The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications
Abstract
Abstract Transparent conducting oxides (TCO) have integral and emerging roles in photovoltaic, thermoelectric energy conversion, and more recently, photocatalytic systems. The functional properties of TCOs, and thus their role in these applications, are often mediated by the bulk electronic band structure but are also strongly influenced by the electronic structure of the native surface 2D electron gas (2DEG), particularly under operating conditions. This study investigates the 2DEG, and its response to changes in chemistry, at the (111) surface of the model TCO In 2 O 3 , through angle resolved and core level X‐ray photoemission spectroscopy. It is found that the itinerant charge carriers of the 2DEG reside in two quantum well subbands penetrating up to 65 Å below the surface. The charge carrier concentration of this 2DEG, and thus the high surface n‐type conductivity, emerges from donor‐type oxygen vacancies of surface character and proves to be remarkably robust against surface absorbents and contamination. The optical transparency, however, may rely on the presence of ubiquitous surface adsorbed oxygen groups and hydrogen defect states that passivate localized oxygen vacancy states in the bandgap of In 2 O 3 .
- Authors:
-
[6];
- National Isotope Center GNS Science MacDiarmid Institute for Advanced Materials and Nanotechnology Lower Hutt Wellington 5010 New Zealand, School of Chemical Sciences The University of Auckland Auckland 1010 New Zealand
- Physikalisches Institut Universität Würzburg Würzburg D‐97074 Germany, Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
- Paul‐Drude‐Institut für Festkörperelektronik Leibniz‐Institut im Forschungsverbund Berlin e.V. Hausvogteiplatz 5‐7 Berlin 10117 Germany
- Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
- Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Department of Physics University of California Davis CA 95616 USA
- National Isotope Center GNS Science MacDiarmid Institute for Advanced Materials and Nanotechnology Lower Hutt Wellington 5010 New Zealand
- Department of Physics Boston University Boston MA 02215 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1560691
- Grant/Contract Number:
- DEFG02‐98ER45680
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Small
- Additional Journal Information:
- Journal Name: Small Journal Volume: 16 Journal Issue: 12; Journal ID: ISSN 1613-6810
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Jovic, Vedran, Moser, Simon, Papadogianni, Alexandra, Koch, Roland J., Rossi, Antonio, Jozwiak, Chris, Bostwick, Aaron, Rotenberg, Eli, Kennedy, John V., Bierwagen, Oliver, and Smith, Kevin E. The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications. Germany: N. p., 2019.
Web. doi:10.1002/smll.201903321.
Jovic, Vedran, Moser, Simon, Papadogianni, Alexandra, Koch, Roland J., Rossi, Antonio, Jozwiak, Chris, Bostwick, Aaron, Rotenberg, Eli, Kennedy, John V., Bierwagen, Oliver, & Smith, Kevin E. The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications. Germany. https://doi.org/10.1002/smll.201903321
Jovic, Vedran, Moser, Simon, Papadogianni, Alexandra, Koch, Roland J., Rossi, Antonio, Jozwiak, Chris, Bostwick, Aaron, Rotenberg, Eli, Kennedy, John V., Bierwagen, Oliver, and Smith, Kevin E. Thu .
"The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications". Germany. https://doi.org/10.1002/smll.201903321.
@article{osti_1560691,
title = {The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications},
author = {Jovic, Vedran and Moser, Simon and Papadogianni, Alexandra and Koch, Roland J. and Rossi, Antonio and Jozwiak, Chris and Bostwick, Aaron and Rotenberg, Eli and Kennedy, John V. and Bierwagen, Oliver and Smith, Kevin E.},
abstractNote = {Abstract Transparent conducting oxides (TCO) have integral and emerging roles in photovoltaic, thermoelectric energy conversion, and more recently, photocatalytic systems. The functional properties of TCOs, and thus their role in these applications, are often mediated by the bulk electronic band structure but are also strongly influenced by the electronic structure of the native surface 2D electron gas (2DEG), particularly under operating conditions. This study investigates the 2DEG, and its response to changes in chemistry, at the (111) surface of the model TCO In 2 O 3 , through angle resolved and core level X‐ray photoemission spectroscopy. It is found that the itinerant charge carriers of the 2DEG reside in two quantum well subbands penetrating up to 65 Å below the surface. The charge carrier concentration of this 2DEG, and thus the high surface n‐type conductivity, emerges from donor‐type oxygen vacancies of surface character and proves to be remarkably robust against surface absorbents and contamination. The optical transparency, however, may rely on the presence of ubiquitous surface adsorbed oxygen groups and hydrogen defect states that passivate localized oxygen vacancy states in the bandgap of In 2 O 3 .},
doi = {10.1002/smll.201903321},
journal = {Small},
number = 12,
volume = 16,
place = {Germany},
year = {Thu Sep 05 00:00:00 EDT 2019},
month = {Thu Sep 05 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/smll.201903321
https://doi.org/10.1002/smll.201903321
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 14 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Surface Origin of High Conductivities in Undoped Thin Films
journal, January 2012
- Lany, S.; Zakutayev, A.; Mason, T. O.
