Characterizing interstate vibrational coherent dynamics of surface adsorbed catalysts by fourth-order 3D SFG spectroscopy

- First fourth order 3D SFG spectrum of molecular monolayer.
- Fourth order 3D SFG spectroscopy can better resolve the peak lineshapes of interstate vibrational coherences.
- Surface attachment does not disrupt interstate coherences but molecular/metal surface interactions induce additional homogenous dephasing pathways.