Vibrational two-photon resonance linewidths in liquid media

✍ Scribed by S.R.J. Brueck

• Publisher: Elsevier Science
• Year: 1977
• Tongue: English
• Weight: 476 KB
• Volume: 50
• Category: Article
• ISSN: 0009-2614
• DOI: 10.1016/0009-2614(77)80381-3

✦ Synopsis

An extension of thcJ-diffusion description of rotational motion is developed for the contribution of the rotation-vibration interaction to the linewidths and Iineshapes of polarized vibrational Raman scattering, two-photon absorption and twophoton-resonant four-wave mixing processes in liquid media. In the motional narrowing limit, which is appropriate for many mo-Ieculv liquids, a simple expression is &rived for the linewidth involving only known spectroscopic constants and a rotationaI correlation time which can be deduced from infrared or depolarized Raman scattering measurements. Comparison with e.yperimental results for liquid N2,02 and CO indicate that this process contributes significantly to the observed linewidths. The linewidths of two-photon (Raman) susceptibilities in simple cryogenic liquid media such as N2, O,, CO, are a topic of current interest [l-5]. From a fundamental viewpokt, the observed dephasing times (TZ ~75 ps for liquid N2, refs. [6,7] ) are as much as 12 orders of magnitude faster than the T1 times inferred from recent measurements of energy relaxation processes for these liquids (e.g. T1 ~56 + 10 s for liquid