Origin of insulating and nonferromagnetic SrRuO3 monolayers

Ali, Zeeshan; Wang, Zhen; O’Hara, Andrew; Saghayezhian, Mohammad; Shin, Donghan; Zhu, Yimei; Pantelides, Sokrates T.; Zhang, Jiandi

doi:10.1103/physrevb.105.054429

Title: Origin of insulating and nonferromagnetic SrRuO₃ monolayers

Journal Article · 24 February 2022 · Physical Review. B

DOI: https://doi.org/10.1103/physrevb.105.054429 · OSTI ID:1867028

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Louisiana State Univ., Baton Rouge, LA (United States); Louisiana State University and A&M College
Louisiana State Univ., Baton Rouge, LA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Vanderbilt Univ., Nashville, TN (United States)
Louisiana State Univ., Baton Rouge, LA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Louisiana State Univ., Baton Rouge, LA (United States); Chinese Academy of Sciences (CAS), Beijing (China)

The electro-magnetic properties of ultrathin epitaxial ruthenate films have long been the subject of debate. Here we combine experimental with theoretical investigations of (SrTiO₃)⁵-(SrRuO₃)ⁿ-(SrTiO₃)⁵ (STO⁵-SROⁿ-STO⁵) heterostructures with n = 1 and 2 unit cells, including extensive atomic-resolution scanning-transmission-electron-microscopy imaging, electron-energy-loss-spectroscopy chemical mapping, as well as transport and magneto-transport measurements. The experimental data demonstrate that the STO⁵-SRO²-STO⁵ heterostructure is nearly stoichiometric, metallic, and ferromagnetic with T_C ~ 128 K, even though it lacks the characteristic bulk-SRO octahedral tilts and matches the cubic STO structure. In contrast, the STO⁵-SRO¹-STO⁵ heterostructure features Ru-Ti intermixing in the RuO₂ layer, also without octahedral tilts, but is accompanied by a loss of metallicity and ferromagnetism. Density-functional-theory calculations show that stoichiometric n = 1 and n = 2 heterostructures are metallic and ferromagnetic with no octahedral tilts, while non-stoichiometry in the Ru sublattice in the n = 1 case opens an energy gap and induces antiferromagnetic ordering. Furthermore, the results indicate that the observed non-stoichiometry is the cause of the observed loss of metallicity and ferromagnetism in the n = 1 case.

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Research Organization:: Louisiana State Univ., Baton Rouge, LA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: SC0002136; SC0012704; FG02-09ER46554; AC02-05CH11231

OSTI ID:: 1867028

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 5 Vol. 105; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Origin of insulating and nonferromagnetic SrRuO3 monolayers

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Title: Origin of insulating and nonferromagnetic SrRuO₃ monolayers