Growth control of oxygen stoichiometry in homoepitaxial SrTiO3 films by pulsed laser epitaxy in high vacuum

Lee, Ho Nyung; Ambrose Seo, Sung S.; Choi, Woo Seok; Rouleau, Christopher M.

doi:10.1038/srep19941

Title: Growth control of oxygen stoichiometry in homoepitaxial SrTiO₃ films by pulsed laser epitaxy in high vacuum

Journal Article · Fri Jan 29 00:00:00 EST 2016 · Scientific Reports

DOI:https://doi.org/10.1038/srep19941· OSTI ID:1247940

Lee, Ho Nyung ^[1]; Ambrose Seo, Sung S. ^[2]; Choi, Woo Seok ^[3]; Rouleau, Christopher M. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Kentucky, Lexington, KY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Sungkyunkwan Univ., Suwon (Republic of Korea)

In many transition metal oxides, oxygen stoichiometry is one of the most critical parameters that plays a key role in determining the structural, physical, optical, and electrochemical properties of the material. However, controlling the growth to obtain high quality single crystal films having the right oxygen stoichiometry, especially in a high vacuum environment, has been viewed as a challenge. In this work, we show that, through proper control of the plume kinetic energy, stoichiometric crystalline films can be synthesized without generating oxygen defects even in high vacuum. We use a model homoepitaxial system of SrTiO₃ (STO) thin films on single crystal STO substrates. Physical property measurements indicate that oxygen vacancy generation in high vacuum is strongly influenced by the energetics of the laser plume, and it can be controlled by proper laser beam delivery. Thus, our finding not only provides essential insight into oxygen stoichiometry control in high vacuum for understanding the fundamental properties of STO-based thin films and heterostructures, but it expands the utility of pulsed laser epitaxy of other materials as well.₃

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; NRF-2014R1A2A2A01006478

OSTI ID:: 1247940

Journal Information:: Scientific Reports, Vol. 6; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 65 works

Citation information provided by
Web of Science

References (49)

