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Route to achieving perfect B-site ordering in double perovskite thin films

Josée E Kleibeuker, Eun-Mi Choi, Edward D Jones, Tse-Min Yu, Bianca Sala, Belinda A MacLaren, Demie Kepaptsoglou, David Hernandez-Maldonado, Quentin M Ramasse, Lewys Jones, Juri Barthel, Ian MacLaren and Judith L MacManus-Driscoll

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Figure 1 - Unfortunately we are unable to provide accessible alternative text for this. If you require assistance to access this image, please contact help@nature.com or the author

Figure 1.

The effect of compressive in-plane strain on the BO6 octahedra of a cubic ABO3 structure on substrates with (001)-orientation (a) and (111)-orientation (b), where the green lines indicate a reduced dB-O and the red lines indicate an elongated dB-O compared to the non-strained BO6. Schematic drawings of the oxygen octahedra in perovskite films that contain anti-phase rotations after applying in-plane compressive strain are shown in (c and d); (c) for (001)-oriented films and (d) for (111)-oriented films. The oxygen ions are at the corners of the octahedra and the B cations are at the center of the octahedra. The A-site cations are not depicted but would lie in the open spaces between the octahedra. The cubes depict the pseudocubic ABO3 unit cell. The two different octahedra formed in a film on the (111)-oriented substrate are depicted in blue and red. The zig-zag pattern of the -O-B-O-B- chain is highlighted in black.

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Figure 2.

(a) The pseudocubic lattice parameters and mismatch of various perovskite substrates and La2CoMnO6. (b) XRD out-of-plane diffraction patterns around the (111)pc of La2CoMnO6 films grown on the various substrates along the (111). The La2CoMnO6 peak is marked by (*), the sharp intense peaks are from the substrate. (c and d) Reciprocal space maps of La2CoMnO6 grown on LSAT (111) and (001), respectively.

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Figure 3.

The normalized M(T) data of the La2CoMnO6 films on (a) the (111)-oriented substrates and (b) the (001)-oriented substrates. The arrow in a marks the TC of La2CoMnO6 on LSAT (111) at 211K. The inset of a shows normalized M(T) and χ(T) of La2CoMnO6 on LSAT (111) near TC as well as its corresponding Curie–Weiss fit. The in-plane M(H) hysteresis curves of the corresponding films at 5K are shown in c and d. A linear paramagnetic background of the SrTiO3 substrate was subtracted.

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Figure 4.

STEM of the structure and chemistry of La2CoMnO6 films on (111)-oriented LSAT and (111)-oriented SrTiO3: (a) high-angle annular dark field STEM image of 10nm2 of the substrate-film interface for the La2CoMnO6 film on LSAT, with the approximate interface position delineated, the partial Al-Ta ordering in the LSAT is easily seen; (b) superimposed EELS maps of Mn (green) and Co (blue) showing a high degree of ordering for the La2CoMnO6 film on LSAT; (c) detailed EEL spectrum around the Mn-L2,3 edge for the bulk of the La2CoMnO6 film on LSAT compared to standards; (d) detailed EEL spectrum around the Co-L2,3 edge from the same area as (c) compared to standards; (e) low-angle annular dark field-STEM image of 10nm2 of La2CoMnO6 on SrTiO3, with the approximate interface position delineated; (f) superimposed Mn (green) and Co (blue) EELS maps of an area within the centre of the film on SrTiO3 showing some columns richer in one element, but no clear evidence of long-range Co-Mn ordering; (g) detailed EEL spectrum around the Mn-L2,3 edge for the bulk of the La2CoMnO6 film on SrTiO3 compared to standards; (h) detailed EEL spectrum around the Co-L2,3 edge from the same area as (g) compared to standards.

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Figure 5.

(a) Superimposed EELS maps of oxygen (red), Mn (green) and Co (blue) of La2CoMnO6 on LSAT from the same area as Figure 4b showing a clear zig-zag pattern of the oxygen positions, meaning strong correlated octahedral tilting; (b) ABF image (5nm2) of La2CoMnO6 on SrTiO3 at the interface showing a clear zig-zag of the oxygen positions, which is consistent with octahedral tilting; (c) plot of tilt angle for the octahedral tilting going from the SrTiO3 substrate into La2CoMnO6, the dotted line is a guide-to-the-eye; (d) plot of (111)pc spacings between A-site layers going from the LSAT substrate into the La2CoMnO6 film, the dotted line is a guide-to-the-eye; and (e) plot of (111)pc spacings between A-site layers going from the SrTiO3 substrate into the La2CoMnO6 film, the dotted line is a guide-to-the-eye.

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Figure 6.

STEM imaging and electron energy loss spectroscopy spectrum imaging of non-stoichiometry at the substrate-film interface: (a) high-angle annular dark field-STEM image of Co-rich particles at the interface of La2CoMnO6 on SrTiO3; (b) atomic resolution high-angle annular dark-field-STEM image of the atomic structure of a particle in the La2CoMnO6 film on LSAT; (c) superimposed Co-Mn EELS map of the particle in b, where Co is blue and Mn is green; (d) superimposed Co-Mn EELS map, where Co is blue and Mn is green, of an interface area on LSAT that was free of Co-rich particles. The yellow dotted line indicates the interface between LSAT and La2CoMnO6.

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