Vibrational spectroscopy experiments were carried out in a home-built guided ion beam/ion trap/tandem time-of-flight (ToF) photofragmentation mass spectrometer described in detail elsewhere. Once generated via ESI, the ions were transported into a vacuum system and accumulated in a room temperature octopole ion trap. From here, the ions were transferred to an octopole ion trap mounted onto a closed-cycle cryocooler capable of operating between 3-310 K. The cryogenic ion vibrational predissociation (CIVP) spectra discussed in this work were collected as previously described. Briefly, buffer gas cooling of the clusters to the temperature of the ion trap encouraged the formation of "tagged" clusters whereby a single N 2 (40 -50 K) or D 2 (17 -20 K) molecule physisorbed onto the clusters. The tagged clusters were then extracted into the ToF stage and ions with the mass of interest were intersected by a tunable infrared (IR) laser pulse from an Nd:YAG pumped OPO/OPA system (LaserVision). Absorption of a single photon resonant with a vibrational transition of the cluster resulted in the desorption of the tags, thereby producing fragment ions that subsequently were mass separated and quantified by a reflectron mass spectrometer. The CIVP spectra of each cluster were generated by computing the ratio of the integrated intensity of the untagged fragment ions to sum of the integrated intensities of both the tagged parent and the untagged fragment ions, corrected for laser power, at each wavelength.