Ultrafast Photofragmentation of Ln(hfac)3 with a Proposed Mechanism for forming High Mass Fluorinated Products

Author:

Chen Jiangchao,Xing Xi,Rey-de-Castro Roberto,Rabitz Herschel

Abstract

AbstractThe 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) CF3 elimination, 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.

Funder

National Science Foundation

U.S. Department of Energy

United States Department of Defense | United States Army | U.S. Army Research, Development and Engineering Command | Army Research Office

Publisher

Springer Science and Business Media LLC

Subject

Multidisciplinary

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