Complementary scanning tunneling microscopy and surface infrared measuremen
ts show that H reacts strongly with Al(111), producing a variety of new ala
ne (aluminum hydride) surface species. Alane oligomers, ranging in size fro
m the monomer to 30-mers, form through a sequence of surface etching and co
ndensation reactions. Atomic hydrogen initiates production by extracting al
uminum atoms from the surface lattice to create mobile monohydride monomers
(ad-Al-H), which predominate in the low-coverage regime. At higher hydroge
n coverages, multihydride oligomers form in coexistence with the ad-Al-H. T
hese alane oligomers are more thermally stable, remaining on the surface at
room temperature, where they are directly imaged. The mass transfer of alu
minum to surface alanes is discussed in relationship to alane stoichiometry
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