- Physical Review Letters, Vol. 108, Issue 1
Quantized Electron Accumulation States in Indium Nitride Studied by Angle-Resolved Photoemission Spectroscopy
journal, December 2006
- Colakerol, Leyla; Veal, T. D.; Jeong, Hae-Kyung
- Physical Review Letters, Vol. 97, Issue 23
Surface Electron Accumulation and the Charge Neutrality Level in
journal, September 2008
- King, P. D. C.; Veal, T. D.; Payne, D. J.
- Physical Review Letters, Vol. 101, Issue 11
The role of surface electron accumulation and bulk doping for gas-sensing explored with single-crystalline In2O3 thin films
journal, November 2016
- Rombach, Julius; Papadogianni, Alexandra; Mischo, Markus
- Sensors and Actuators B: Chemical, Vol. 236
Photocatalytic Hydrogenation of Carbon Dioxide with High Selectivity to Methanol at Atmospheric Pressure
journal, July 2018
- Wang, Lu; Ghoussoub, Mireille; Wang, Hong
- Joule, Vol. 2, Issue 7
Creation and control of a two-dimensional electron liquid at the bare SrTiO3 surface
journal, January 2011
- Meevasana, W.; King, P. D. C.; He, R. H.
- Nature Materials, Vol. 10, Issue 2
Highly Conductive Coaxial SnO 2 −In 2 O 3 Heterostructured Nanowires for Li Ion Battery Electrodes
journal, October 2007
- Kim, Dong-Wan; Hwang, In-Sung; Kwon, S. Joon
- Nano Letters, Vol. 7, Issue 10
Many-electron effects on the dielectric function of cubic : Effective electron mass, band nonparabolicity, band gap renormalization, and Burstein-Moss shift
journal, January 2016
- Feneberg, Martin; Nixdorf, Jakob; Lidig, Christian
- Physical Review B, Vol. 93, Issue 4
Indium oxide—a transparent, wide-band gap semiconductor for (opto)electronic applications
journal, January 2015
- Bierwagen, Oliver
- Semiconductor Science and Technology, Vol. 30, Issue 2
How Indium Nitride Senses Water
journal, November 2017
- Jovic, Vedran; Moser, Simon; Ulstrup, Søren
- Nano Letters, Vol. 17, Issue 12
On the nature and temperature dependence of the fundamental band gap of In 2 O 3 : Nature and temperature dependence of the fundamental band gap of In
journal, September 2013
- Irmscher, K.; Naumann, M.; Pietsch, M.
- physica status solidi (a), Vol. 211, Issue 1
Photoexcited Surface Frustrated Lewis Pairs for Heterogeneous Photocatalytic CO 2 Reduction
journal, January 2016
- Ghuman, Kulbir Kaur; Hoch, Laura B.; Szymanski, Paul
- Journal of the American Chemical Society, Vol. 138, Issue 4
Subband Structure of a Two-Dimensional Electron Gas Formed at the Polar Surface of the Strong Spin-Orbit Perovskite
journal, March 2012
- King, P. D. C.; He, R. H.; Eknapakul, T.
- Physical Review Letters, Vol. 108, Issue 11
Tin indium oxide/graphene nanosheet nanocomposite as an anode material for lithium ion batteries with enhanced lithium storage capacity and rate capability
journal, February 2013
- Yang, Hongxun; Song, Taeseup; Lee, Sangkyu
- Electrochimica Acta, Vol. 91
Vacancy defects in indium oxide: An ab-initio study
journal, May 2011
- Reunchan, Pakpoom; Zhou, Xin; Limpijumnong, Sukit
- Current Applied Physics, Vol. 11, Issue 3
Evaporated Sn‐doped In 2 O 3 films: Basic optical properties and applications to energy‐efficient windows
journal, December 1986
- Hamberg, I.; Granqvist, C. G.
- Journal of Applied Physics, Vol. 60, Issue 11
Nature of the Band Gap of Revealed by First-Principles Calculations and X-Ray Spectroscopy
journal, April 2008
- Walsh, Aron; Da Silva, Juarez L. F.; Wei, Su-Huai
- Physical Review Letters, Vol. 100, Issue 16
Tunable Polaronic Conduction in Anatase
journal, May 2013
- Moser, S.; Moreschini, L.; Jaćimović, J.
