Theory for Nonlinear Spectroscopy of Vibrational Polaritons

The Journal of Physical Chemistry Letters
Raphael F RibeiroJoel Yuen-Zhou

Abstract

Molecular polaritons have gained considerable attention due to their potential to control nanoscale molecular processes by harnessing electromagnetic coherence. Although recent experiments with liquid-phase vibrational polaritons have shown great promise for exploiting these effects, significant challenges remain in interpreting their spectroscopic signatures. We develop a quantum-mechanical theory of pump-probe spectroscopy for this class of polaritons based on the quantum Langevin equation and the input-output theory. Comparison with recent experimental data shows good agreement upon consideration of the various vibrational anharmonicities that modulate the signals. Finally, a simple and intuitive interpretation of the data based on an effective mode-coupling theory is provided. Our work provides a solid theoretical framework to elucidate nonlinear optical properties of molecular polaritons as well as to analyze further multidimensional spectroscopy experiments on these systems.

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Citations

Oct 13, 2018·Chemical Science·Raphael F RibeiroJoel Yuen-Zhou
Oct 17, 2019·The Journal of Chemical Physics·Federico J Hernández, Felipe Herrera
Jul 19, 2020·Proceedings of the National Academy of Sciences of the United States of America·Tao E LiAbraham Nitzan
Mar 17, 2020·The Journal of Chemical Physics·Felipe Herrera, Jeffrey Owrutsky
Feb 17, 2021·The Journal of Chemical Physics·Tamás SzidarovszkyÁgnes Vibók
Jan 13, 2021·Nature Communications·Andrea B GraftonJeffrey C Owrutsky
Mar 10, 2021·The Journal of Chemical Physics·Tao E LiJoseph E Subotnik
Mar 19, 2020·The Journal of Physical Chemistry Letters·Courtney A DelPoGregory D Scholes
Jul 21, 2021·The Journal of Physical Chemistry Letters·Xinyang LiPengfei Huo
Jul 27, 2021·The Journal of Physical Chemistry. B·Justin D ErwinJames V Coe
Jul 4, 2019·The Journal of Physical Chemistry. a·Bo XiangWei Xiong
Jul 16, 2019·The Journal of Physical Chemistry Letters·Zhedong ZhangShaul Mukamel
Nov 2, 2019·Nano Letters·Mohammad RamezaniJaime Gómez Rivas
Nov 19, 2021·The Journal of Physical Chemistry Letters·Francesca FassioliGregory D Scholes

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