Electronic and vibrational signatures of ruthenium vacancies in 
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 thin films

Kim, Gideok; Suyolcu, Y. Eren; Herrero‐Martín, Javier; Putzky, Daniel; Nair, Hari P.; Ruf, Jacob; Schreiber, Nathaniel J.; Dietl, Christopher; Christiani, G.; Логвенов, Г.; Minola, M.; Aken, Peter A. van; Shen, Kyle; Schlom, Darrell G.; Keimer, B.

doi:10.1103/physrevmaterials.3.094802

Cited by 12 publications

(4 citation statements)

References 38 publications

(55 reference statements)

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“…We modified the density of Ru vacancies and the physical properties by adding Ru metal to the target and by varying the growth temperature. Following recent work on Sr 2 RuO 4 films 34 , we monitored the intensity of a Raman-active mode attributable to Ru vacancies and found that it is inversely related to the residual resistivity ratio (RRR), R xx (T = 320K)/R xx (T → 0), indicating that Ru vacancies are the major source of scattering of the conduction electrons (Fig. 1(c)).…”

Section: Resultsmentioning

confidence: 87%

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Kim,

Son,

Suyolcu

et al. 2020

Preprint

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Topological transport phenomena in magnetic materials are a major topic of current condensed matter research. One of the most widely studied phenomena is the "topological Hall effect" (THE), which is generated via spin-orbit interactions between conduction electrons and topological spin textures such as skyrmions. We report a comprehensive set of Hall effect and magnetization measurements on epitaxial films of the prototypical ferromagnetic metal SrRuO3 whose magnetic and transport properties were systematically modulated by varying the concentration of Ru vacancies. We observe Hall effect anomalies that closely resemble signatures of the THE, but a quantitative analysis demonstrates that they result from inhomogeneities in the ferromagnetic magnetization caused by a non-random distribution of Ru vacancies. As such inhomogeneities are difficult to avoid and are rarely characterized independently, our results call into question the identification of topological spin textures in numerous prior transport studies of quantum materials, heterostructures, and devices. Firm conclusions regarding the presence of such textures must meet stringent conditions such as probes that couple directly to the non-collinear magnetization on the atomic scale.

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Section: Resultsmentioning

confidence: 87%

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Kim,

Son,

Suyolcu

et al. 2020

Preprint

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“…Further studies are highly desirable. Additionally, since STEM-EDX confirms stoichiometric Ru content 36 on the SRO 214 thin films (see example in Supplementary Fig. 2b), our study focuses on the analysis of structural defects that could alter the superconducting transition.…”

Section: Resultsmentioning

confidence: 99%

Pair suppression caused by mosaic-twist defects in superconducting Sr2RuO4 thin-films prepared using pulsed laser deposition

et al. 2020

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Sr 2 RuO 4 (SRO 214) is a prototypical unconventional superconductor. However, since the discovery of its superconductivity a quarter of a century ago, the symmetry of the bulk and surface superconducting states in single crystal SRO 214 remains controversial. Solving this problem is massively impeded by the fact that superconducting SRO 214 is extremely challenging to achieve in thin-films as structural defects and impurities sensitively annihilate superconductivity. Here we report a protocol for the reliable growth of superconducting SRO 214 thin-films by pulsed laser deposition and identify universal materials properties that are destructive to the superconducting state. We demonstrate that careful control of the starting material is essential in order to achieve superconductivity and use a single crystal target of Sr 3 Ru 2 O 7 (SRO 327). By systematically varying the SRO 214 film thickness, we identify mosaic twist as the key in-plane defect that suppresses superconductivity. The results are central to the development of unconventional superconductivity.

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“…Note that the ρ ab of Sample set A was proportional to T 2 , which is indicative of SRO214. , Nevertheless, we only observed a plateau or slight drop in ρ ab down to 0.4 K (inset), indicating the absence of superconductivity or possibly incipient superconductivity, at best. Given that Sample set A exhibited no evidence of Ru deficiency according to Raman spectroscopy measurements (Figure S3 in the Supporting Information), we suggest that the high-density of OPBs is responsible for the absence of superconductivity in Sample set A.…”

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confidence: 87%

Superconducting Sr₂RuO₄ Thin Films without Out-of-Phase Boundaries by Higher-Order Ruddlesden–Popper Intergrowth

et al. 2021

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Ruddlesden–Popper (RP) phases (A n+1 B n O3n+1, n = 1, 2,···) have attracted intensive research with diverse functionalities for device applications. However, the realization of a high-quality RP-phase film is hindered by the formation of out-of-phase boundaries (OPBs) that occur at terrace edges, originating from lattice mismatch in the c-axis direction with the A′B′O3 (n = ∞) substrate. Here, using strontium ruthenate RP-phase Sr2RuO4 (n = 1) as a model system, an experimental approach for suppressing OPBs was developed. By tuning the growth parameters, the Sr3Ru2O7 (n = 2) phase was formed in a controlled manner near the film–substrate interface. This higher-order RP-phase then blocked the subsequent formation of OPBs, resulting in nearly defect-free Sr2RuO4 layer at the upper region of the film. Consequently, the Sr2RuO4 thin films exhibited superconductivity up to 1.15 K, which is the highest among Sr2RuO4 films grown by pulsed laser deposition. This work paves the way for synthesizing pristine RP-phase heterostructures and exploring their unique physical properties.

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Electronic and vibrational signatures of ruthenium vacancies in Sr2RuO4 thin films

Cited by 12 publications

References 38 publications

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Pair suppression caused by mosaic-twist defects in superconducting Sr2RuO4 thin-films prepared using pulsed laser deposition

Superconducting Sr₂RuO₄ Thin Films without Out-of-Phase Boundaries by Higher-Order Ruddlesden–Popper Intergrowth

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Electronic and vibrational signatures of ruthenium vacancies in Sr2RuO4 thin films

Cited by 12 publications

References 38 publications

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Pair suppression caused by mosaic-twist defects in superconducting Sr2RuO4 thin-films prepared using pulsed laser deposition

Superconducting Sr2RuO4 Thin Films without Out-of-Phase Boundaries by Higher-Order Ruddlesden–Popper Intergrowth

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Superconducting Sr₂RuO₄ Thin Films without Out-of-Phase Boundaries by Higher-Order Ruddlesden–Popper Intergrowth