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Abstract The photo-induced dissociative-ionization of lanthanide complexes Ln(hfac)₃(Ln = Pr, Er, Yb) is studied using intense ultrafast transform limited (TL) and linearly chirped laser pulses in a time-of-flight (TOF) mass spectrometry setup. Various fluorine and Ln-containing high-mass fragments were observed in this experiment, including the molecular parent ion, which have not been seen with previous studies relying on relatively long-duration laser pulses (i.e., ns or longer). These new high-mass observations provide important formerly missing information for deducing a set of photo-fragmentation mechanistic pathways for Ln(hfac)₃. An overall ultrafast control mechanism is proposed by combining insights from earlier studies and the fragments observed in this research to result in three main distinct photo-fragmentation processes: (a) ligand-metal charge transfer, (b) CF₃elimination, and (c) C-C bond rotation processes. We conclude that ultrafast dissociative-ionization could be a promising technique for generating high-mass fragments for potential use in material science applications.