- Physical Review Letters, Vol. 110, Issue 19
Evidence for -Type Doping of InN
journal, March 2006
- Jones, R. E.; Yu, K. M.; Li, S. X.
- Physical Review Letters, Vol. 96, Issue 12
Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO 2 reduction
journal, November 2016
- Hoch, Laura B.; Szymanski, Paul; Ghuman, Kulbir Kaur
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 50
How to extract the surface potential profile from the ARPES signature of a 2DEG
journal, May 2018
- Moser, S.; Jovic, V.; Koch, R.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 225
Towards Understanding the Cross-Sensitivity of In 2 O 3 Based Ozone Sensors: Effects of O 3 , O 2 and H 2 O Adsorption at In 2 O 3 (111) Surfaces
journal, December 2017
- Berthold, Theresa; Katzer, Simeon; Rombach, Julius
- physica status solidi (b), Vol. 255, Issue 4
Microscopic Origin of Electron Accumulation in
journal, January 2013
- Zhang, K. H. L.; Egdell, R. G.; Offi, F.
- Physical Review Letters, Vol. 110, Issue 5
Surface oxygen vacancy origin of electron accumulation in indium oxide
journal, June 2011
- Walsh, Aron
- Applied Physics Letters, Vol. 98, Issue 26
Band gap, electronic structure, and surface electron accumulation of cubic and rhombohedral
journal, May 2009
- King, P. D. C.; Veal, T. D.; Fuchs, F.
- Physical Review B, Vol. 79, Issue 20
Consequences of plasma oxidation and vacuum annealing on the chemical properties and electron accumulation of In 2 O 3 surfaces
journal, December 2016
- Berthold, Theresa; Rombach, Julius; Stauden, Thomas
- Journal of Applied Physics, Vol. 120, Issue 24
Indium-oxide polymorphs from first principles: Quasiparticle electronic states
journal, April 2008
- Fuchs, F.; Bechstedt, F.
- Physical Review B, Vol. 77, Issue 15
In2O3 and MoO3–In2O3 thin film semiconductor sensors: interaction with NO2 and O3
journal, April 1998
- Gurlo, A.; Bârsan, N.; Ivanovskaya, M.
- Sensors and Actuators B: Chemical, Vol. 47, Issue 1-3
Electronic structure of and Sn-doped by hard x-ray photoemission spectroscopy
journal, April 2010
- Körber, C.; Krishnakumar, V.; Klein, A.
- Physical Review B, Vol. 81, Issue 16
Experimental electronic structure of In 2 O 3 and Ga 2 O 3
journal, August 2011
- Janowitz, Christoph; Scherer, Valentina; Mohamed, Mansour
- New Journal of Physics, Vol. 13, Issue 8
Mixed Dimensionality of Confined Conducting Electrons in the Surface Region of
journal, August 2014
- Plumb, N. C.; Salluzzo, M.; Razzoli, E.
- Physical Review Letters, Vol. 113, Issue 8
Atomically Precise Lateral Modulation of a Two-Dimensional Electron Liquid in Anatase TiO 2 Thin Films
journal, March 2017
- Wang, Z.; Zhong, Z.; McKeown Walker, S.
- Nano Letters, Vol. 17, Issue 4
Dopability, Intrinsic Conductivity, and Nonstoichiometry of Transparent Conducting Oxides
journal, January 2007
- Lany, Stephan; Zunger, Alex
- Physical Review Letters, Vol. 98, Issue 4
Hydrogen doping in indium oxide: An ab initio study
journal, November 2009
- Limpijumnong, Sukit; Reunchan, Pakpoom; Janotti, Anderson
- Physical Review B, Vol. 80, Issue 19
Using hydrogen-doped In 2 O 3 films as a transparent back contact in (Ag,Cu)(In,Ga)Se 2 solar cells
journal, January 2018
- Keller, Jan; Shariati Nilsson, Nina; Aijaz, Asim
- Progress in Photovoltaics: Research and Applications, Vol. 26, Issue 3
Spatial Separation of Charge Carriers in In 2 O 3– x (OH) y Nanocrystal Superstructures for Enhanced Gas-Phase Photocatalytic Activity
journal, May 2016
- He, Le; Wood, Thomas E.; Wu, Bo
- ACS Nano, Vol. 10, Issue 5
Observation of quantized subband states and evidence for surface electron accumulation in CdO from angle-resolved photoemission spectroscopy
journal, October 2008
- Piper, L. F. J.; Colakerol, Leyla; King, P. D. C.
- Physical Review B, Vol. 78, Issue 16
Band structure of indium antimonide
journal, January 1957
- Kane, Evan O.
- Journal of Physics and Chemistry of Solids, Vol. 1, Issue 4