Abstract

In this paper we characterize the ultrafast fragmentation in electronically excited Fe(CO)2(NO)2 and CpMn(CO)3 by means of femtosecond time-resolved spectroscopy combined with mass spectrometry. From the transient two-color multi-photon ionization data, it was possible to record the transients of the parent molecule ions and their photofragment ions. The experimentally observed decay times indicated an ultrafast loss of the first ligands (sub-100 fs decay times). Further we performed a feedback control experiment on the photofragmenting CpMn(CO)3 molecular system in order to maximize the yield of desired ionic products through pulse modulation. The shape of the pulses obtained from optimization reflect well the intrinsic molecular dynamics during photofragmentation and the change of the CpMn(CO)+/CpMn(CO)3 + ratio shows a clear evidence for the capability of the optimization method to find tailor-made system-specific pulses.

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