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Polarization Control of Morphological Pattern Orientation During Light-Mediated Synthesis of Nanostructured Se-Te
Azhar I Carim1, Nicolas A Batara1, Anjali Premkumar1
1Division 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.
Abstract:
The template-free growth of well ordered, highly anisotropic lamellar structures has been demonstrated during the photoelectrodeposition of Se-Te films, wherein the orientation of the pattern can be directed by orienting the linear polarization of the incident light. This control mechanism was investigated further herein by examining the morphologies of films grown photoelectrochemically using light from two simultaneous sources that had mutually different linear polarizations. Photoelectrochemical growth with light from two nonorthogonally polarized same-wavelength sources generated lamellar morphologies in which the long axes of the lamellae were oriented parallel to the intensity-weighted average polarization orientation. Simulations of light scattering at the solution-film interface were consistent with this observation. Computer modeling of these growths using combined full-wave electromagnetic and Monte Carlo growth simulations successfully reproduced the experimental morphologies and quantitatively agreed with the pattern orientations observed experimentally by considering only the fundamental light-material interactions during growth. Deposition with light from two orthogonally polarized same-wavelength as well as different-wavelength sources produced structures that consisted of two intersecting sets of orthogonally oriented lamellae in which the relative heights of the two sets could be varied by adjusting the relative source intensities. Simulations of light absorption were performed in analogous, idealized intersecting lamellar structures and revealed that the lamellae preferentially absorbed light polarized with the electric field vector along their long axes. These data sets cumulatively indicate that anisotropic light scattering and light absorption generated by the light polarization produces the anisotropic morphology and that the resultant morphology is a function of all illumination inputs despite differing polarizations.
