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Inclination of unpatterned, linearly polarized illumination in the plane of the electric field oscillation effected increased directional feature alignment and decreased off-axis order in Se–Te deposits generated by inorganic phototropic growth relative to that produced using normal incidence. Optically based growth simulations reproduced the experimental results indicating a photonic basis for the morphology change. Modeling of the light scattering at the growth interface revealed that illumination inclination enhances scattering that localizes the optical field along the polarization plane and suppresses cooperativity in defect-driven scattering. Thus, the symmetry of the deposited structures increased as the asymmetry of the illumination increased, as measured by the inclination of the illumination incidence away from the surface normal. 

The role of nucleation was investigated during phototropic growth of Se–Te. Under low levels of mass deposition (mass equivalent of −3.75 mC cm −2 of charge passed) that produced small nucleate spacings, patterns in photoelectrochemically deposited Se–Te films converged at relatively earlier levels of mass deposition and ultimately exhibited higher pattern fidelity throughout pattern development as compared to pattern formation from larger initial nucleate spacings. Consistently, use of an applied striking potential during very early levels of mass deposition produced more spatially random dark-phase electrodeposited nucleates and led to phototropic Se–Te photoelectrodeposited films that exhibited improved pattern fidelity relative to depositions performed with no striking step. Collectively, the data indicate that increases in randomness and spatial disorder of the dispersion of the initial nucleates produces increases in the fidelity and spatial order in the resulting phototropically grown electrodeposits. 

Inorganic phototropic growth using only spatially conformal illumination generated Se–Cd films that exhibited precise light-defined mesoscale morphologies including highly ordered, anisotropic, and periodic ridge and trench nanotextures over entire macroscopic substrates. Growth was accomplished via a light-induced electrochemical method using an optically and chemically isotropic solution, an unpatterned substrate, and unstructured, incoherent, low-intensity illumination in the absence of chemical directing agents or physical templates and masks. The morphologies were defined by the illumination inputs: the nanotexture long axes aligned parallel to the optical E-field vector, and the feature sizes and periods scaled with the wavelength. Optically based modeling of the growth closely reproduced the experimental results, confirming the film morphologies were fully determined by the light–matter interactions during growth. Solution processing of the Se–Cd films resulted in stoichiometric, crystalline CdSe films that also exhibited ordered nanotextures, demonstrating that inorganic phototropic growth can effect tunable, template-free generation of ordered CdSe nanostructures over macroscopic length scales.