Abstract
This chapter presents time resolved high-resolution rotational Raman spectroscopy of cyclopropane and cyclobutane. Cycloalkanes exhibit no electric dipole moment and conventional microwave and infrared spectroscopies are not possible. From time resolved femtosecond Raman spectroscopy, a background free method, with a signal/noise ratio of 103 or better, it is possible to extract the rotational constants and their higher order centrifugal distortion constants with high accuracy. Moreover, the experiment is sensitive enough to probe the intensity distribution of Raman lines of molecules that show alternation of intensity due to spin statistics. The width of the recurrences is very sensitive to the population of the initial state; therefore, the temperature has to be known. To determine the rotational constants however it is sufficient to know an approximate or even to fit the temperature. Molecular beam experiments exclude collisional dephasing which is equivalent with a higher accuracy of the molecular constants.
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