Hamann, Kathryn R. and Meier, Madeline C. and Lewis, Nathan S. and Carim, Azhar I. (2022) Plastic Morphological Response to Spectral Shifts during Inorganic Phototropic Growth. JACS Au, 2 (4). pp. 865-874. ISSN 2691-3704. PMCID PMC9088297. doi:10.1021/jacsau.1c00588. https://resolver.caltech.edu/CaltechAUTHORS:20220406-400053753
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Abstract
Plants exhibit phototropism in which growth is directed toward sunlight and demonstrate morphological plasticity in response to changes in the spectral distribution of the incident illumination. Inorganic phototropic growth via template-free, light-directed electrochemical deposition of semiconductor material can spontaneously generate highly ordered mesostructures with anisotropic, nanoscale lamellar features that exhibit a pitch proportional to the wavelength (λ) of the stimulating illumination. In this work, Se–Te films were generated via a two-step inorganic phototropic growth process using a series of narrowband light-emitting diode sources with discrete output wavelengths (λ₀ ≠ λ₁). Analogous to the plasticity observed in plants, changes in illumination wavelength from λ₀ to λ₁ resulted in morphological changes including feature branching, termination, and/or fusion along the growth direction. The interfacial feature pitch changed with the growth duration, in some cases in a notably nonmonotonic fashion, and eventually matched that obtained for growth using only λ₁. Simulated morphologies generated by modeling light–material interactions at the growth interface closely matched the evolved structures observed experimentally, indicating that the characteristics of the optical stimulation produce the observed plastic response during inorganic phototropic growth. Examination of the interfacial electric field modulation for λ1 illumination of simplified structures, representative of those generated experimentally, revealed the interfacial light scattering and concentration behavior that directed phototropic growth away from equilibrium, as well as the emergent nature of the phenomena that reestablish equilibrium.
| Item Type: | Article | ||||||||||
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| Additional Information: | © 2022 The Authors. Published by American Chemical Society. Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0). Received 31 December 2021. Accepted 4 March 2022. Revised 3 March 2022. Published online 4 April 2022. This work was supported by the National Science Foundation, Directorate for Mathematical & Physical Sciences, Division of Materials Research under Award No. DMR-1905963. The authors gratefully acknowledge J.R. Thompson for insightful discussions, E.D. Simonoff and S. Yalamanchili for assistance with substrate preparation, and R. Gerhart, N. Hart, and B. Markowicz for assistance with photoelectrochemical cell fabrication. KRH and MCM acknowledge Graduate Research Fellowships from the National Science Foundation. MCM also acknowledges the Resnick Institute at Caltech for fellowship support. The authors declare no competing financial interest. | ||||||||||
| Group: | Resnick Sustainability Institute | ||||||||||
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| Subject Keywords: | photoelectrodeposition photoelectrochemistry; mesostructure; template-free; maskless; optical | ||||||||||
| Issue or Number: | 4 | ||||||||||
| PubMed Central ID: | PMC9088297 | ||||||||||
| DOI: | 10.1021/jacsau.1c00588 | ||||||||||
| Record Number: | CaltechAUTHORS:20220406-400053753 | ||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20220406-400053753 | ||||||||||
| Official Citation: | Hamann, K. R., Meier, M. C., Lewis, N. S., & Carim, A. I. (2022). Plastic Morphological Response to Spectral Shifts during Inorganic Phototropic Growth. JACS Au, 2(4), 865–874. https://doi.org/10.1021/jacsau.1c00588 | ||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||
| ID Code: | 114177 | ||||||||||
| Collection: | CaltechAUTHORS | ||||||||||
| Deposited By: | George Porter | ||||||||||
| Deposited On: | 06 Apr 2022 13:36 | ||||||||||
| Last Modified: | 13 May 2022 16:04 |
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- Plastic Morphological Response to Spectral Shifts during Inorganic Phototropic Growth. (deposited 06 Apr 2022 13:36) [Currently Displayed]
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- Hamann, Kathryn R. and Meier, Madeline C. and Lewis, Nathan S. and Carim, Azhar I. Plastic Morphological Response to Spectral Shifts during Inorganic Phototropic Growth. (deposited 06 Apr 2022 13:36) [Currently Displayed]
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