Multiple conducting carriers generated in LaAlO3/SrTiO3 heterostructures Seo, S. S. A.; Marton, Z.; Choi, W. S. Applied Physics Letters, Vol. 95, Issue 8 https://doi.org/10.1063/1.3213390	journal	August 2009
Growth mode control of the free carrier density in SrTiO3−δ films Ohtomo, A.; Hwang, H. Y. Journal of Applied Physics, Vol. 102, Issue 8 https://doi.org/10.1063/1.2798385	journal	October 2007
Strain screening by mobile oxygen vacancies in SrTiO3 Kim, Yongsam; Disa, Ankit S.; Babakol, Timur E. Applied Physics Letters, Vol. 96, Issue 25 https://doi.org/10.1063/1.3455157	journal	June 2010
Epitaxial SrTiO₃ films with electron mobilities exceeding 30,000 cm² V^-1 s^-1 Son, Junwoo; Moetakef, Pouya; Jalan, Bharat Nature Materials, Vol. 9, Issue 6, p. 482-484 https://doi.org/10.1038/nmat2750	journal	April 2010
Resonant tunnelling in a quantum oxide superlattice Choi, Woo Seok; Lee, Sang A.; You, Jeong Ho Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8424	journal	June 2015
Initial growth stages of epitaxial BaTiO[sub 3] films on vicinal SrTiO[sub 3] (001) substrate surfaces Visinoiu, A.; Alexe, M.; Lee, H. N. Journal of Applied Physics, Vol. 91, Issue 12 https://doi.org/10.1063/1.1478800	journal	January 2002
Time-resolved study of SrTiO3 homoepitaxial pulsed-laser deposition using surface x-ray diffraction Eres, G.; Tischler, J. Z.; Yoon, M. Applied Physics Letters, Vol. 80, Issue 18 https://doi.org/10.1063/1.1477279	journal	May 2002
Growth control of stoichiometry in LaMnO3 epitaxial thin films by pulsed laser deposition Marton, Zsolt; A. Seo, Sung Seok; Egami, Takeshi Journal of Crystal Growth, Vol. 312, Issue 20 https://doi.org/10.1016/j.jcrysgro.2010.07.013	journal	October 2010
The value of seeing nothing Mannhart, Jochen; Schlom, Darrell G. Nature, Vol. 430, Issue 7000 https://doi.org/10.1038/430620a	journal	August 2004
Improved stoichiometry and misfit control in perovskite thin film formation at a critical fluence by pulsed laser deposition Ohnishi, T.; Lippmaa, M.; Yamamoto, T. Applied Physics Letters, Vol. 87, Issue 24 https://doi.org/10.1063/1.2146069	journal	December 2005
Thermal stability of epitaxial SrRuO3 films as a function of oxygen pressure Lee, Ho Nyung; Christen, Hans M.; Chisholm, Matthew F. Applied Physics Letters, Vol. 84, Issue 20 https://doi.org/10.1063/1.1753650	journal	May 2004
Defects and transport in complex oxide thin films Ohnishi, Tsuyoshi; Shibuya, Keisuke; Yamamoto, Takahisa Journal of Applied Physics, Vol. 103, Issue 10 https://doi.org/10.1063/1.2921972	journal	May 2008
Impact of the interplay between nonstoichiometry and kinetic energy of the plume species on the growth mode of SrTiO ₃ thin films Xu, C.; Wicklein, S.; Sambri, A. Journal of Physics D: Applied Physics, Vol. 47, Issue 3 https://doi.org/10.1088/0022-3727/47/3/034009	journal	December 2013
Strong polarization enhancement in asymmetric three-component ferroelectric superlattices Lee, Ho Nyung; Christen, Hans M.; Chisholm, Matthew F. Nature, Vol. 433, Issue 7024 https://doi.org/10.1038/nature03261	journal	January 2005
Atomic Control of the SrTiO₃ Crystal Surface Kawasaki, M.; Takahashi, K.; Maeda, T. Science, Vol. 266, Issue 5190, p. 1540-1542 https://doi.org/10.1126/science.266.5190.1540	journal	December 1994
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
Room-temperature ferroelectricity in strained SrTiO₃ Haeni, J. H.; Irvin, P.; Chang, W. Nature, Vol. 430, Issue 7001, p. 758-761 https://doi.org/10.1038/nature02773	journal	August 2004
Growth of homoepitaxial SrTiO3 thin films by molecular-beam epitaxy Brooks, C. M.; Kourkoutis, L. Fitting; Heeg, T. Applied Physics Letters, Vol. 94, Issue 16 https://doi.org/10.1063/1.3117365	journal	April 2009
Ion-deficient Phases in Titanium and Vanadium Compounds of the Perovskite Type ^1,2 Kestigian, Michael; Dickinson, John G.; Ward, Roland Journal of the American Chemical Society, Vol. 79, Issue 21 https://doi.org/10.1021/ja01578a003	journal	November 1957
Growth‐related stress and surface morphology in homoepitaxial SrTiO ₃ films Tarsa, E. J.; Hachfeld, E. A.; Quinlan, F. T. Applied Physics Letters, Vol. 68, Issue 4 https://doi.org/10.1063/1.116376	journal	January 1996
Epitaxial growth and electronic structure of LaTiOx films Ohtomo, A.; Muller, D. A.; Grazul, J. L. Applied Physics Letters, Vol. 80, Issue 21 https://doi.org/10.1063/1.1481767	journal	May 2002
Molecular beam epitaxy of SrTiO3 with a growth window Jalan, Bharat; Moetakef, Pouya; Stemmer, Susanne Applied Physics Letters, Vol. 95, Issue 3 https://doi.org/10.1063/1.3184767	journal	July 2009
Dynamics of laser-ablated particles in newly developed eclipse PLD Nakatsuka, Hiroshi; Ishibashi, Hiroshige; Kobayashi, Takeshi Laser interaction and related plasma phenomena: 12th international conference, AIP Conference Proceedings https://doi.org/10.1063/1.50419	conference	January 1996
Pulsed laser deposition-induced reduction of SrTiO3 crystals Scullin, Matthew L.; Ravichandran, Jayakanth; Yu, Choongho Acta Materialia, Vol. 58, Issue 2 https://doi.org/10.1016/j.actamat.2009.09.024	journal	January 2010
