The Vacancy-Induced Electronic Structure of the SrTiO3-δ Surface

Cook, Seyoung; Dylla, Maxwell T.; Rosenberg, Richard A.; Mansley, Zachary R.; Snyder, G. Jeffrey; Marks, Laurence D.; Fong, Dillon D.

doi:10.1002/aelm.201800460

Title: The Vacancy-Induced Electronic Structure of the SrTiO_3-δ Surface

Journal Article · Wed Nov 14 00:00:00 EST 2018 · Advanced Electronic Materials

DOI:https://doi.org/10.1002/aelm.201800460· OSTI ID:1499278

^[1]; Dylla, Maxwell T. ^[2]; Rosenberg, Richard A. ^[3]; Mansley, Zachary R. ^[2]; Snyder, G. Jeffrey ^[2]; Marks, Laurence D. ^[2];

^[3]

Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

The emergence of a 2D electron gas (2DEG) on the (001) surface of oxygen-deficient strontium titanate (SrTiO3-δ) is investigated. Using in situ soft X-ray spectroscopy and effective mass modeling, a series of quantitative band dia-grams are developed to describe the evolution of near-surface and bulk car-rier concentrations, downward band bending, and Fermi level along a lateral gradient of oxygen vacancies formed on SrTiO3-δ by direct-current resistive heating under ultrahigh vacuum conditions. Electrons are accumulated over a 3 nm region near the surface, confined within a potential well with saturated 300 meV downward band bending. The relation between Fermi levels and carrier concentrations near the surface suggests the density of states near the surface is much lower than the bulk density of states, which is consistent with the quantum-confined subbands of a 2DEG. The quantitative relation-ship between the surface and bulk electronic structures developed in this work provides a guide for precise engineering of the oxygen-vacancy-induced 2DEG in SrTiO3.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); Institute for Catalysis in Energy Processes (ICEP); USDOE

Grant/Contract Number:: AC02-06CH11357; DMR-1334713; DMR-1333335; FG02-03ER15457; FG02-01ER45945; DE‐AC02‐06CH11357; DE‐FG02‐03ER15457; DE‐FG02‐01ER45945

OSTI ID:: 1499278

Alternate ID(s):: OSTI ID: 1482131; OSTI ID: 1870982

Journal Information:: Advanced Electronic Materials, Vol. 5, Issue 1; ISSN 2199-160X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 14 works

Citation information provided by
Web of Science

References (51)

