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Title: Resolving the Structure of a Well-Ordered Hydroxyl Overlayer on In 2O 3 (111): Nanomanipulation and Theory

Abstract

Changes in chemical and physical properties resulting from water adsorption play an important role in the characterization and performance of device-relevant materials. Studies of model oxides with well-characterized surfaces can provide detailed information that is vital for a general understanding of water–oxide interactions. In this work, we study single crystals of indium oxide, the prototypical transparent contact material that is heavily used in a wide range of applications and most prominently in optoelectronic technologies. Water adsorbs dissociatively already at temperatures as low as 100 K, as confirmed by scanning tunneling microscopy (STM), photoelectron spectroscopy, and density functional theory. This dissociation takes place on lattice sites of the defect-free surface. While the In 2O 3(111)-(1 × 1) surface offers four types of surface oxygen atoms (12 atoms per unit cell in total), water dissociation happens exclusively at one of them together with a neighboring pair of 5-fold coordinated In atoms. These O–In groups are symmetrically arranged around the 6-fold coordinated In atoms at the surface. At room temperature, the In 2O 3(111) surface thus saturates at three dissociated water molecules per unit cell, leading to a well-ordered hydroxylated surface with (1 × 1) symmetry, where the three water OWH groups plusmore » the surface OSH groups are imaged together as one bright triangle in STM. Manipulations with the STM tip by means of voltage pulses preferentially remove the H atom of one surface OSH group per triangle. The change in contrast due to strong local band bending provides insights into the internal structure of these bright triangles. The experimental results are further confirmed by quantitative simulations of the STM image corrugation.« less

Authors:
ORCiD logo [1];  [1];  [2];  [2];  [1];  [1]; ORCiD logo [1];  [3];  [3]; ORCiD logo [4];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Technische Univ. Wien, Vienna (Austria). Inst. of Applied Physics
  2. Friedrich-Alexander Univ., Erlangen-Nurnberg (Germany). Interdisciplinary Center for Molecular Materials and Computer-Chemistry-Center
  3. Lund Univ. (Sweden)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1408068
Alternate Identifier(s):
OSTI ID: 1421789; OSTI ID: 1426584
Grant/Contract Number:
AC05-00OR22725
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; density functional theory; hydroxylation; indium oxide; scanning tunneling microscopy; water dissociation

Citation Formats

Wagner, Margareta, Lackner, Peter, Seiler, Steffen, Brunsch, Achim, Bliem, Roland, Gerhold, Stefan, Wang, Zhiming, Osiecki, Jacek, Schulte, Karina, Boatner, Lynn A., Schmid, Michael, Meyer, Bernd, and Diebold, Ulrike. Resolving the Structure of a Well-Ordered Hydroxyl Overlayer on In 2O3 (111): Nanomanipulation and Theory. United States: N. p., 2017. Web. doi:10.1021/acsnano.7b06387.
Wagner, Margareta, Lackner, Peter, Seiler, Steffen, Brunsch, Achim, Bliem, Roland, Gerhold, Stefan, Wang, Zhiming, Osiecki, Jacek, Schulte, Karina, Boatner, Lynn A., Schmid, Michael, Meyer, Bernd, & Diebold, Ulrike. Resolving the Structure of a Well-Ordered Hydroxyl Overlayer on In 2O3 (111): Nanomanipulation and Theory. United States. doi:10.1021/acsnano.7b06387.
Wagner, Margareta, Lackner, Peter, Seiler, Steffen, Brunsch, Achim, Bliem, Roland, Gerhold, Stefan, Wang, Zhiming, Osiecki, Jacek, Schulte, Karina, Boatner, Lynn A., Schmid, Michael, Meyer, Bernd, and Diebold, Ulrike. Wed . "Resolving the Structure of a Well-Ordered Hydroxyl Overlayer on In 2O3 (111): Nanomanipulation and Theory". United States. doi:10.1021/acsnano.7b06387.
@article{osti_1408068,
title = {Resolving the Structure of a Well-Ordered Hydroxyl Overlayer on In 2O3 (111): Nanomanipulation and Theory},
author = {Wagner, Margareta and Lackner, Peter and Seiler, Steffen and Brunsch, Achim and Bliem, Roland and Gerhold, Stefan and Wang, Zhiming and Osiecki, Jacek and Schulte, Karina and Boatner, Lynn A. and Schmid, Michael and Meyer, Bernd and Diebold, Ulrike},
abstractNote = {Changes in chemical and physical properties resulting from water adsorption play an important role in the characterization and performance of device-relevant materials. Studies of model oxides with well-characterized surfaces can provide detailed information that is vital for a general understanding of water–oxide interactions. In this work, we study single crystals of indium oxide, the prototypical transparent contact material that is heavily used in a wide range of applications and most prominently in optoelectronic technologies. Water adsorbs dissociatively already at temperatures as low as 100 K, as confirmed by scanning tunneling microscopy (STM), photoelectron spectroscopy, and density functional theory. This dissociation takes place on lattice sites of the defect-free surface. While the In2O3(111)-(1 × 1) surface offers four types of surface oxygen atoms (12 atoms per unit cell in total), water dissociation happens exclusively at one of them together with a neighboring pair of 5-fold coordinated In atoms. These O–In groups are symmetrically arranged around the 6-fold coordinated In atoms at the surface. At room temperature, the In2O3(111) surface thus saturates at three dissociated water molecules per unit cell, leading to a well-ordered hydroxylated surface with (1 × 1) symmetry, where the three water OWH groups plus the surface OSH groups are imaged together as one bright triangle in STM. Manipulations with the STM tip by means of voltage pulses preferentially remove the H atom of one surface OSH group per triangle. The change in contrast due to strong local band bending provides insights into the internal structure of these bright triangles. The experimental results are further confirmed by quantitative simulations of the STM image corrugation.},
doi = {10.1021/acsnano.7b06387},
journal = {ACS Nano},
number = 11,
volume = 11,
place = {United States},
year = {Wed Nov 01 00:00:00 EDT 2017},
month = {Wed Nov 01 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acsnano.7b06387

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