期刊
JOURNAL OF CHEMICAL PHYSICS
卷 116, 期 21, 页码 9333-9340出版社
AMER INST PHYSICS
DOI: 10.1063/1.1473653
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We carried out a wavelength-dependent homodyne and heterodyne transient grating (TG) studies on a resonant system, rhodamine 640 in dimethylsulfoxide, with a simplified diffractive optics method. The real and imaginary components of the third-order molecular polarization at different excitation wavelengths have a similar longtime decay (>200 fs), while the amplitude of the real component is strongly wavelength dependent. The nonresonant solvent and the resonant solute contributions to the third-order polarization are found to have a similar magnitude in a dilute solution. The interference of the wavelength-dependent resonant solute contributions with the nonresonant solvent contribution is found to be crucial to properly understand the wavelength dependence of the initial dynamics in homodyne TG and other four-wave mixing techniques. Such an interference effect is further confirmed by concentration-dependent homodyne TG measurements. (C) 2002 American Institute of Physics.
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