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Path-Dependent Morphological Evolution of Se–Te Mesostructures Prepared by Inorganic Phototropic Growth

Hamann, Kathryn R. and Carim, Azhar I. and Meier, Madeline C. and Lewis, Nathan S. (2020) Path-Dependent Morphological Evolution of Se–Te Mesostructures Prepared by Inorganic Phototropic Growth. Journal of the American Chemical Society, 142 (47). pp. 19840-19843. ISSN 0002-7863. doi:10.1021/jacs.0c09798.

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We describe herein a path-dependent “history” effect wherein the film morphology generated in the second step of a two-step inorganic phototropic growth process depends on a preexisting structure that has been first grown under different optical stimulation conditions. Se–Te generated with static illumination exhibited a highly anisotropic lamellar morphology with a characteristic feature pitch proportional to the input wavelength. Growth using first a short wavelength of light, followed by growth using a longer wavelength, resulted in the second-stage morphology exhibiting termination of lamellae formed during the first growth step. The lamellar pitch at the end of the second growth step was larger than that effected in the first step. In contrast, use of the same input wavelengths but in the opposite order produced no change in the feature pitch but rather only linear feature extension. Analysis of light absorption in simulated structures, in tandem with the empirical data, indicated that the history effect and asymmetric path dependence are a result of emergent nanophotonic processes at the growth interface that dynamically shape the optical field and direct morphological evolution of the photodeposit in a continuous feedback loop.

Item Type:Article
Related URLs:
URLURL TypeDescription
Hamann, Kathryn R.0000-0003-1163-7173
Carim, Azhar I.0000-0003-3630-6872
Meier, Madeline C.0000-0003-1608-0810
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2020 American Chemical Society. Received: September 13, 2020; Published: November 11, 2020. 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 Number DE-SC0001293 and was also supported by the National Science Foundation, Directorate for Mathematical & Physical Sciences, Division of Materials Research, under Award Number DMR 1905963. The authors gratefully acknowledge J. Thompson for insightful discussions, E. Simonoff and S. Yalamanchili for assistance with substrate preparation, and R. Gerhart, N. Hart, and B. Markowicz for assistance with photoelectrochemical cell fabrication. K.R.H. and M.C.M. acknowledge Graduate Research Fellowships from the National Science Foundation. M.C.M. also acknowledges the Resnick Sustainability Institute at Caltech for fellowship support. The authors declare no competing financial interest.
Group:Resnick Sustainability Institute
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0001293
NSF Graduate Research FellowshipUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
Subject Keywords:Morphology, Crystallization, Absorption, Deposition, Quantum mechanics
Issue or Number:47
Record Number:CaltechAUTHORS:20201112-103612027
Persistent URL:
Official Citation:Path-Dependent Morphological Evolution of Se–Te Mesostructures Prepared by Inorganic Phototropic Growth. Kathryn R. Hamann, Azhar I. Carim, Madeline C. Meier, and Nathan S. Lewis. Journal of the American Chemical Society 2020 142 (47), 19840-19843; DOI: 10.1021/jacs.0c09798
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106643
Deposited By: George Porter
Deposited On:16 Nov 2020 15:57
Last Modified:16 Nov 2021 18:55

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