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INFRARED RESONANCE ENHANCED PHOTODISSOCIATION SPECTROSCOPY OF $Fe^{+}-(CO_{2})_{n}$ CLUSTERS

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Abstract

Mid-infrared $(2100-2900 cm^{-1})$ photodissociation spectra of mass selected $Fe^{+}-(CO_{2})_{n=2-6}$ clusters are presented. The observed fragmentation channels correspond to the loss of $CO_{2}$ molecules, their numbers depending on the infrared laser intensity. In low power condition, namely a few $mJ/cm^{2}$, clusters undergo simple evaporation of one $CO^{2}$ molecule, while at higher power (hundreds of $mJ/cm^{2}$), multi photon absorption leads to multiple fragment detection, ranking from $Fe^{+}-(CO_{2})_{n-1}$ to $Fe^{+}-(CO_{2})_{2}$. In the latter case, step-by-step solvent evaporation within the temporal width of the laser (8ns) is observed, reflecting that the dissociation rate constant is faster than a few nanosecond. Photodissociation spectra of these clusters show a general blue shift of the resonant $CO^{2}$ asymmetric stretch within the complexes, and this shift decreases as the cluster size increases, which is consistent with the lowering of the $Fe^{+}-(CO_{2})_{2}$ interaction at the expense of the solvation. Furthermore, weaker transitions are observed which could correspond to combination bands with low frequency mode of about $20 cm^{-1}$.

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