Intrinsic Optical Heterodyne Detection of a Two-Dimensional Fifth Order Raman Response

AUTHORS

Tokmakoff A. , Lang M.J. , Larsen D.S. , Fleming G.R. . Chemical Physics Letters. 1997 ; 272(1-2). 48-54

ABSTRACT

Intrinsic optical heterodyne detection is applied to femtosecond two-dimensional (2-D) vibrational spectroscopy of the Raman active inter- and intramolecular modes of liquid CS₂ between 1 and 1000 cm⁻¹. Heterodyne detection is accomplished with a novel wave vector matching geometry that allows detection of the cross term between the third and fifth order response, R⁽³⁾R⁽⁵⁾. The increase in the bandwidth and sensitivity through this detection technique will allow the measurement of 2-D temporal or spectral responses for a wide variety of systems in this frequency range.