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Annick De Backer

Publications and source records attributed to Annick De Backer.

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Designing dislocation-driven polar vortex networks in twisted perovskites

Twisting two atomic layers produces a geometric moire pattern, but bonding-induced interfacial reconstruction fundamentally transforms this into an ordered dislocation network - a distinction obscured in weakly-bonded van der Waals systems. Although in-plane topological vortex nanostructures arising from twisting-induced lateral strain modulation have been linked to periodic moire patterns in freestanding perovskite layers and 2D bilayers, their coupling to the interfacial dislocation network in twisted layers remains unresolved. Here we demonstrate that twisting freestanding SrTiO3 layers undergo interfacial reconstruction into a network of screw dislocations, accompanied by the emergence of in-plane topological vortices. Unlike in previous reports, these vortices are associated with the periodicity of the dislocation network rather than with geometric moire patterns. Four-dimensional scanning transmission electron microscopy (4D-STEM) reveals long-range ordered vortex-antivortex arrays with nearly continuous polarisation rotation. A machine-learning interatomic potential, trained on first-principles calculations, together with phase-field modelling, confirms that competing strains within the dislocation network stabilize polar vortex-antivortex pairs and drive the emergence of an electronic superlattice with a well-defined periodicity. Our results establish twist-controlled dislocation networks as a new and versatile route to designing local polar and electronic structures in oxide materials.

cond-mat.mtrl-sci

Halide Perovskite-Chalcohalide Nanocrystal Heterostructures as a Platform for the Synthesis and Investigation of the CsPbCl3-CsPbI3 Epitaxial Interface

Halide exchange in lead-based halide perovskites has been studied extensively. While mixed Cl-Br or Br-I alloy compositions can be formed with no miscibility gaps, this is precluded for mixed Cl-I compositions, due to the large difference in Cl and I ionic radii. Here, we exploit perovskite-chalcohalide CsPbCl3-Pb4S3Cl2 heterostructures to study the Cl-I exchange and isolate new types of intermediate structures. The epitaxial interface between the Pb4S3Cl2 chalcohalide and the CsPbCl3 perovskite domain significantly influences the intermediate stages of halide exchange in the perovskite domain, leading to coexisting CsPbCl3 and CsPbI3 domains, thereby delivering segmented CsPbI3-CsPbCl3-Pb4S3Cl2 energetically favorable heterostructures, with partial iodide alloying of the CsPbCl3 domain and at the perovskite-chalcohalide interface. The I:CsPbCl3 domain between CsPbI3 and Pb4S3Cl2 enables a gradual lattice expansion across the heterostructure. This design accommodates interfacial strain, with a 5.6% mismatch at the CsPbCl3-CsPbI3 interface and a 3.4% mismatch at the perovskite-chalcohalide interface. Full halide exchange leads to CsPbI3-Pb4S3Cl2 heterostructures. Both in intermediate and fully exchanged heterostructures, the CsPbI3 domain is emissive. In the intermediate structures, the band alignment between the two perovskite domains is type-I, with carriers photogenerated in the CsPbCl3 domain quickly transferring to the CsPbI3 domain, where they can recombine radiatively.

cond-mat.mtrl-sci

Towards atom counting from first moment STEM images: methodology and possibilities

Through a simulation-based study we develop a statistical model-based quantification method for atomic resolution first moment scanning transmission electron microscopy (STEM) images. This method uses the uniformly weighted least squares estimator to determine the unknown structure parameters of the images and to isolate contributions from individual atomic columns. In this way, a quantification of the projected potential per atomic column is achieved. Since the integrated projected potential of an atomic column scales linearly with the number of atoms it contains, it can serve as a basis for atom counting. The performance of atom counting from first moment STEM imaging is compared to that from traditional HAADF STEM in the presence of noise. Through this comparison, we demonstrate the advantage of first moment STEM images to attain more precise atom counts. Finally, we compare the integrated intensities extracted from first-moment images of a wedge-shaped sample to those values from the bulk crystal. The excellent agreement found between these values proves the robustness of using bulk crystal simulations as a reference library. This enables atom counting for samples with different shapes by comparison with these library values.

cond-mat.mtrl-sci

Fast generation of calculated ADF-EDX scattering cross-sections under channelling conditions

Advanced materials often consist of multiple elements which are arranged in a complicated structure. Quantitative scanning transmission electron microscopy is useful to determine the composition and thickness of nanostructures at the atomic scale. However, significant difficulties remain to quantify mixed columns by comparing the resulting atomic resolution images and spectroscopy data with multislice simulations where dynamic scattering needs to be taken into account. The combination of the computationally intensive nature of these simulations and the enormous amount of possible mixed column configurations for a given composition indeed severely hamper the quantification process. To overcome these challenges, we here report the development of an incoherent non-linear method for the fast prediction of ADF-EDX scattering cross-sections of mixed columns under channelling conditions. We first explain the origin of the ADF and EDX incoherence from scattering physics suggesting a linear dependence between those two signals in the case of a high-angle ADF detector. Taking EDX as a perfect incoherent reference mode, we quantitatively examine the ADF longitudinal incoherence under different microscope conditions using multislice simulations. Based on incoherent imaging, the atomic lensing model previously developed for ADF is now expanded to EDX, which yields ADF-EDX scattering cross-section predictions in good agreement with multislice simulations for mixed columns in a core-shell nanoparticle and a high entropy alloy. The fast and accurate prediction of ADF-EDX scattering cross-sections opens up new opportunities to explore the wide range of ordering possibilities of heterogeneous materials with multiple elements.

physics.app-ph

Procedure for 3D atomic resolution reconstructions using atom-counting and a Bayesian genetic algorithm

We introduce a Bayesian genetic algorithm for reconstructing atomic models of nanoparticles from a single projection using Z-contrast imaging. The number of atoms in a projected atomic column obtained from annular dark field scanning transmission electron microscopy (ADF STEM) images serves as an input for the initial three-dimensional (3D) model. The novel algorithm minimizes the energy of the structure while utilizing a priori information about the finite precision of the atom-counting results and neighbor-mass relations. The results show excellent prospects for obtaining reliable reconstructions of beam-sensitive nanoparticles during dynamical processes from images acquired with sufficiently low incident electron doses.

cond-mat.mtrl-sci