Structure, Reactivity, and Fragmentation of Small Multi-Charged Methane Clusters

The Journal of Physical Chemistry. a
A Sanaa ZaagM Hochlaf

Abstract

Small methane clusters (CH4)n are irradiated using intense femtosecond laser excitation at 624 nm. The ionized species and those resulting from their fragmentation are detected via time-of-flight mass spectrometry (TOF MS). We find evidence of bound, multiply charged methane molecules and clusters resulting from Coulomb explosion upon exposure to highly energetic, ultrafast radiation. The assignment of the mass spectra is done after first-principles calculations (at the (R)MP2/aug-cc-pVXZ (X = D,T) level) on the charged (CH4)n(q+) clusters (n = 1-4, q = 1-4). We also considered the cluster stabilities and fragments that may result from intracluster molecular reactivity. Complex intracluster ion-molecule reactions induced by photoionization are expected to occur. Interestingly, we show that multi charged small methane clusters undergo intracluster reactions and fragmentations which are different from those observed for isolated methane ions or for large ionized methane clusters.

References

Jun 4, 2008·Physical Review Letters·Sasi PalaniyappanB C Walker
Nov 6, 2009·Proceedings of the National Academy of Sciences of the United States of America·Richard A Himes, Kenneth D Karlin
Jun 4, 2011·Physical Chemistry Chemical Physics : PCCP·Scott G SayresA W Castleman
Jun 10, 2011·Angewandte Chemie·Helmut Schwarz
Jul 16, 2011·Physical Chemistry Chemical Physics : PCCP·V BritesM Hochlaf
Aug 10, 2011·The Journal of Chemical Physics·Scott G SayresA W Castleman
Dec 14, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Christian LeidlmairPaul Scheier

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Citations

Jul 27, 2017·Physical Chemistry Chemical Physics : PCCP·Majdi Hochlaf
Dec 9, 2020·Physical Chemistry Chemical Physics : PCCP·Lukas TiefenthalerOlof Echt
Mar 18, 2021·The Journal of Physical Chemistry. a·Roberto DonosoPatricio Fuentealba

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