Origin of surface roughness for c ‐axis oriented Y‐Ba‐Cu‐O superconducting films Chang, C. C.; Wu, X. D.; Ramesh, R. Applied Physics Letters, Vol. 57, Issue 17 https://doi.org/10.1063/1.104143	journal	October 1990
Electric-field-induced superconductivity in an insulator Ueno, K.; Nakamura, S.; Shimotani, H. Nature Materials, Vol. 7, Issue 11, p. 855-858 https://doi.org/10.1038/nmat2298	journal	October 2008
The production of low scattering dielectric mirrors using rotating vane particle filtration Barr, W. P. Journal of Physics E: Scientific Instruments, Vol. 2, Issue 12 https://doi.org/10.1088/0022-3735/2/12/432	journal	December 1969
A new laser ablation geometry for the production of smooth thin single-layer YBa2Cu3O7−x and multilayer YBa2Cu3O7−x/PrBa2Cu3O7−x films Kennedy, Robin J. Thin Solid Films, Vol. 214, Issue 2 https://doi.org/10.1016/0040-6090(92)90774-6	journal	July 1992
Dynamics of laser ablation plume penetration through low pressure background gases Geohegan, David B.; Puretzky, Alexander A. Applied Physics Letters, Vol. 67, Issue 2 https://doi.org/10.1063/1.114665	journal	July 1995
Atomic Layer Engineering of Perovskite Oxides for Chemically Sharp Heterointerfaces Choi, Woo Seok; Rouleau, Christopher M.; Seo, Sung Seok A. Advanced Materials, Vol. 24, Issue 48 https://doi.org/10.1002/adma.201202691	journal	October 2012
Artificial charge-modulationin atomic-scale perovskite titanate superlattices Ohtomo, A.; Muller, D. A.; Grazul, J. L. Nature, Vol. 419, Issue 6905 https://doi.org/10.1038/nature00977	journal	September 2002
Strain Tuning of Ferroelectric Thin Films Schlom, Darrell G.; Chen, Long-Qing; Eom, Chang-Beom Annual Review of Materials Research, Vol. 37, Issue 1 https://doi.org/10.1146/annurev.matsci.37.061206.113016	journal	August 2007
Superconducting Transition Temperatures of Semiconducting SrTi $O_{3}$ Koonce, C. S.; Cohen, Marvin L.; Schooley, J. F. Physical Review, Vol. 163, Issue 2 https://doi.org/10.1103/PhysRev.163.380	journal	November 1967
Ferroelectricity in Strain-Free ${SrTiO}_{3}$ Thin Films Jang, H. W.; Kumar, A.; Denev, S. Physical Review Letters, Vol. 104, Issue 19, Article No. 197601 https://doi.org/10.1103/PhysRevLett.104.197601	journal	May 2010
Nonlinear Hall effect and multichannel conduction in ${LaTiO}_{3} / {SrTiO}_{3}$ superlattices Kim, J. S.; Seo, S. S. A.; Chisholm, M. F. Physical Review B, Vol. 82, Issue 20 https://doi.org/10.1103/PhysRevB.82.201407	journal	November 2010
Suppressed Dependence of Polarization on Epitaxial Strain in Highly Polar Ferroelectrics Lee, Ho Nyung; Nakhmanson, Serge M.; Chisholm, Matthew F. Physical Review Letters, Vol. 98, Issue 21 https://doi.org/10.1103/PhysRevLett.98.217602	journal	May 2007
Reflection high-energy electron diffraction and atomic force microscopy studies on homoepitaxial growth of SrTiO3(001) Naito, Michio; Yamamoto, Hideki; Sato, Hisashi Physica C: Superconductivity, Vol. 305, Issue 3-4 https://doi.org/10.1016/S0921-4534(98)00338-4	journal	September 1998
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
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
Optical absorption and transport in semiconducting SrTi $O_{3}$ Lee, C.; Destry, J.; Brebner, J. L. Physical Review B, Vol. 11, Issue 6 https://doi.org/10.1103/PhysRevB.11.2299	journal	March 1975
Free-Carrier Absorption in Reduced SrTi $O_{3}$ Baer, W. S. Physical Review, Vol. 144, Issue 2 https://doi.org/10.1103/PhysRev.144.734	journal	April 1966
Elastic effects of vacancies in strontium titanate: Short- and long-range strain fields, elastic dipole tensors, and chemical strain Freedman, Daniel A.; Roundy, D.; Arias, T. A. Physical Review B, Vol. 80, Issue 6 https://doi.org/10.1103/PhysRevB.80.064108	journal	August 2009
Oxygen-deficient SrTiO3−x, x = 0.28, 0.17, and 0.08. Crystal growth, crystal structure, magnetic, and transport properties Gong, Wenhe; Yun, H.; Ning, Y. B. Journal of Solid State Chemistry, Vol. 90, Issue 2 https://doi.org/10.1016/0022-4596(91)90149-C	journal	February 1991
Strain and oxygen vacancy ordering in ${SrTiO}_{3}$ : Diffuse x-ray scattering studies Kim, Yongsam; Disa, Ankit S.; Babakol, Timur E. Physical Review B, Vol. 92, Issue 6 https://doi.org/10.1103/PhysRevB.92.064105	journal	August 2015
Strong polarization enhancement in asymmetric three-component ferroelectric superlattices Lee, Ho Nyung; Christen, Hans M.; Chisholm, Matthew F. Nature, Vol. 434, Issue 7034 https://doi.org/10.1038/nature03517	journal	April 2005
Suppressed dependence of polarization on epitaxial strain in highly polar ferroelectrics Lee, Ho Nyung; Nakhmanson, Serge M.; Chisholm, Matthew F. arXiv https://doi.org/10.48550/arxiv.0704.2401	text	January 2007
Atomic layer engineering of perovskite oxides for chemically sharp heterointerfaces Choi, Woo Seok; Rouleau, Christopher M.; Seo, Sung Seok A. arXiv https://doi.org/10.48550/arxiv.1210.2007	text	January 2012
Growth mode control of the free carrier density in SrTiO3-d films Ohtomo, Akira; Hwang, Harold Y. arXiv https://doi.org/10.48550/arxiv.cond-mat/0604117	text	January 2006
Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3 Muller, David A.; Nakagawa, Naoyuki; Ohtomo, Akira Nature, Vol. 430, Issue 7000 https://doi.org/10.1038/nature02756	journal	August 2004

