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Title: Laser ablation synthesis of lanthanide oxide cluster ions incorporating a heterovalent metal

Abstract

Lanthanide (Ln) oxide cluster ions produced directly by excimer laser ablation of oxalates into vacuum were investigated by time-of-flight mass spectrometry. Whereas previous studies in our laboratory identified pure Ln{sub m}O{sub n}{sup +} and mixed Ln{sub m1}Ln`{sub m2}O{sub n}{sup +}, the present work focused on analogous clusters incorporating an alkaline earth (A) or transition (T) metal: [C@Ln{sub m}O{sub n}.@pAO]C{sup +} and [C@Ln{sub m}O{sub n}.TO{sub 2}]C{sup +} (Ln = La, Tb, Ho or Yb; A = Ca or Sr; T = Ta, Zr, or Hf). The formation of atomically combined clusters from physical mixtures of a solid lanthanide oxalate with a heterovalent metal oxide supports gas-phase coalescence as the dominant formation mechanism (vs direct cluster ejection). The stoichiometries and abundance distributions of the bimetallic oxide cluster ions are interpreted in the context of their chemical and structural constitutions. Ion abundance maxima for [C@LnO.3AO]C{sup +} are consistent with an ionically bonded cuboid microlattice; this cubic structure type may also pertain to related binary Ln{sub m}O{sub n}{sup +}. Distinctive abundances (stabilities) of such compositions as [C@Ln{sub 3}O{sub 4}.@2AO]C{sup +} and [C@Ln{sub 5}O{sub 7}.@AO]C{sup +} suggest similar cuboid structures there. 29 refs., 4 figs., 1 tab.

Authors:
 [1]
  1. Oak Ridge National Lab., TN (United States)
Publication Date:
OSTI Identifier:
196645
DOE Contract Number:  
AC05-84OR21400
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry
Additional Journal Information:
Journal Volume: 100; Journal Issue: 2; Other Information: PBD: 11 Jan 1996
Country of Publication:
United States
Language:
English
Subject:
40 CHEMISTRY; 42 ENGINEERING NOT INCLUDED IN OTHER CATEGORIES; MOLECULAR IONS; SYNTHESIS; MASS SPECTRA; LASER RADIATION; USES; SOLID CLUSTERS; RARE EARTH COMPOUNDS; OXIDES; STOICHIOMETRY; ABUNDANCE; DISTRIBUTION; CRYSTAL STRUCTURE; TIME-OF-FLIGHT METHOD

Citation Formats

Gibson, J K. Laser ablation synthesis of lanthanide oxide cluster ions incorporating a heterovalent metal. United States: N. p., 1996. Web. doi:10.1021/jp951677p.
Gibson, J K. Laser ablation synthesis of lanthanide oxide cluster ions incorporating a heterovalent metal. United States. doi:10.1021/jp951677p.
Gibson, J K. Thu . "Laser ablation synthesis of lanthanide oxide cluster ions incorporating a heterovalent metal". United States. doi:10.1021/jp951677p.
@article{osti_196645,
title = {Laser ablation synthesis of lanthanide oxide cluster ions incorporating a heterovalent metal},
author = {Gibson, J K},
abstractNote = {Lanthanide (Ln) oxide cluster ions produced directly by excimer laser ablation of oxalates into vacuum were investigated by time-of-flight mass spectrometry. Whereas previous studies in our laboratory identified pure Ln{sub m}O{sub n}{sup +} and mixed Ln{sub m1}Ln`{sub m2}O{sub n}{sup +}, the present work focused on analogous clusters incorporating an alkaline earth (A) or transition (T) metal: [C@Ln{sub m}O{sub n}.@pAO]C{sup +} and [C@Ln{sub m}O{sub n}.TO{sub 2}]C{sup +} (Ln = La, Tb, Ho or Yb; A = Ca or Sr; T = Ta, Zr, or Hf). The formation of atomically combined clusters from physical mixtures of a solid lanthanide oxalate with a heterovalent metal oxide supports gas-phase coalescence as the dominant formation mechanism (vs direct cluster ejection). The stoichiometries and abundance distributions of the bimetallic oxide cluster ions are interpreted in the context of their chemical and structural constitutions. Ion abundance maxima for [C@LnO.3AO]C{sup +} are consistent with an ionically bonded cuboid microlattice; this cubic structure type may also pertain to related binary Ln{sub m}O{sub n}{sup +}. Distinctive abundances (stabilities) of such compositions as [C@Ln{sub 3}O{sub 4}.@2AO]C{sup +} and [C@Ln{sub 5}O{sub 7}.@AO]C{sup +} suggest similar cuboid structures there. 29 refs., 4 figs., 1 tab.},
doi = {10.1021/jp951677p},
journal = {Journal of Physical Chemistry},
number = 2,
volume = 100,
place = {United States},
year = {1996},
month = {1}
}