Subharmonic resonances in nonlinear spectroscopy
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Summary form only given. Most experiments in nonlinear spectroscopy are characterized in terms of the third order susceptibilities which exhibit a resonant character when the pump and probe frequencies wl, wsdiffer by the Raman frequency wR. Thus the scan of the four wave mixing signal as a function of wsyields the Raman resonance w - ws= wRwith a line width R. If the intensities of the pump and probe start to become large, higher order nonlinearities X(5), X(7), etc. become important. Consideration of these can lead to the fractional Raman resonances wl- ws= wR/n with a width rR/n, where n is an integer. Almost universal existence of such Raman resonances in nonlinear mixing experiments in any type of medium was demonstrated. Several models which are typically used to describe the vibrational Raman effect and electronic Raman effect were considered. Results for the nonlinearly generated signals which explicitly show the subharmonic Raman resonances were given. For understanding subharmonic Raman resonances at still higher intensities nonperturbative models for the calculation of the signals were developed. A fully quantized treatment of such resonances was given. The transient growth of the nonlinear signal in the region of subharmonic Raman resonances was also discussed.
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Digest on Nonlinear Optics: Materials, Phenomena and Devices
