University 4 , Mesa, Arizona 85212, USA

5. Department of Physical Chemistry, School of Chemistry, The Raymond and Beverly Sackler Faculty of Exact Sciences and The Sackler Center for Computational Molecular and Materials Science, Tel Aviv University 5 , Tel Aviv 6997801, Israel

Abstract

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.

Funder

Basic Energy Sciences

National Science Foundation

Air Force Office of Scientific Research

Publisher

AIP Publishing

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