Tailoring the nature and strength of electron–phonon interactions in the SrTiO3(001) 2D electron liquid Wang, Z.; McKeown Walker, S.; Tamai, A. Nature Materials, Vol. 15, Issue 8 https://doi.org/10.1038/nmat4623	journal	April 2016
Photoemission study of the metallic state of lightly electron-doped SrTiO3 Aiura, Y.; Hase, I.; Bando, H. Surface Science, Vol. 515, Issue 1 https://doi.org/10.1016/S0039-6028(02)01784-3	journal	August 2002
Oxide Interfaces--An Opportunity for Electronics Mannhart, J.; Schlom, D. G. Science, Vol. 327, Issue 5973, p. 1607-1611 https://doi.org/10.1126/science.1181862	journal	March 2010
Epitaxial growth, structure, and intermixing at the ${LaAlO}_{3}$ / ${SrTiO}_{3}$ interface as the film stoichiometry is varied Qiao, L.; Droubay, T. C.; Varga, T. Physical Review B, Vol. 83, Issue 8 https://doi.org/10.1103/PhysRevB.83.085408	journal	February 2011
Two-dimensional electron liquid state at ${LaAlO}_{3} {-SrTiO}_{3}$ interfaces Breitschaft, M.; Tinkl, V.; Pavlenko, N. Physical Review B, Vol. 81, Issue 15 https://doi.org/10.1103/PhysRevB.81.153414	journal	April 2010
Electric field control of the LaAlO3/SrTiO3 interface ground state Caviglia, A. D.; Gariglio, S.; Reyren, N. Nature, Vol. 456, Issue 7222 https://doi.org/10.1038/nature07576	journal	December 2008
Spatial distribution of carriers in ${SrTiO}_{3}$ revealed by photoluminescence dynamics measurements Yasuda, Hideki; Yamada, Yasuhiro; Tayagaki, Takeshi Physical Review B, Vol. 78, Issue 23 https://doi.org/10.1103/PhysRevB.78.233202	journal	December 2008
Large modulation of the Shubnikov–de Haas oscillations by the Rashba interaction at the LaAlO ₃ /SrTiO ₃ interface Fête, A.; Gariglio, S.; Berthod, C. New Journal of Physics, Vol. 16, Issue 11 https://doi.org/10.1088/1367-2630/16/11/112002	journal	November 2014
Spatial density profile of electrons near the LaAlO ₃ /SrTiO ₃ heterointerface revealed by time-resolved photoluminescence spectroscopy Yamada, Yasuhiro; Sato, Hiroki K.; Hikita, Yasuyuki Applied Physics Letters, Vol. 104, Issue 15 https://doi.org/10.1063/1.4872171	journal	April 2014
Interface superconductor with gap behaviour like a high-temperature superconductor Richter, C.; Boschker, H.; Dietsche, W. Nature, Vol. 502, Issue 7472 https://doi.org/10.1038/nature12494	journal	October 2013
Temperature Dependence of Photoluminescence Spectra of Nondoped and Electron-Doped ${SrTiO}_{3}$ : Crossover from Auger Recombination to Single-Carrier Trapping Yamada, Yasuhiro; Yasuda, Hideki; Tayagaki, Takeshi Physical Review Letters, Vol. 102, Issue 24 https://doi.org/10.1103/PhysRevLett.102.247401	journal	June 2009
Effect of oxygen vacancies in the ${SrTiO}_{3}$ substrate on the electrical properties of the ${LaAlO}_{3} ∕ {SrTiO}_{3}$ interface Kalabukhov, Alexey; Gunnarsson, Robert; Börjesson, Johan Physical Review B, Vol. 75, Issue 12 https://doi.org/10.1103/PhysRevB.75.121404	journal	March 2007
Why Some Interfaces Cannot be Sharp Nakagawa, Naoyuki; Hwang, Harold Y.; Muller, David A. arXiv https://doi.org/10.48550/arxiv.cond-mat/0510491	text	January 2005
Quasiparticle dynamics and spin-orbital texture of the SrTiO3 two-dimensional electron gas King, P. D. C.; Walker, S. McKeown; Tamai, A. arXiv https://doi.org/10.48550/arxiv.1403.0520	text	January 2014
Two-dimensional electron gas with universal subbands at the surface of SrTiO₃ Santander-Syro, A. F.; Copie, O.; Kondo, T. Nature, Vol. 469, Issue 7329, p. 189-193 https://doi.org/10.1038/nature09720	journal	January 2011
Coexistence of magnetic order and two-dimensional superconductivity at LaAlO₃/SrTiO₃ interfaces Li, Lu; Richter, C.; Mannhart, J. Nature Physics, Vol. 7, Issue 10, p. 762-766 https://doi.org/10.1038/nphys2080	journal	September 2011
Blue-light emission at room temperature from Ar+-irradiated SrTiO3 Kan, Daisuke; Terashima, Takahito; Kanda, Ryoko Nature Materials, Vol. 4, Issue 11 https://doi.org/10.1038/nmat1498	journal	October 2005
High mobility conduction at (110) and (111) LaAlO3/SrTiO3 interfaces Herranz, G.; Sánchez, F.; Dix, N. Scientific Reports, Vol. 2, Issue 1 https://doi.org/10.1038/srep00758	journal	October 2012
Creation and control of a two-dimensional electron liquid at the bare SrTiO3 surface Meevasana, W.; King, P. D. C.; He, R. H. Nature Materials, Vol. 10, Issue 2 https://doi.org/10.1038/nmat2943	journal	January 2011
Mapping the spatial distribution of charge carriers in LaAlO3/SrTiO3 heterostructures Basletic, M.; Maurice, J. -L.; Carrétéro, C. Nature Materials, Vol. 7, Issue 8 https://doi.org/10.1038/nmat2223	journal	June 2008
High Mobility in ${LaAlO}_{3} / {SrTiO}_{3}$ Heterostructures: Origin, Dimensionality, and Perspectives Herranz, G.; Basletić, M.; Bibes, M. Physical Review Letters, Vol. 98, Issue 21, Article No. 216803 https://doi.org/10.1103/PhysRevLett.98.216803	journal	May 2007
$d_{x z / y z}$ orbital subband structures and chiral orbital angular momentum in the (001) surface states of ${SrTiO}_{3}$ Soltani, Shoresh; Cho, Soohyun; Ryu, Hanyoung Physical Review B, Vol. 95, Issue 12 https://doi.org/10.1103/PhysRevB.95.125103	journal	March 2017
Vacancies and small polarons in ${SrTiO}_{3}$ Janotti, Anderson; Varley, Joel B.; Choi, Minseok Physical Review B, Vol. 90, Issue 8 https://doi.org/10.1103/PhysRevB.90.085202	journal	August 2014
Carrier-Density Control of the SrTiO ₃ (001) Surface 2D Electron Gas studied by ARPES Walker, Siobhan McKeown; Bruno, Flavio Yair; Wang, Zhiming Advanced Materials, Vol. 27, Issue 26 https://doi.org/10.1002/adma.201501556	journal	May 2015
X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 Henke, B. L.; Gullikson, E. M.; Davis, J. C. Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342 https://doi.org/10.1006/adnd.1993.1013	journal	July 1993
