Doubly resonant IR-UV sum-frequency vibrational spectroscopy on molecular chirality.

We show theoretically and experimentally that for sum-frequency vibrational spectroscopy near electronic transitions, resonant enhancement of the chiral response can be much stronger than that of the achiral response. The doubly resonant spectrum selectively enhances the vibrational modes through their different electron-vibration couplings. The unusually strong resonant enhancement significantly improves sensitivity of chiral spectroscopy and allows detection of the chiral vibrational spectrum of a molecular monolayer for the first time.