Abstract
In this chapter, I discuss the application of two-dimensional infrared (2D IR) spectroscopy to understand the ultrafast dynamics of molecular vibrational polaritons. When molecular vibrational modes and photon cavity modes strongly couple to each other, they form hybridized quasiparticles, the so-called molecular vibrational polaritons. Polaritons thereby possess half-photon half-matter characters, which render them to inherit characters from both sides, e.g., lead to modified chemical reactions. It is pertinent to understand the ultrafast molecular dynamics of polaritons, in order to rationally design polariton-modified reactions. The intrinsic timescale of molecular vibrational and cavity modes makes polaritons evolve in ultrafast timescales, e.g. polaritons relax to dark modes in a few picosecond. Therefore, femtosecond vibrational spectroscopy is ideal to follow such dynamics. In this chapter, I provide an overview of femtosecond 2D IR spectroscopic studies from my group. I will first introduce the spectral interpretation. Then, I will show that the dynamics of molecular vibrational polaritons are different from the ones of their molecular counterparts, such as hot vibrational dynamics and intermolecular vibrational energy transfer. These distinct dynamics can serve as the foundation for further design of polariton-modified reactions.
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 call