  Understanding the pathways to crystallization during the deposition of a
vapor phase on a cold solid substrate is of great interest in industry, e.g.,
for the realization of electronic devices made of crystallites-free glassy
materials, as well as in the atmospheric science in relation to ice nucleation
and growth in clouds. Here we numerically investigate the nucleation process
during the deposition of a glassformer by using a Lennard-Jones mixture, and
compare the properties of this nucleation process with both its quenched
counterpart and the bulk system. We find that all three systems homogeneously
nucleate crystals in a narrow range of temperatures. However, the deposited
layer shows a peculiar formation of ordered domains, promoted by the faster
relaxation dynamics toward the free surface even in an as-deposited state. In
contrast, the formation of such domains in the other systems occurs only when
the structures are fully relaxed by quenching. Furthermore, the nucleus
initially grows in an isotropic symmetrical manner, but eventually shows sub-3D
growth due to its preference to grow along the basal plane, irrespective of the
layer production procedure.