Transport in ferromagnetic GdTiO3/SrTiO3 heterostructures Moetakef, Pouya; Zhang, Jack Y.; Kozhanov, Alexander Applied Physics Letters, Vol. 98, Issue 11 https://doi.org/10.1063/1.3568894	journal	March 2011
Blue luminescence from electron-doped SrTiO3 Kan, D.; Kanda, R.; Kanemitsu, Y. Applied Physics Letters, Vol. 88, Issue 19 https://doi.org/10.1063/1.2202750	journal	May 2006
A polarity-induced defect mechanism for conductivity and magnetism at polar-nonpolar oxide interfaces Yu, Liping; Zunger, Alex arXiv https://doi.org/10.48550/arxiv.1402.0895	text	January 2014
Emergent phenomena at oxide interfaces Hwang, H. Y.; Iwasa, Y.; Kawasaki, M. Nature Materials, Vol. 11, Issue 2 https://doi.org/10.1038/nmat3223	journal	January 2012
Non-Volatile Control of 2DEG Conductivity at Oxide Interfaces Kim, Shin-Ik; Kim, Dai-Hong; Kim, Yoonjung Advanced Materials, Vol. 25, Issue 33 https://doi.org/10.1002/adma.201301097	journal	June 2013
Nanoscale control of an interfacial metal–insulator transition at room temperature Cen, C.; Thiel, S.; Hammerl, G. Nature Materials, Vol. 7, Issue 4 https://doi.org/10.1038/nmat2136	journal	March 2008
In Situ Control of Separate Electronic Phases on SrTiO ₃ Surfaces by Oxygen Dosing Dudy, Lenart; Sing, Michael; Scheiderer, Philipp Advanced Materials, Vol. 28, Issue 34 https://doi.org/10.1002/adma.201600046	journal	June 2016
Probing depth of soft x-ray absorption spectroscopy measured in total-electron-yield mode Abbate, M.; Goedkoop, J. B.; de Groot, F. M. F. Surface and Interface Analysis, Vol. 18, Issue 1 https://doi.org/10.1002/sia.740180111	journal	January 1992
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface Ohtomo, A.; Hwang, H. Y. Nature, Vol. 427, Issue 6973 https://doi.org/10.1038/nature02308	journal	January 2004
Origin of Charge Density at ${LaAlO}_{3}$ on ${SrTiO}_{3}$ Heterointerfaces: Possibility of Intrinsic Doping Siemons, Wolter; Koster, Gertjan; Yamamoto, Hideki Physical Review Letters, Vol. 98, Issue 19, Article No. 196802 https://doi.org/10.1103/PhysRevLett.98.196802	journal	May 2007
Large modulation of the Shubnikov-de Haas oscillations by the Rashba interaction at the LaAlO$_{3}$/SrTiO$_{3}$ interface Fête, A.; Gariglio, S.; Berthod, C. arXiv https://doi.org/10.48550/arxiv.1407.4925	text	January 2014
Field-effect control of superconductivity and Rashba spin-orbit coupling in top-gated LaAlO3/SrTiO3 devices Hurand, S.; Jouan, A.; Feuillet-Palma, C. Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep12751	journal	August 2015
Mixed Dimensionality of Confined Conducting Electrons in the Surface Region of ${SrTiO}_{3}$ Plumb, N. C.; Salluzzo, M.; Razzoli, E. Physical Review Letters, Vol. 113, Issue 8 https://doi.org/10.1103/PhysRevLett.113.086801	journal	August 2014
Tunable Quasi-Two-Dimensional Electron Gases in Oxide Heterostructures Thiel, S. Science, Vol. 313, Issue 5795, p. 1942-1945 https://doi.org/10.1126/science.1131091	journal	September 2006
Why some interfaces cannot be sharp Nakagawa, Naoyuki; Hwang, Harold Y.; Muller, David A. Nature Materials, Vol. 5, Issue 3, p. 204-209 https://doi.org/10.1038/nmat1569	journal	January 2006
Effect of oxygen deficiency on SrTiO ₃ (001) surface reconstructions Shimizu, Ryota; Iwaya, Katsuya; Ohsawa, Takeo Applied Physics Letters, Vol. 100, Issue 26 https://doi.org/10.1063/1.4730409	journal	June 2012
Superconducting Interfaces Between Insulating Oxides Reyren, N.; Thiel, S.; Caviglia, A. D. Science, Vol. 317, Issue 5842 https://doi.org/10.1126/science.1146006	journal	August 2007
Metallic and Insulating Interfaces of Amorphous SrTiO ₃ -Based Oxide Heterostructures Chen, Yunzhong; Pryds, Nini; Kleibeuker, Josée E. Nano Letters, Vol. 11, Issue 9 https://doi.org/10.1021/nl201821j	journal	September 2011
Dynamics of nonlinear blue photoluminescence and Auger recombination in ${SrTiO}_{3}$ Yasuda, Hideki; Kanemitsu, Yoshihiko Physical Review B, Vol. 77, Issue 19 https://doi.org/10.1103/PhysRevB.77.193202	journal	May 2008
Time-Resolved Synchrotron Radiation Excited Optical Luminescence: Light-Emission Properties of Silicon-Based Nanostructures Sham, Tsun-Kong; Rosenberg, Richard A. ChemPhysChem, Vol. 8, Issue 18 https://doi.org/10.1002/cphc.200700226	journal	December 2007
A polarity-induced defect mechanism for conductivity and magnetism at polar–nonpolar oxide interfaces Yu, Liping; Zunger, Alex Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6118	journal	October 2014
Quasiparticle dynamics and spin–orbital texture of the SrTiO3 two-dimensional electron gas King, P. D. C.; McKeown Walker, S.; Tamai, A. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4414	journal	February 2014
Orientational Tuning of the Fermi Sea of Confined Electrons at the ${SrTiO}_{3}$ (110) and (111) Surfaces Rödel, T. C.; Bareille, C.; Fortuna, F. Physical Review Applied, Vol. 1, Issue 5 https://doi.org/10.1103/PhysRevApplied.1.051002	journal	June 2014
A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3 Chen, Y. Z.; Bovet, N.; Trier, F. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2394	journal	January 2013
Tunable Rashba Spin-Orbit Interaction at Oxide Interfaces Caviglia, A. D.; Gabay, M.; Gariglio, S. Physical Review Letters, Vol. 104, Issue 12, Article No. 126803 https://doi.org/10.1103/PhysRevLett.104.126803	journal	March 2010
Tuning Spin-Orbit Coupling and Superconductivity at the ${SrTiO}_{3} / {LaAlO}_{3}$ Interface: A Magnetotransport Study Ben Shalom, M.; Sachs, M.; Rakhmilevitch, D. Physical Review Letters, Vol. 104, Issue 12 https://doi.org/10.1103/PhysRevLett.104.126802	journal	March 2010

