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In this Letter we report our first results on femtosecond photofragment spectroscopy. The reaction studied is I-CN - [I-CN] -I + CN. A photolysis-and-probe scheme is used to measure the rate of the primary photodissociation of ICN under collisionless conditions. The CN buildup time is measured from these preliminary results to be 600 100 fs. These direct measurements for the time of bond breakage in ICN are discussed in relation to the dynamics of the recoil process of the reaction. IntroductionStudies of the dynamics of primary photofragmentation processes offer new opportunities for the direct viewing of the process of bond breakage, its dependence on the nature of the transition state, and the resultant internal states of the products. Information about (average) photodissociation lifetimes, t, has in the past been obtained from knowledge of the product angular distribution(s) and from the calculated average rotational period of the parent, Q, as is illustrated, for the case of ICN, in the pioneering work of Ling and Wilson.' To obtain, t, however, one

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public-access-plan). *Revised Manuscript with No Changes Marked Click here to download Revised Manuscript with No Changes Marked: AEJ_revision_R2_notmarked_03_2015.docx

We describe a single-sideband frequency demodulation scheme with large dynamic range which gives linear response and is capable of shot-noise-limited performance when used with time-resolved pump and probe, polarization, and three- and four-wave mixing spectroscopies.

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