INTRINSIC OPTICAL HETERODYNE-DETECTION OF A 2-DIMENSIONAL 5TH-ORDER RAMAN RESPONSE

Intrinsic optical heterodyne detection is applied to femtosecond two-d imensional (2-D) vibrational spectroscopy of the Raman active inter- a nd intramolecular modes of liquid CS, between 1 and 1000 cm(-1). Heter odyne detection is accomplished with a novel wave vector matching geom etry that allows detection of the cross term between the third and fif th order response, R-(3)R-(5). The increase in the bandwidth and sensi tivity through this detection technique will allow the measurement of 2-D temporal or spectral responses for a wide variety of systems in th is frequency range. (C) 1997 Elsevier Science B.V.