Off-Resonant Fifth-Order Response Function for Two-Dimensional Raman Spectroscopy of Liquidsand
- 30 April 2002
- journal article
- research article
- Published by American Physical Society (APS) in Physical Review Letters
- Vol. 88 (20), 207401
- https://doi.org/10.1103/physrevlett.88.207401
Abstract
The off-resonant fifth-order response functions for two-dimensional (2D) Raman spectroscopy of molecular liquids CS2 and H2O are investigated by using molecular dynamics calculation. This spectroscopy, able to deal with a phase space dynamics, shows the existence of nodal lines in several polarization tensor elements [see L. Kaufman et al., Phys. Rev. Lett. 88, 207402 (2002) for experimental results]. The nodal property is found to arise from the dynamical couplings among rotational modes, not accounted for in a normal mode picture. The effects of anharmonicities and "mode coupling through polarizability" are also investigated by comparing the 2D Raman signal with a constant temperature velocity reassignment echo method.Keywords
This publication has 32 references indexed in Scilit:
- Fifth-order electronically non-resonant Raman scattering: two-dimensional Fourier deconvolutionChemical Physics, 2001
- Polarization selectivity in fifth-order electronically nonresonant Raman scattering from CS2The Journal of Chemical Physics, 2001
- Separation of cascaded and direct fifth-order Raman signals using phase-sensitive intrinsic heterodyne detectionThe Journal of Chemical Physics, 2000
- Multidimensional Femtosecond Correlation Spectroscopies of Electronic and Vibrational ExcitationsAnnual Review of Physical Chemistry, 2000
- Diffractive optics based two-color six-wave mixing: phase contrast heterodyne detection of the fifth order Raman response of liquidsChemical Physics Letters, 2000
- Direct fifth-order electronically nonresonant Raman scattering from CS2 at room temperatureThe Journal of Chemical Physics, 2000
- Diffractive optics implementation of six-wave mixingOptics Letters, 2000
- Intrinsic cascading contributions to the fifth- and seventh-order electronically off-resonant Raman spectroscopiesThe Journal of Chemical Physics, 2000
- Fifth-order two-dimensional Raman spectra of CS2 are dominated by third-order cascadesThe Journal of Chemical Physics, 1999
- Two-dimensional femtosecond vibrational spectroscopy of liquidsThe Journal of Chemical Physics, 1993