Cited By (23)

Nonequilibrium Synthesis of Highly Porous Single-Crystalline Oxide Nanostructures Lee, Dongkyu; Gao, Xiang; Fan, Lisha Advanced Materials Interfaces, Vol. 4, Issue 3 https://doi.org/10.1002/admi.201601034	journal	January 2017
Enhanced flexoelectricity at reduced dimensions revealed by mechanically tunable quantum tunnelling Das, Saikat; Wang, Bo; Paudel, Tula R. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08462-0	journal	February 2019
UV radiation enhanced oxygen vacancy formation caused by the PLD plasma plume Hensling, F. V. E.; Keeble, D. J.; Zhu, J. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-27207-5	journal	June 2018
Pulsed-laser epitaxy of topological insulator Bi ₂ Te ₃ thin films Liao, Zhaoliang; Brahlek, Matthew; Ok, Jong Mok APL Materials, Vol. 7, Issue 4 https://doi.org/10.1063/1.5088190	journal	April 2019
Unraveling the enhanced Oxygen Vacancy Formation in Complex Oxides during Annealing and Growth Hensling, Felix V. E.; Xu, Chencheng; Gunkel, Felix RWTH Aachen University https://doi.org/10.18154/rwth-2017-01950	text	January 2017
Enhanced magnetism in lightly doped manganite heterostructures: strain or stoichiometry? Mbatang, Richard; Xue, Deqing; Enriquez, Erik Nanoscale, Vol. 11, Issue 15 https://doi.org/10.1039/c8nr09693g	journal	January 2019
Metal Oxide Nanocomposites: A Perspective from Strain, Defect, and Interface Chen, Aiping; Su, Qing; Han, Hyungkyu Advanced Materials, Vol. 31, Issue 4 https://doi.org/10.1002/adma.201803241	journal	October 2018
Metallicity in SrTiO ₃ substrates induced by pulsed laser deposition Balakrishnan, Purnima P.; Veit, Michael J.; Alaan, Urusa S. APL Materials, Vol. 7, Issue 1 https://doi.org/10.1063/1.5080939	journal	January 2019
Strain coupling of oxygen non-stoichiometry in perovskite thin films Herklotz, Andreas; Lee, Dongkyu; Guo, Er-Jia Journal of Physics: Condensed Matter, Vol. 29, Issue 49 https://doi.org/10.1088/1361-648x/aa949b	journal	December 2017
Oxygen diffusion in oxide thin films grown on $SrTi O_{3}$ Schneider, Christof W.; Döbeli, Max; Richter, Christoph Physical Review Materials, Vol. 3, Issue 12 https://doi.org/10.1103/physrevmaterials.3.123401	journal	December 2019
Graphene/BiVO4/TiO2 nanocomposite: tuning band gap energies for superior photocatalytic activity under visible light Nanakkal, A. R.; Alexander, L. K. Journal of Materials Science, Vol. 52, Issue 13 https://doi.org/10.1007/s10853-017-1002-0	journal	March 2017
Strain-enhanced topotactic hydrogen substitution for oxygen in SrTiO ₃ epitaxial thin film Kutsuzawa, Dai; Hirose, Yasushi; Chikamatsu, Akira Applied Physics Letters, Vol. 113, Issue 25 https://doi.org/10.1063/1.5057370	journal	December 2018
Surface Characterizations and Selective Etching of Sr‐Rich Segregation on Top of SrVO ₃ Thin‐Films Grown by Pulsed Laser Deposition Bourlier, Yoan; Frégnaux, Mathieu; Bérini, Bruno ChemNanoMat, Vol. 5, Issue 5 https://doi.org/10.1002/cnma.201900017	journal	March 2019
Probing vacancy behavior across complex oxide heterointerfaces Zhu, Jiaxin; Lee, Jung-Woo; Lee, Hyungwoo RWTH Aachen University https://doi.org/10.18154/rwth-2020-04157	text	January 2019
Tuning of the Optical Properties of the Transparent Conducting Oxide SrVO ₃ by Electronic Correlations Boileau, Alexis; Cheikh, Aïmane; Fouchet, Arnaud Advanced Optical Materials, Vol. 7, Issue 7 https://doi.org/10.1002/adom.201801516	journal	January 2019
Stimulating Oxide Heterostructures: A Review on Controlling SrTiO ₃ ‐Based Heterointerfaces with External Stimuli Christensen, Dennis Valbjørn; Trier, Felix; Niu, Wei Advanced Materials Interfaces, Vol. 6, Issue 21 https://doi.org/10.1002/admi.201900772	journal	August 2019
Multistaged discharge constructing heterostructure with enhanced solid-solution behavior for long-life lithium-oxygen batteries Xu, Shu-Mao; Liang, Xiao; Wu, Xue-Yan Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13712-2	journal	December 2019
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
UV radiation enhanced oxygen vacancy formation caused by the PLD plasma plume Hensling, F. V. E.; Keeble, D. J.; Zhu, J. RWTH Aachen University https://doi.org/10.18154/rwth-2018-226838	text	January 2018
Probing vacancy behavior across complex oxide heterointerfaces Zhu, Jiaxin; Lee, Jung-Woo; Lee, Hyungwoo Science Advances, Vol. 5, Issue 2 https://doi.org/10.1126/sciadv.aau8467	journal	February 2019
Unraveling the enhanced Oxygen Vacancy Formation in Complex Oxides during Annealing and Growth Hensling, Felix V. E.; Xu, Chencheng; Gunkel, Felix Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/srep39953	journal	January 2017
Investigations of metastable Ca2IrO4 epitaxial thin-films: systematic comparison with Sr2IrO4 and Ba2IrO4 Souri, M.; Gruenewald, J. H.; Terzic, J. arXiv https://doi.org/10.48550/arxiv.1605.06146	text	January 2016
Tuning electromagnetic properties of SrRuO3 epitaxial thin films via atomic control of cation vacancies Lee, Sang A.; Oh, Seokjae; Lee, Jegon arXiv https://doi.org/10.48550/arxiv.1709.07600	text	January 2017

