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Title: Conducting interface in oxide homojunction: Understanding of superior properties in black TiO2

Abstract

Black TiO2 nanoparticles with a crystalline core and amorphous-shell structure exhibit superior optoelectronic properties in comparison with pristine TiO2. The fundamental mechanisms underlying these enhancements, however, remain unclear, largely due to the inherent complexities and limitations of powder materials. Here, we fabricate TiO2 homojunction films consisting of an oxygen-deficient amorphous layer on top of a highly crystalline layer, to simulate the structural/functional configuration of black TiO2 nanoparticles. Metallic conduction is achieved at the crystalline–amorphous homointerface via electronic interface reconstruction, which we show to be the main reason for the enhanced electron transport of black TiO2. As a result, this work not only achieves an unprecedented understanding of black TiO2 but also provides a new perspective for investigating carrier generation and transport behavior at oxide interfaces, which are of tremendous fundamental and technological interest.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1331278
Report Number(s):
LA-UR-16-22153
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 9; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Material Science

Citation Formats

Lu, Xujie, Chen, Aiping, Luo, Yongkang, Lu, Ping, Dai, Yaomin, Enriquez, Erik M., Dowden, Paul Charles, Xu, Hongwu, Kotula, Paul G., Azad, Abul Kalam, Yarotski, Dmitry Anatolievitch, Prasankumar, Rohit Prativadi, Taylor, Antoinette Jane, Thompson, Joe David, and Jia, Quanxi. Conducting interface in oxide homojunction: Understanding of superior properties in black TiO2. United States: N. p., 2016. Web. doi:10.1021/acs.nanolett.6b02454.
Lu, Xujie, Chen, Aiping, Luo, Yongkang, Lu, Ping, Dai, Yaomin, Enriquez, Erik M., Dowden, Paul Charles, Xu, Hongwu, Kotula, Paul G., Azad, Abul Kalam, Yarotski, Dmitry Anatolievitch, Prasankumar, Rohit Prativadi, Taylor, Antoinette Jane, Thompson, Joe David, & Jia, Quanxi. Conducting interface in oxide homojunction: Understanding of superior properties in black TiO2. United States. https://doi.org/10.1021/acs.nanolett.6b02454
Lu, Xujie, Chen, Aiping, Luo, Yongkang, Lu, Ping, Dai, Yaomin, Enriquez, Erik M., Dowden, Paul Charles, Xu, Hongwu, Kotula, Paul G., Azad, Abul Kalam, Yarotski, Dmitry Anatolievitch, Prasankumar, Rohit Prativadi, Taylor, Antoinette Jane, Thompson, Joe David, and Jia, Quanxi. Wed . "Conducting interface in oxide homojunction: Understanding of superior properties in black TiO2". United States. https://doi.org/10.1021/acs.nanolett.6b02454. https://www.osti.gov/servlets/purl/1331278.
@article{osti_1331278,
title = {Conducting interface in oxide homojunction: Understanding of superior properties in black TiO2},
author = {Lu, Xujie and Chen, Aiping and Luo, Yongkang and Lu, Ping and Dai, Yaomin and Enriquez, Erik M. and Dowden, Paul Charles and Xu, Hongwu and Kotula, Paul G. and Azad, Abul Kalam and Yarotski, Dmitry Anatolievitch and Prasankumar, Rohit Prativadi and Taylor, Antoinette Jane and Thompson, Joe David and Jia, Quanxi},
abstractNote = {Black TiO2 nanoparticles with a crystalline core and amorphous-shell structure exhibit superior optoelectronic properties in comparison with pristine TiO2. The fundamental mechanisms underlying these enhancements, however, remain unclear, largely due to the inherent complexities and limitations of powder materials. Here, we fabricate TiO2 homojunction films consisting of an oxygen-deficient amorphous layer on top of a highly crystalline layer, to simulate the structural/functional configuration of black TiO2 nanoparticles. Metallic conduction is achieved at the crystalline–amorphous homointerface via electronic interface reconstruction, which we show to be the main reason for the enhanced electron transport of black TiO2. As a result, this work not only achieves an unprecedented understanding of black TiO2 but also provides a new perspective for investigating carrier generation and transport behavior at oxide interfaces, which are of tremendous fundamental and technological interest.},
doi = {10.1021/acs.nanolett.6b02454},
journal = {Nano Letters},
number = 9,
volume = 16,
place = {United States},
year = {Wed Sep 14 00:00:00 EDT 2016},
month = {Wed Sep 14 00:00:00 EDT 2016}
}

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Cited by: 80 works
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Figures / Tables:

Figure 1 Figure 1: (a) Illustration of black TiO2 nanoparticle and thin film with crystalline-amorphous bilayer structure. (b) XRD 2θ-ω scans of TiO2 films on LAO (001). (c) RHEED patterns taken during growth of the TiO2 crystalline layer. The roughness of crystalline-amorphous interface is determined to be 1~2 unit cells by X-raymore » reflectivity (Figure S1). (d) Cross-sectional HAADF-STEM image of the bilayer film. (e) Magnified STEM image at the interface.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.