Nonlinear Vibronic and Electronic Spectroscopy of Molecules in the Condensed Phase

点击翻译按钮获取中文摘要

The Experimental Physical Chemistry Program supports Andreas Albrecht of Cornell University in his continuing studies on the use of `noisy` light to achieve femtosecond scale time resolution in condensed phase spectroscopy using nanosecond pulses. The noisy light-based timing is formally generalized to nonlinear spectroscopies using a new diagrammatic technique. Focus is on second and third order nonlinear electrical susceptibilities. Two-dimensional array detection of the noisy light interferograms will be incorporated to shorten data acquisition by nearly two orders of magnitude. These new spectroscopic techniques will potentially lead to more accurate measurements of vibrational frequencies and shed light on relaxation processes and coherence transfer in polyatomic molecules in condensed phases. The very practical advantage of this technique is that noisy light spectra in the nanosecond time domain can probe dynamics approaching the femtosecond regime, without the need for (expensive) coherent femtosecond pulses.