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Title: High-fraction brookite films from amorphous precursors

Structure-specific synthesis processes are of key importance to the growth of polymorphic functional compounds such as TiO 2, where material properties strongly depend on structure as well as chemistry. The robust growth of the brookite polymorph of TiO 2, a promising photocatalyst, has been difficult in both powder and thin-film forms due to the disparity of reported synthesis techniques, their highly specific nature, and lack of mechanistic understanding. In this work, we report the growth of high-fraction (~95%) brookite thin films prepared by annealing amorphous titania precursor films deposited by pulsed laser deposition. We characterize the crystallization process, eliminating the previously suggested roles of substrate templating and Na helper ions in driving brookite formation. Instead, we link phase selection directly to film thickness, offering a novel, generalizable route to brookite growth that does not rely on the presence of extraneous elements or particular lattice-matched substrates. In addition to providing a new synthesis route to brookite thin films, our results take a step towards resolving the problem of phase selection in TiO 2 growth, contributing to the further development of this promising functional material.
Authors:
 [1] ;  [2] ; ORCiD logo [3] ;  [4] ;  [5] ;  [6] ; ORCiD logo [7] ;  [5] ; ORCiD logo [8] ;  [6] ;  [5] ;  [9] ;  [1]
  1. Oregon State Univ., Corvallis, OR (United States). Dept. of Physics
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Applied Energy Programs
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  4. Colorado School of Mines, Golden, CO (United States). Dept. of Metallurgical and Materials Engineering
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Applied Energy Programs; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  9. Colorado School of Mines, Golden, CO (United States). Dept. of Metallurgical and Materials Engineering
Publication Date:
Report Number(s):
NREL/JA-5K00-70535
Journal ID: ISSN 2045-2322
Grant/Contract Number:
AC36-08GO28308; AC02-76SF00515; ACI-1548562; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; brookite; thin films; precursors; Materials for energy and catalysis; Surfaces, interfaces and thin films
OSTI Identifier:
1409492
Alternate Identifier(s):
OSTI ID: 1410515; OSTI ID: 1418211; OSTI ID: 1419455

Haggerty, James E. S., Schelhas, Laura T., Kitchaev, Daniil A., Mangum, John S., Garten, Lauren M., Sun, Wenhao, Stone, Kevin H., Perkins, John D., Toney, Michael F., Ceder, Gerbrand, Ginley, David S., Gorman, Brian P., and Tate, Janet. High-fraction brookite films from amorphous precursors. United States: N. p., Web. doi:10.1038/s41598-017-15364-y.
Haggerty, James E. S., Schelhas, Laura T., Kitchaev, Daniil A., Mangum, John S., Garten, Lauren M., Sun, Wenhao, Stone, Kevin H., Perkins, John D., Toney, Michael F., Ceder, Gerbrand, Ginley, David S., Gorman, Brian P., & Tate, Janet. High-fraction brookite films from amorphous precursors. United States. doi:10.1038/s41598-017-15364-y.
Haggerty, James E. S., Schelhas, Laura T., Kitchaev, Daniil A., Mangum, John S., Garten, Lauren M., Sun, Wenhao, Stone, Kevin H., Perkins, John D., Toney, Michael F., Ceder, Gerbrand, Ginley, David S., Gorman, Brian P., and Tate, Janet. 2017. "High-fraction brookite films from amorphous precursors". United States. doi:10.1038/s41598-017-15364-y. https://www.osti.gov/servlets/purl/1409492.
@article{osti_1409492,
title = {High-fraction brookite films from amorphous precursors},
author = {Haggerty, James E. S. and Schelhas, Laura T. and Kitchaev, Daniil A. and Mangum, John S. and Garten, Lauren M. and Sun, Wenhao and Stone, Kevin H. and Perkins, John D. and Toney, Michael F. and Ceder, Gerbrand and Ginley, David S. and Gorman, Brian P. and Tate, Janet},
abstractNote = {Structure-specific synthesis processes are of key importance to the growth of polymorphic functional compounds such as TiO2, where material properties strongly depend on structure as well as chemistry. The robust growth of the brookite polymorph of TiO2, a promising photocatalyst, has been difficult in both powder and thin-film forms due to the disparity of reported synthesis techniques, their highly specific nature, and lack of mechanistic understanding. In this work, we report the growth of high-fraction (~95%) brookite thin films prepared by annealing amorphous titania precursor films deposited by pulsed laser deposition. We characterize the crystallization process, eliminating the previously suggested roles of substrate templating and Na helper ions in driving brookite formation. Instead, we link phase selection directly to film thickness, offering a novel, generalizable route to brookite growth that does not rely on the presence of extraneous elements or particular lattice-matched substrates. In addition to providing a new synthesis route to brookite thin films, our results take a step towards resolving the problem of phase selection in TiO2 growth, contributing to the further development of this promising functional material.},
doi = {10.1038/s41598-017-15364-y},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {2017},
month = {11}
}