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Published May 30, 2018 | Supplemental Material
Journal Article Open

Template-Free Synthesis of Periodic Three-Dimensional PbSe Nanostructures via Photoelectrodeposition


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.

Additional Information

© 2018 American Chemical Society. Received: March 15, 2018; Published: May 9, 2018. This work was supported by the "Light-Material Interactions in Energy Conversion" Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DE-SC0001293. The authors gratefully acknowledge R. Gerhart for assistance with photoelectrochemical cell fabrication and M. Meier and S. Yalamanchili for assistance with computer simulations. A.I.C. acknowledges a Graduate Research Fellowship from the National Science Foundation. Author Contributions: A.I.C. and K.R.H. contributed equally. The authors declare no competing financial interest.

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