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arXiv · 1711.11222

Revealing Hidden Vibration Polariton Interactions by 2D IR Spectroscopy

Bo Xiang·Raphael F. Ribeiro·Adam D. Dunkelberger·Jiaxi Wang·Yingmin Li·Blake S. Simpkins·Jeffrey C. Owrutsky·Joel Yuen-Zhou·Wei Xiong
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Abstract

We report the first experimental two-dimensional infrared (2D IR) spectra of novel molecular photonic excitations - vibrational-polaritons. The application of advanced 2D IR spectroscopy onto novel vibrational-polariton challenges and advances our understanding in both fields. From spectroscopy aspect, 2D IR spectra of polaritons differ drastically from free uncoupled molecules; from vibrational-polariton aspects, 2D IR uniquely resolves hybrid light-matter polariton excitations and unexpected dark states in a state-selective manner and revealed hidden interactions between them. Moreover, 2D IR signals highlight the role of vibrational anharmonicities in generating non-linear signals. To further advance our knowledge on 2D IR of vibrational polaritons, we develop a new quantum-mechanical model incorporating the effects of both nuclear and electrical anharmonicities on vibrational-polaritons and their 2D IR signals. This work reveals polariton physics that is difficult or impossible to probe with traditional linear spectroscopy and lays the foundation for investigating new non-linear optics and chemistry of molecular vibrational-polaritons.

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Bo Xiang, Raphael F. Ribeiro, Adam D. Dunkelberger, Jiaxi Wang, Yingmin Li, Blake S. Simpkins, Jeffrey C. Owrutsky, Joel Yuen-Zhou, Wei Xiong. 2017-11-30. Revealing Hidden Vibration Polariton Interactions by 2D IR Spectroscopy. https://arxiv.org/abs/1711.11222

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