Abstract
Significant debate surrounds the origin of nonlinear optical responses from cavity-coupled molecular vibrations. Several groups, including our own, have previously assigned portions of the nonlinear response to polariton excited-state transitions. Here, we report a new method to approximate two-dimensional infrared spectra under vibrational strong coupling, which properly accounts for inhomogeneous broadening. We find excellent agreement between this model and experimental results for prototypical systems exhibiting both homogeneous and inhomogeneous broadening. This work implies that reservoir excitation is solely responsible for all optical response measured after the polariton modes dephase and represents an important new method for predicting and interpreting the nonlinear optical response of molecular vibrational polaritons.
Published Version
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
