Syntheses of Colloidal F:In2O3 Cubes: Fluorine-Induced Faceting and Infrared Plasmonic Response

Cho, Shin Hum; Ghosh, Sandeep; Berkson, Zachariah J.; Hachtel, Jordan A.; Shi, Jianjian; Zhao, Xunhua; Reimnitz, Lauren C.; Dahlman, Clayton J.; Ho, Yujing; Yang, Anni; Liu, Yuanyue; Idrobo, Juan-Carlos; Chmelka, Bradley F.; Milliron, Delia J.

doi:10.1021/acs.chemmater.9b00906

Title: Syntheses of Colloidal F:In₂O₃ Cubes: Fluorine-Induced Faceting and Infrared Plasmonic Response

Journal Article · Thu Mar 21 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b00906· OSTI ID:1558540

^[1];

^[2];

^[3]; Shi, Jianjian ^[1]; Zhao, Xunhua ^[1]; Reimnitz, Lauren C. ^[1];

^[4]; Ho, Yujing ^[1]; Yang, Anni ^[1];

^[1]; Idrobo, Juan-Carlos ^[3];

^[2];

^[1]

Univ. of Texas, Austin, TX (United States)
Univ. of California, Santa Barbara, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Materials Department, University of California, Santa Barbara, Engineering II Building 1355, Santa Barbara, California 93106-5050, United States

Cube-shaped nanocrystals (NCs) of conventional metals like gold and silver generally exhibit localized surface plasmon resonance (LSPR) in the visible region with spectral modes determined by their faceted shapes. Yet, faceted NCs exhibiting LSPR response in the infrared (IR) region are relatively rare. Here, we describe the colloidal synthesis of nanoscale fluorine-doped indium oxide (F:In₂O₃) cubes with LSPR response in the IR region, wherein fluorine was discovered to both direct the cubic morphology and act as an aliovalent dopant. Single-crystalline 160 nm F:In₂O₃ cubes terminated by (100) facets and concave cubes were synthesized using a colloidal heat-up method. The presence of fluorine was found to impart higher stabilization to the (100) facets through density functional theory calculations that evaluated the energetics of F-substitution at surface oxygen sites. These calculations suggest that the cubic morphology results from surface binding of F atoms. In addition, fluorine acts as an anionic aliovalent dopant in the cubic bixbyite lattice of In₂O₃, introducing a high concentration of free electrons leading to LSPR. We confirmed the presence of lattice fluorine dopants in these cubes using solid-state ¹⁹F and ¹¹⁵In nuclear magnetic resonance spectroscopy. The cubes exhibit narrow, shape-dependent multimodal LSPR extinction peaks due to corner- and edge-centered modes. The spatial origin of these different contributions to the spectral response is directly visualized by electron energy loss spectroscopy in a scanning transmission electron microscope.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1558540

Journal Information:: Chemistry of Materials, Vol. 31, Issue 7; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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Fluoride-Assisted Synthesis of Plasmonic Colloidal Ta-Doped TiO ₂ Nanocrystals for Near-Infrared and Visible-Light Selective Electrochromic Modulation Cao, Sheng; Zhang, Shengliang; Zhang, Tianran Chemistry of Materials, Vol. 30, Issue 14 https://doi.org/10.1021/acs.chemmater.8b02196	journal	June 2018

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Emerging Electron Microscopy Techniques for Probing Functional Interfaces in Energy Materials Zachman, Michael J.; Hachtel, Jordan A.; Idrobo, Juan Carlos Angewandte Chemie International Edition, Vol. 59, Issue 4 https://doi.org/10.1002/anie.201902993	journal	January 2020

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