We use scanning tunneling microscopy to study the initial stages of ultrahi
gh-vacuum chemical vapor deposition of Al on the Si(001)-(2 x 1) surface fr
om dimethylaluminum hydride (DMAH). At room tempera ture (300 K), the DMAH
molecules adsorb intact in seven distinct configurations, which we identify
as the DMAH dimer. After annealing above 525 K the molecules decompose int
o H, CH3, and Al. By contrast, the majority of impinging DMAH molecules cra
ck when dosed on a surface as cool as 350 K. Dosing at the industrial proce
ss temperature of 575 K produces the cleanest aluminum growth. [S0163-1829(
99)07011-3].