Highly
periodic, geometrically directed, anisotropic Se–Pb
films have been synthesized at room temperature from an isotropic
aqueous solution without the use of physical templates by photoelectrodeposition
using a series of discrete input illumination polarizations and wavelengths
from an unstructured, uncorrelated, incoherent light source. Dark
growth did not generate deposits with substantial long-range order,
but growth using unpolarized illumination resulted in an ordered,
nanoscale, mesh-type morphology. Linearly polarized illumination generated
Se–Pb deposits that displayed an ordered, highly anisotropic
lamellar pattern wherein the long axes of the lamellae were aligned
parallel to the light polarization vector. The pitch of the lamellar
features was proportional to the input light wavelength, as confirmed
by Fourier analysis. Full-wave electromagnetic and Monte Carlo growth
simulations that incorporated only the fundamental light–matter
interactions during growth successfully reproduced the experimentally
observed morphologies and quantitatively matched the pattern periodicities.
Electrochemical postprocessing of the as-deposited Se–Pb structures
resulted in the generation of stoichiometric, crystalline PbSe while
preserving the nanopatterned morphology, thus broadening the genus
of materials that can be prepared with controlled three-dimensional
morphologies through maskless photoelectrodeposition.