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Molecular orientational mechanism during physical vapor deposition of various linear long-chain compounds has been interpreted on the basis of a classical nucleation theory modified for the anisotropic nucleus formation. In this model, the anisotropy of the surface energy is considered, and initial small nuclei with two fundamental orientations (normal and lateral) are assumed to be formed and dissociated repeatedly by the thermal energy. The critical energy of nucleus formation for each orientation is calculated as a function of the chemical-potential change of the system. The calculated results are similar to those observed for actual orientational phenomena of long-chain molecules at various chemical-potential changes; i.e., a higher substrate temperature and/or a lower deposition rate result/s in a higher degree of normal orientation.