Quantum Materials Corp. (fka QTMM)

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Theory for Nonlinear Spectroscopy of Vibrational Polaritons

Raphael F. Ribeiro, Adam D. Dunkelberger, Bo Xiang, Wei Xiong, Blake S. Simpkins, Jeffrey C. Owrutsky, Joel Yuen-Zhou
Subjects: Quantum Physics (quant-ph); Chemical Physics (physics.chem-ph)


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. In this letter, we develop a quantum-mechanical theory of pump-probe spectroscopy for this class of polaritons based on the quantum Langevin equations 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.

https://arxiv.org/abs/1711.11242