UV‐laser photodeposition has been used to predispose surfaces to pyrolytic chemical vapor deposition (CVD) of Al from triisobutylaluminum. Two laser beam (UV and IR) experiments indicate that the predisposition is due to the formation of a catalytic surface for heterogeneous chemistry. Time‐resolved transmission measurements indicate that a few photodeposited monolayers are sufficient to nucleate CVD growth. The technique may be generally useful for maskless patterned growth by CVD processes with large nucleation barriers.

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