Chemistry, growth kinetics, and epitaxial stabilization of Sn2+ in Sn-doped SrTiO3 using (CH3)6Sn2 tin precursor

Tianqi Wang, Krishna Chaitanya Pitike, Yakun Yuan, Serge M. Nakhmanson, Venkatraman Gopalan, Bharat Jalan

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Abstract

PbTiO3-based ferroelectrics have impressive electroactive properties, originating from the Pb2+ 6s2 electron lone-pair, which cause large elastic distortion and electric polarization due to cooperative pseudo Jahn-Teller effect. Recently, tin-based perovskite oxide (SnTiO3) containing Sn2+ and a chemistry similar to that of the 6s2 lone-pair has been identified as a thermally stable, environmentally friendly substitute for PbTiO3-based ferroelectrics. However experimental attempts to stabilize Sn2+ on the A-site of perovskite ATiO3 have so far failed. In this work, we report on the growth of atomically smooth, epitaxial, and coherent Sn-alloyed SrTiO3 films on SrTiO3 (001) substrates using a hybrid molecular beam epitaxy approach. With increasing Sn concentration, the out-of-plane lattice parameter first increases in accordance with the Vegard’s law and then decreases for Sn(Sr+Ti+Sn) at. % ratio > 0.1 due to the incorporation of Sn2+ at the A-site. Using a combination of high-resolution X-ray photoelectron spectroscopy and density functional calculations, we show that while majority of Sn is on the B-site, there is a quantitatively unknown fraction of Sn being consistent with the A-site occupancy making SrTiO3 polar. A relaxor-like ferroelectric local distortion with monoclinic symmetry, induced by A-site Sn2+, was observed in Sn-doped SrTiO3 with Sn(Sr+Ti+Sn) at. % ratio = 0.1 using optical second harmonic generation measurements. The role of growth kinetics on the stability of Sn2+ in SrTiO3 is discussed.

Original languageEnglish (US)
Article number126111
JournalAPL Materials
Volume4
Issue number12
DOIs
StatePublished - Dec 1 2016

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Tin
Growth kinetics
Ferroelectric materials
Stabilization
Perovskite
Jahn-Teller effect
Harmonic generation
Molecular beam epitaxy
Lattice constants
Density functional theory
X ray photoelectron spectroscopy
Polarization
Oxides
Electrons
Substrates
strontium titanium oxide

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Engineering(all)

Cite this

Wang, Tianqi ; Pitike, Krishna Chaitanya ; Yuan, Yakun ; Nakhmanson, Serge M. ; Gopalan, Venkatraman ; Jalan, Bharat. / Chemistry, growth kinetics, and epitaxial stabilization of Sn2+ in Sn-doped SrTiO3 using (CH3)6Sn2 tin precursor. In: APL Materials. 2016 ; Vol. 4, No. 12.
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abstract = "PbTiO3-based ferroelectrics have impressive electroactive properties, originating from the Pb2+ 6s2 electron lone-pair, which cause large elastic distortion and electric polarization due to cooperative pseudo Jahn-Teller effect. Recently, tin-based perovskite oxide (SnTiO3) containing Sn2+ and a chemistry similar to that of the 6s2 lone-pair has been identified as a thermally stable, environmentally friendly substitute for PbTiO3-based ferroelectrics. However experimental attempts to stabilize Sn2+ on the A-site of perovskite ATiO3 have so far failed. In this work, we report on the growth of atomically smooth, epitaxial, and coherent Sn-alloyed SrTiO3 films on SrTiO3 (001) substrates using a hybrid molecular beam epitaxy approach. With increasing Sn concentration, the out-of-plane lattice parameter first increases in accordance with the Vegard’s law and then decreases for Sn(Sr+Ti+Sn) at. {\%} ratio > 0.1 due to the incorporation of Sn2+ at the A-site. Using a combination of high-resolution X-ray photoelectron spectroscopy and density functional calculations, we show that while majority of Sn is on the B-site, there is a quantitatively unknown fraction of Sn being consistent with the A-site occupancy making SrTiO3 polar. A relaxor-like ferroelectric local distortion with monoclinic symmetry, induced by A-site Sn2+, was observed in Sn-doped SrTiO3 with Sn(Sr+Ti+Sn) at. {\%} ratio = 0.1 using optical second harmonic generation measurements. The role of growth kinetics on the stability of Sn2+ in SrTiO3 is discussed.",
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Chemistry, growth kinetics, and epitaxial stabilization of Sn2+ in Sn-doped SrTiO3 using (CH3)6Sn2 tin precursor. / Wang, Tianqi; Pitike, Krishna Chaitanya; Yuan, Yakun; Nakhmanson, Serge M.; Gopalan, Venkatraman; Jalan, Bharat.

In: APL Materials, Vol. 4, No. 12, 126111, 01.12.2016.

Research output: Contribution to journalArticle

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AU - Wang, Tianqi

AU - Pitike, Krishna Chaitanya

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AB - PbTiO3-based ferroelectrics have impressive electroactive properties, originating from the Pb2+ 6s2 electron lone-pair, which cause large elastic distortion and electric polarization due to cooperative pseudo Jahn-Teller effect. Recently, tin-based perovskite oxide (SnTiO3) containing Sn2+ and a chemistry similar to that of the 6s2 lone-pair has been identified as a thermally stable, environmentally friendly substitute for PbTiO3-based ferroelectrics. However experimental attempts to stabilize Sn2+ on the A-site of perovskite ATiO3 have so far failed. In this work, we report on the growth of atomically smooth, epitaxial, and coherent Sn-alloyed SrTiO3 films on SrTiO3 (001) substrates using a hybrid molecular beam epitaxy approach. With increasing Sn concentration, the out-of-plane lattice parameter first increases in accordance with the Vegard’s law and then decreases for Sn(Sr+Ti+Sn) at. % ratio > 0.1 due to the incorporation of Sn2+ at the A-site. Using a combination of high-resolution X-ray photoelectron spectroscopy and density functional calculations, we show that while majority of Sn is on the B-site, there is a quantitatively unknown fraction of Sn being consistent with the A-site occupancy making SrTiO3 polar. A relaxor-like ferroelectric local distortion with monoclinic symmetry, induced by A-site Sn2+, was observed in Sn-doped SrTiO3 with Sn(Sr+Ti+Sn) at. % ratio = 0.1 using optical second harmonic generation measurements. The role of growth kinetics on the stability of Sn2+ in SrTiO3 is discussed.

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