Cited By (2)

Emergent magnetic phase transitions in Fe-doped SrTiO _3−δ Pei, Yujuan; Zhang, Ruyi; Song, Yang AIP Advances, Vol. 9, Issue 12 https://doi.org/10.1063/1.5116671	journal	December 2019
Effect of Annealing Temperature for Ni/AlOx/Pt RRAM Devices Fabricated with Solution-Based Dielectric Shen, Zongjie; Qi, Yanfei; Mitrovic, Ivona Micromachines, Vol. 10, Issue 7 https://doi.org/10.3390/mi10070446	journal	July 2019

Similar Records

Switchable Induced Polarization in LaAlO3/SrTiO3 Heterostructures

Journal Article · Sun Jan 01 00:00:00 EST 2012 · Nano Letters · OSTI ID:1499278

Bark, C; Sharma, P.; Wang, Y.; +12 more

Structural and electronic properties of n-doped and p-dopedSrTiO3

Journal Article · Sun Aug 15 00:00:00 EDT 2004 · Physical Review B · OSTI ID:1499278

Luo, Weidong; Duan, Wenhui; Louie, Steven G; +1 more

The Itinerant 2D Electron Gas of the Indium Oxide (111) Surface: Implications for Carbon‐ and Energy‐Conversion Applications

Journal Article · Thu Sep 05 00:00:00 EDT 2019 · Small · OSTI ID:1499278

Jovic, Vedran; Moser, Simon; Papadogianni, Alexandra; +8 more

Related Subjects

36 MATERIALS SCIENCE
SrTiO3 surface
effective mass modeling
electronic structure
in-situ x-ray spectroscopy
oxygen vacancies

Title: The Vacancy-Induced Electronic Structure of the SrTiO3-δ Surface

Citation Formats

References (51)

Cited By (2)

Similar Records

Related Subjects

Title: The Vacancy-Induced Electronic Structure of the SrTiO_3-δ Surface