Similar Records

Defects, stoichiometry, and electronic transport in SrTiO{sub 3-δ} epilayers: A high pressure oxygen sputter deposition study

Journal Article · Sun Aug 07 00:00:00 EDT 2016 · Journal of Applied Physics · OSTI ID:1247940

Ambwani, P.; Xu, P.; Jeong, J. S.; +4 more

δ-Doping of oxygen vacancies dictated by thermodynamics in epitaxial SrTiO₃ films

Journal Article · Thu Jun 01 00:00:00 EDT 2017 · AIP Advances · OSTI ID:1247940

Li, Fengmiao; Yang, Fang; Liang, Yan; +9 more

Growth of homoepitaxial SrTiO{sub 3} thin films by molecular-beam epitaxy

Journal Article · Mon Apr 20 00:00:00 EDT 2009 · Applied Physics Letters · OSTI ID:1247940

Brooks, C M; Kourkoutis, L Fitting; Muller, D A; +3 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
surfaces
interfaces and thin films
synthesis and processing
SrTiO₃

Title: Growth control of oxygen stoichiometry in homoepitaxial SrTiO3 films by pulsed laser epitaxy in high vacuum

Citation Formats

References (49)

Cited By (23)

Similar Records

Related Subjects

Title: Growth control of oxygen stoichiometry in homoepitaxial SrTiO₃ films by pulsed laser epitaxy in high vacuum