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Precursor selection in hybrid molecular beam epitaxy of alkaline-earth stannates

Journal Article · · Journal of Vacuum Science and Technology A
DOI:https://doi.org/10.1116/6.0000590· OSTI ID:1853511
One of the challenges of oxide molecular beam epitaxy (MBE) is the synthesis of oxides containing metals with high electronegativity (metals that are hard to oxidize). The use of reactive organometallic precursors can potentially address this issue. To investigate the formation of radicals in MBE, we explored three carefully chosen metal-organic precursors of tin for SnO2 and BaSnO3 growth: tetramethyltin (TMT), tetraethyltin (TET), and hexamethylditin (HMDT). All three precursors produced single-crystalline, atomically smooth, and epitaxial SnO2 (101) films on r-Al2O3 (101¯2) in the presence of oxygen plasma. The study of growth kinetics revealed reaction-limited and flux-limited regimes except for TET, which also exhibited a decrease in the deposition rate with increasing temperature above ~800 °C. Contrary to these similarities, the performance of these precursors was dramatically different for BaSnO3 growth. TMT and TET were ineffective in supplying adequate tin, whereas HMDT yielded phase-pure, stoichiometric BaSnO3 films. Significantly, HMDT resulted in phase-pure and stoichiometric BaSnO3 films even without the use of an oxygen plasma (i.e., with molecular oxygen alone). Furthermore, these results are discussed using the ability of HMDT to form tin radicals and therefore assisting with Sn → Sn4+ oxidation reaction. Structural and electronic transport properties of films grown using HMDT with and without oxygen plasma are compared. This study provides guideline for the choice of precursors that will enable the synthesis of metal oxides containing hard-to-oxidize metals using reactive radicals in MBE.
Research Organization:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC)
Grant/Contract Number:
SC0020211
OSTI ID:
1853511
Alternate ID(s):
OSTI ID: 1698052
Journal Information:
Journal of Vacuum Science and Technology A, Journal Name: Journal of Vacuum Science and Technology A Journal Issue: 6 Vol. 38; ISSN 0734-2101
Publisher:
American Vacuum Society / AIPCopyright Statement
Country of Publication:
United States
Language:
English

References (32)

Frontiers in the Growth of Complex Oxide Thin Films: Past, Present, and Future of Hybrid MBE journal December 2017
Highly Conductive SrVO 3 as a Bottom Electrode for Functional Perovskite Oxides journal May 2013
Wide Bandgap Perovskite Oxides with High Room‐Temperature Electron Mobility journal June 2019
Enthalpies of vaporization of tetramethyltin, tetraethyltin, tetra-n-propyltin, and tetraethyl-lead, and a survey of the Group IV tetramethyl and tetraethyl compounds journal June 1980
Preparation of yttrium barium copper oxide superconducting films by metalorganic molecular beam epitaxy journal December 1991
Synthesis of conducting oxides by ML-ALE journal December 1994
Epitaxial growth and properties of thin film oxides journal August 2000
Plasma-assisted molecular beam epitaxy of SnO2 on TiO2 journal August 2008
Computational Thermochemistry of Mono- and Dinuclear Tin Alkyls Used in Vapor Deposition Processes journal February 2019
Separating Electrons and Donors in BaSnO 3 via Band Engineering journal November 2019
Dissociation Dynamics and Thermochemistry of Tin Species, (CH3)4Sn and (CH3)6Sn2, by Threshold Photoelectron−Photoion Coincidence Spectroscopy journal December 2010
Wide bandgap BaSnO3 films with room temperature conductivity exceeding 104 S cm−1 journal May 2017
Adsorption-controlled growth and the influence of stoichiometry on electronic transport in hybrid molecular beam epitaxy-grown BaSnO 3 films journal January 2017
In situ deposition of superconducting YBa 2 Cu 3 O 7− x and DyBa 2 Cu 3 O 7− x thin films by organometallic molecular‐beam epitaxy journal December 1991
Investigation of (110) SnO2 growth mechanisms on TiO2 substrates by plasma-assisted molecular beam epitaxy journal July 2009
Molecular beam epitaxy of SrTiO3 with a growth window journal July 2009
Critical thickness and strain relaxation in molecular beam epitaxy-grown SrTiO 3 films journal November 2013
Perspective: Oxide molecular-beam epitaxy rocks! journal June 2015
High-mobility BaSnO 3 grown by oxide molecular beam epitaxy journal January 2016
Adsorption-controlled growth of La-doped BaSnO 3 by molecular-beam epitaxy journal November 2017
GenX : an extensible X-ray reflectivity refinement program utilizing differential evolution journal November 2007
Plasma-assisted molecular beam epitaxy and characterization of SnO2 (101) on r-plane sapphire journal September 2008
Growth modes in metal-organic molecular beam epitaxy of TiO2 on r-plane sapphire
  • Jalan, Bharat; Engel-Herbert, Roman; Cagnon, Joël
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 27, Issue 2 https://doi.org/10.1116/1.3065713
journal March 2009
Analysis of carbon in SrTiO3 grown by hybrid molecular beam epitaxy
  • Jalan, Bharat; Cagnon, Joël; Mates, Thomas E.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 27, Issue 6 https://doi.org/10.1116/1.3253355
journal November 2009
Atomic layer deposition of tin oxide and zinc tin oxide using tetraethyltin and ozone
  • Warner, Ellis J.; Johnson, Forrest; Campbell, Stephen A.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 33, Issue 2 https://doi.org/10.1116/1.4907562
journal February 2015
Molecular beam epitaxy growth of SnO2 using a tin chemical precursor
  • Wang, Tianqi; Prakash, Abhinav; Warner, Ellis
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 33, Issue 2 https://doi.org/10.1116/1.4913294
journal February 2015
Hybrid molecular beam epitaxy for the growth of stoichiometric BaSnO 3
  • Prakash, Abhinav; Dewey, John; Yun, Hwanhui
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 33, Issue 6 https://doi.org/10.1116/1.4933401
journal November 2015
Cheap and stable titanium source for use in oxide molecular beam epitaxy systems journal July 1996
THE REACTIVITY OF METAL–METAL BONDS: I. THE Sn–Sn BOND journal April 1966
High-Temperature Superconducting Multilayers and Heterostructures Grown by Atomic Layer-By-Layer Molecular Beam Epitaxy journal August 1995
Reactive Pathways in the Chemical Vapor Deposition of Tin Oxide Films by Tetramethyltin Oxidation journal December 1989
Electron transport in semiconducting SnO2: Intentional bulk donors and acceptors, the interface, and the surface journal June 2012

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