skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Kinetically controlled fabrication of single-crystalline TiO 2 nanobrush architectures with high energy {001} facets

Abstract

Here, this study demonstrates that precise control of nonequilibrium growth conditions during pulsed laser deposition (PLD) can be exploited to produce single-crystalline anatase TiO 2 nanobrush architectures with large surface areas terminated with high energy {001} facets. The data indicate that the key to nanobrush formation is controlling the atomic surface transport processes to balance defect aggregation and surface-smoothing processes. High-resolution scanning transmission electron microscopy data reveal that defect-mediated aggregation is the key to TiO 2 nanobrush formation. The large concentration of defects present at the intersection of domain boundaries promotes aggregation of PLD growth species, resulting in the growth of the single-crystalline nanobrush architecture. This study proposes a model for the relationship between defect creation and growth mode in nonequilibrium environments, which enables application of this growth method to novel nanostructure design in a broad range of materials.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1349945
Alternate Identifier(s):
OSTI ID: 1349946; OSTI ID: 1351772
Grant/Contract Number:
AC05-00OR22725
Resource Type:
Journal Article: Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 8; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; nanobrush; anatase; defect-mediated aggregation; single crystalline; pulsed laser deposition

Citation Formats

Fan, Lisha, Gao, Xiang, Lee, Dongkyu, Guo, Er -Jia, Lee, Shinbuhm, Snijders, Paul C., Ward, Thomas Zac, Eres, Gyula, Chisholm, Matthew F., and Lee, Ho Nyung. Kinetically controlled fabrication of single-crystalline TiO2 nanobrush architectures with high energy {001} facets. United States: N. p., 2017. Web. doi:10.1002/advs.201700045.
Fan, Lisha, Gao, Xiang, Lee, Dongkyu, Guo, Er -Jia, Lee, Shinbuhm, Snijders, Paul C., Ward, Thomas Zac, Eres, Gyula, Chisholm, Matthew F., & Lee, Ho Nyung. Kinetically controlled fabrication of single-crystalline TiO2 nanobrush architectures with high energy {001} facets. United States. doi:10.1002/advs.201700045.
Fan, Lisha, Gao, Xiang, Lee, Dongkyu, Guo, Er -Jia, Lee, Shinbuhm, Snijders, Paul C., Ward, Thomas Zac, Eres, Gyula, Chisholm, Matthew F., and Lee, Ho Nyung. Wed . "Kinetically controlled fabrication of single-crystalline TiO2 nanobrush architectures with high energy {001} facets". United States. doi:10.1002/advs.201700045.
@article{osti_1349945,
title = {Kinetically controlled fabrication of single-crystalline TiO2 nanobrush architectures with high energy {001} facets},
author = {Fan, Lisha and Gao, Xiang and Lee, Dongkyu and Guo, Er -Jia and Lee, Shinbuhm and Snijders, Paul C. and Ward, Thomas Zac and Eres, Gyula and Chisholm, Matthew F. and Lee, Ho Nyung},
abstractNote = {Here, this study demonstrates that precise control of nonequilibrium growth conditions during pulsed laser deposition (PLD) can be exploited to produce single-crystalline anatase TiO2 nanobrush architectures with large surface areas terminated with high energy {001} facets. The data indicate that the key to nanobrush formation is controlling the atomic surface transport processes to balance defect aggregation and surface-smoothing processes. High-resolution scanning transmission electron microscopy data reveal that defect-mediated aggregation is the key to TiO2 nanobrush formation. The large concentration of defects present at the intersection of domain boundaries promotes aggregation of PLD growth species, resulting in the growth of the single-crystalline nanobrush architecture. This study proposes a model for the relationship between defect creation and growth mode in nonequilibrium environments, which enables application of this growth method to novel nanostructure design in a broad range of materials.},
doi = {10.1002/advs.201700045},
journal = {Advanced Science},
number = 8,
volume = 4,
place = {United States},
year = {Wed Mar 01 00:00:00 EST 2017},
month = {Wed Mar 01 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/advs.201700045

Save / Share:
  • Here, this study demonstrates that precise control of nonequilibrium growth conditions during pulsed laser deposition (PLD) can be exploited to produce single-crystalline anatase TiO 2 nanobrush architectures with large surface areas terminated with high energy {001} facets. The data indicate that the key to nanobrush formation is controlling the atomic surface transport processes to balance defect aggregation and surface-smoothing processes. High-resolution scanning transmission electron microscopy data reveal that defect-mediated aggregation is the key to TiO 2 nanobrush formation. The large concentration of defects present at the intersection of domain boundaries promotes aggregation of PLD growth species, resulting in the growthmore » of the single-crystalline nanobrush architecture. This study proposes a model for the relationship between defect creation and growth mode in nonequilibrium environments, which enables application of this growth method to novel nanostructure design in a broad range of materials.« less
  • Single-crystalline TiO{sub 2} nanomaterials were synthesized by hydrothermally treating suspensions of H-titanate nanotubes and characterized by XRD, TEM, and HRTEM. The effects of the pH values of the suspensions and the hydrothermal temperatures on the phase composition and morphology of the obtained TiO{sub 2} nanomaterials were systematically investigated. The H-titanate nanotubes were predominately transformed into anatase nanoparticle with rhombic shape when the pH value was greater than or equal to 1.0, whereas primarily turned into rutile nanorod with two pyramidal ends at the pH value less than or equal to 0.5. We propose a possible mechanism for hydrothermal transformation ofmore » H-titanate nanotubes into single-crystalline TiO{sub 2} nanomaterials. While the H-titanate nanotubes transform into tiny anatase nanocrystallites of ca. 3 nm in size, the formed nanocrystallites as an intermediate grow into the TiO{sub 2} nanomaterials with controlled phase composition and morphology. This growth process involves the steps of protonation, oriented attachment, and Ostwald ripening.« less
  • In this work, we developed an innovative approach to self-grow single crystalline CH 3NH 3PbI 3 directly on polycrystalline FTO/TiO 2 substrate, with which n-i-p type of perovskite solar cells were fabricated. The single crystalline nature of CH 3NH 3PbI 3 has been confirmed by X-ray diffraction and high resolution transmission electron microscopy, and it is observed that they possess smaller optic band gap and longer carrier life time. Highly efficient charge extractions occur at the interface between electron collecting TiO 2 and photo-harvesting CH 3NH 3PbI 3, resulting in a maximum short-circuit current density of 24.40 mA/cm 2. Themore » champion cell possesses a photovoltaic conversion efficiency of 8.78%, and there are still substantial room for further improvement, making it promising for the perovskite solar cell applications.« less
  • In this paper, we report on a nonaqueous synthesis of single crystalline anatase TiO{sub 2} nanorods by reaction between TiCl{sub 4} and benzyl alcohol at a low temperature of 80 deg. C. The resulting samples were characterized with X-ray diffraction, scanning electron microscopy, transmission electron microscopy, high resolution transmission electron microscopy, nitrogen adsorption, X-ray photoelectron spectrometry and UV-vis diffuse reflectance spectroscopy. We proposed that the TiO{sub 2} nanorods were formed through an oriented attachment mechanism. More importantly, these single crystalline anatase TiO{sub 2} nanorods exhibited significantly higher photocatalytic activities than commercial photocatalyst P25. This study provides an environmentally friendly andmore » economic approach to produce highly active TiO{sub 2} photocatalyst.« less