Structural effects of (111) growth of <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:msub> <mml:mi>La</mml:mi> <mml:mn>2</mml:mn> </mml:msub> <mml:msub> <mml:mi>CoMnO</mml:mi> <mml:mn>6</mml:mn> </mml:msub> </mml:mrow> </mm

The three-dimensional orientation of La atom modulations has been mapped in two thin films of <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"> <a:mrow> <a:msub> <a:mi>La</a:mi> <a:mn>2</a:mn> </a:msub> <a:msub> <a:mi>CoMnO</a:mi> <a:mn>6</a:mn> </a:msub> </a:mrow> </a:math> grown on <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"> <b:msub> <b:mi>SrTiO</b:mi> <b:mn>3</b:mn> </b:msub> </b:math> and LSAT ([La,Sr,Al,Ta] oxide) using a 4D-scanning transmission electron microscopy method based on the recently developed Digital Dark Field method. This images the shifts of diffraction spots and the azimuthal intensity distribution in the First-Order Laue Zone, and then uses them to reconstruct and map the 3D crystallography. This clearly shows a flip from out-of-plane modulation with tensile strain on <c:math xmlns:c="http://www.w3.org/1998/Math/MathML"> <c:msub> <c:mi>SrTiO</c:mi> <c:mn>3</c:mn> </c:msub> </c:math> to in-plane modulation with compressive strain on LSAT. This hitherto unobserved crystallographic change had a significant influence on the out-of-plane lattice parameter which left more room for the full incorporation of the larger <d:math xmlns:d="http://www.w3.org/1998/Math/MathML"> <d:msub> <d:mi>CoO</d:mi> <d:mn>6</d:mn> </d:msub> </d:math> octahedra in the film grown on LSAT and therefore explained the improved Mn-Co ordering and better properties for this film. Moreover, the method would be applicable to many other systems of epitaxial growth of complex oxides, revealing crystallographic details of crucial importance to properties which are not visible in conventional atomic resolution imaging.