Laser ablation synthesis of lanthanide oxide cluster ions incorporating a heterovalent metal
Journal Article
·
· Journal of Physical Chemistry
- Oak Ridge National Lab., TN (United States)
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.
- DOE Contract Number:
- AC05-84OR21400
- OSTI ID:
- 196645
- Journal Information:
- Journal of Physical Chemistry, Journal Name: Journal of Physical Chemistry Journal Issue: 2 Vol. 100; ISSN JPCHAX; ISSN 0022-3654
- Country of Publication:
- United States
- Language:
- English
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