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Abstract Oxide heterostructures exhibit a vast variety of unique physical properties. Examples are unconventional superconductivity in layered nickelates and topological polar order in (PbTiO₃)_n/(SrTiO₃)_nsuperlattices. Although it is clear that variations in oxygen content are crucial for the electronic correlation phenomena in oxides, it remains a major challenge to quantify their impact. Here, we measure the chemical composition in multiferroic (LuFeO₃)₉/(LuFe₂O₄)₁superlattices, mapping correlations between the distribution of oxygen vacancies and the electric and magnetic properties. Using atom probe tomography, we observe oxygen vacancies arranging in a layered three-dimensional structure with a local density on the order of 10¹⁴cm⁻², congruent with the formula-unit-thick ferrimagnetic LuFe₂O₄layers. The vacancy order is promoted by the locally reduced formation energy and plays a key role in stabilizing the ferroelectric domains and ferrimagnetism in the LuFeO₃and LuFe₂O₄layers, respectively. The results demonstrate pronounced interactions between oxygen vacancies and the multiferroic order in this system and establish an approach for quantifying the oxygen defects with atomic-scale precision in 3D, giving new opportunities for deterministic defect-enabled property control in oxide heterostructures. 

Abstract Measuring local polar ordering is key to understanding ferroelectricity in thin films, especially for systems with small domains or significant disorder. Scanning nanobeam electron diffraction (NBED) provides an effective local probe of lattice parameters, local fields, polarization directions, and charge densities, which can be analyzed using a relatively low beam dose over large fields of view. However, quantitatively extracting the magnitudes and directions of polarization vectors from NBED remains challenging. Here, we use a cepstral approach, similar to a pair distribution function, to determine local polar displacements that drive ferroelectricity from NBED patterns. Because polar distortions generate asymmetry in the diffraction pattern intensity, we can efficiently recover the underlying displacements from the imaginary part of the cepstrum transform. We investigate the limits of this technique using analytical and simulated data and give experimental examples, achieving the order of 1.1 pm precision and mapping of polar displacements with nanometer resolution. 

Abstract The quantum anomalous Hall (QAH) effect is characterized by a dissipationless chiral edge state with a quantized Hall resistance at zero magnetic field. Manipulating the QAH state is of great importance in both the understanding of topological quantum physics and the implementation of dissipationless electronics. Here, the QAH effect is realized in the magnetic topological insulator Cr‐doped (Bi,Sb)₂Te₃(CBST) grown on an uncompensated antiferromagnetic insulator Al‐doped Cr₂O₃. Through polarized neutron reflectometry (PNR), a strong exchange coupling is found between CBST and Al‐Cr₂O₃surface spins fixing interfacial magnetic moments perpendicular to the film plane. The interfacial coupling results in an exchange‐biased QAH effect. This study further demonstrates that the magnitude and sign of the exchange bias can be effectively controlled using a field training process to set the magnetization of the Al‐Cr₂O₃layer. It demonstrates the use of the exchange bias effect to effectively manipulate the QAH state, opening new possibilities in QAH‐based spintronics. 

Transmission electron microscopes use electrons with wavelengths of a few picometers, potentially capable of imaging individual atoms in solids at a resolution ultimately set by the intrinsic size of an atom. However, owing to lens aberrations and multiple scattering of electrons in the sample, the image resolution is reduced by a factor of 3 to 10. By inversely solving the multiple scattering problem and overcoming the electron-probe aberrations using electron ptychography, we demonstrate an instrumental blurring of less than 20 picometers and a linear phase response in thick samples. The measured widths of atomic columns are limited by thermal fluctuations of the atoms. Our method is also capable of locating embedded atomic dopant atoms in all three dimensions with subnanometer precision from only a single projection measurement.