Chiral sum-frequency (SF) spectroscopy that measures both the real and the imaginarycomponents of the SF spectral response was demonstrated for the first time. It was based on interferenceof the SF signal with a dispersionless SF reference. Solutions of 1,1‘-bi-2-naphthol (BN) were used asmodel systems, and their chiral SF spectra over the first exciton-split transitions were obtained. Chiralspectra are useful for determination of absolute configuration and conformation of chiral molecules.
