Heterodyne detected fifth-order Raman response of liquid CS2:: 'Dutch Cross' polarization

The heterodyne detected fifth-order Raman response of liquid CS, was measured using the novel 'Dutch Cross' polarization configuration which provides suppression of lower order processes by several orders of magnitude. The experimental Dutch Cross results show solid agreement with recent molecular dynamics simulations. A three-color modification was also employed to address the possibility of two-photon resonance enhancement and it was found that such effects are negligible. The principle finding is that liquid CS2 quickly loses its rephasing ability (nuclear coherence peaks at 100 fs with a 1/e decay of 320 fs), and reflects the rapid loss in nuclear correlations and modal description of simple liquids. (C) 2003 Published by Elsevier Science B.V.