title: Self-Optimizing Photoelectrochemical Growth of Nanopatterned Se-Te Films in Response to the Spectral Distribution of Incident Illumination.
abstract: Photoelectrochemical growth of Se-Te films spontaneously produces highly ordered, nanoscale lamellar morphologies with periodicities that can be tuned by varying the illumination wavelength during deposition. This phenomenon has been characterized further herein by determining the morphologies of photoelectrodeposited Se-Te films in response to tailored spectral illumination profiles. Se-Te films grown under illumination from four different sources, having similar average wavelengths but having spectral bandwidths that spanned several orders of magnitude, all nevertheless produced similar structures which had a single, common periodicity as quantitatively identified via Fourier analysis. Film deposition using simultaneous illumination from two narrowband sources, which differed in average wavelength by several hundred nanometers, resulted in a structure with only a single periodicity intermediate between the periods observed when either source alone was used. This single periodicity could be varied by manipulating the relative intensity of the two sources. An iterative model that combined full-wave electromagnetic effects with Monte Carlo growth simulations, and that considered only the fundamental light-material interactions during deposition, was in accord with the morphologies observed experimentally. Simulations of light absorption and concentration in idealized lamellar arrays, in conjunction with all of the available data, additionally indicated that a self-optimization of the periodicity of the nanoscale pattern, resulting in the maximization of the anisotropy of interfacial light absorption in the three-dimensional structure, is consistent with the observed growth process of such films.
authors.affiliation: Division of Chemistry and Chemical Engineering, ‡Division of Engineering and Applied Sciences, §The Joint Center for Artificial Photosynthesis, ∥Kavli Nanoscience Institute, and ⊥Beckman Institute, California Institute of Technology , Pasadena, California 91125, United States.
authors.forename: Azhar I
authors.initials: AI
authors.lastname: Carim
authors.affiliation: Division of Chemistry and Chemical Engineering, ‡Division of Engineering and Applied Sciences, §The Joint Center for Artificial Photosynthesis, ∥Kavli Nanoscience Institute, and ⊥Beckman Institute, California Institute of Technology , Pasadena, California 91125, United States.
authors.forename: Nicolas A
authors.initials: NA
authors.lastname: Batara
authors.affiliation: Division of Chemistry and Chemical Engineering, ‡Division of Engineering and Applied Sciences, §The Joint Center for Artificial Photosynthesis, ∥Kavli Nanoscience Institute, and ⊥Beckman Institute, California Institute of Technology , Pasadena, California 91125, United States.
authors.forename: Anjali
authors.initials: A
authors.lastname: Premkumar
authors.affiliation: Division of Chemistry and Chemical Engineering, ‡Division of Engineering and Applied Sciences, §The Joint Center for Artificial Photosynthesis, ∥Kavli Nanoscience Institute, and ⊥Beckman Institute, California Institute of Technology , Pasadena, California 91125, United States.
authors.forename: Harry A
authors.initials: HA
authors.lastname: Atwater
authors.affiliation: Division of Chemistry and Chemical Engineering, ‡Division of Engineering and Applied Sciences, §The Joint Center for Artificial Photosynthesis, ∥Kavli Nanoscience Institute, and ⊥Beckman Institute, California Institute of Technology , Pasadena, California 91125, United States.
authors.forename: Nathan S
authors.initials: NS
authors.lastname: Lewis
keywords: Electrodeposition; chalcogenide; maskless; photodeposition; photoelectrochemistry; template-free