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Ultrafast reaction dynamics of electronically excited [ital [tilde A]] state of ammonia clusters

Journal Article · · Journal of Chemical Physics; (United States)
DOI:https://doi.org/10.1063/1.465752· OSTI ID:6487305
; ; ;  [1]
  1. Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802 (United States)
Femtosecond pump--probe techniques combined with a reflectron time-of-flight mass spectrometer are utilized to study the ultrafast reaction dynamics of the electronically excited [ital [tilde A]] state of ammonia clusters. All of the detected protonated cluster ions, (NH[sub 3])[sub [ital n]]H[sup +] [ital n]=2[minus]6, are observed to display two distinct features with respect to preselected pump--probe time delays; a fast decay, followed by a persistent ion signal leveling off to a finite nonzero value. The fast decay is attributed to a predissociation process; while an intracluster reaction, which leads to formation of long-lived intermediates (NH[sub 3])[sub [ital n]]NH[sub 4], is responsible for the nonzero falling off regime. The results provide conclusive experimental evidence that both an absorption--ionization--dissociation mechanism and an absorption--dissociation--ionization mechanism are operative in the [ital [tilde A]] state of ammonia clusters.
DOE Contract Number:
FG02-88ER60668; FG02-88ER60648
OSTI ID:
6487305
Journal Information:
Journal of Chemical Physics; (United States), Journal Name: Journal of Chemical Physics; (United States) Vol. 99:1; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English