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1.
Nat Commun ; 15(1): 101, 2024 Jan 02.
Article in English | MEDLINE | ID: mdl-38168078

ABSTRACT

The greatly nonlinear diffraction of high-energy electron probes focused to subatomic diameters frustrates the direct inversion of ptychographic data sets to decipher the atomic structure. Several iterative algorithms have been proposed to yield atomically-resolved phase distributions within slices of a 3D specimen, corresponding to the scattering centers of the electron wave. By pixelwise phase retrieval, current approaches do not only involve orders of magnitude more free parameters than necessary, but also neglect essential details of scattering physics such as the atomistic nature of the specimen and thermal effects. Here, we introduce a parametrized, fully differentiable scheme employing neural network concepts which allows the inversion of ptychographic data by means of entirely physical quantities. Omnipresent thermal diffuse scattering in thick specimens is treated accurately using frozen phonons, and atom types, positions and partial coherence are accounted for in the inverse model as relativistic scattering theory demands. Our approach exploits 4D experimental data collected in an aberration-corrected momentum-resolved scanning transmission electron microscopy setup. Atom positions in a 20 nm thick PbZr0.2Ti0.8O3 ferroelectric are measured with picometer precision, including the discrimination of different atom types and positions in mixed columns.

2.
ACS Nano ; 17(24): 25721-25730, 2023 Dec 26.
Article in English | MEDLINE | ID: mdl-38085927

ABSTRACT

Phase-change materials (PCMs) have been established as prime candidates for nonvolatile resonance tuning of nanophotonic components based on a large optical contrast between their amorphous and crystalline states. Recently, the plasmonic PCM In3SbTe2 was introduced, which can be switched from an amorphous dielectric state to a crystalline metallic one over the entire infrared spectral range. While locally switching the PCM around metallic nanorod antennas has already been demonstrated, similar tuning of inverse antenna structures (nanoslits) has not yet been investigated. Here, we demonstrate optical resonance tuning of nanoslit antennas with dielectric and plasmonic PCMs. We compare two geometries with fundamentally different resonance tuning mechanisms: tuning the resonance of aluminum slit antennas by change of the refractive index (dielectric PCM Ge3Sb2Te6), and creating slit-like volumes of amorphous In3SbTe2 and modifying the slit geometry directly (plasmonic PCM In3SbTe2). While the tuning range with the plasmonic PCM is about 3.4 µm and only limited by fabrication, the resonances with the dielectric PCM feature a three times larger quality factor compared to resonances obtained with the plasmonic PCM.

3.
Microsc Microanal ; 29(2): 499-511, 2023 Apr 05.
Article in English | MEDLINE | ID: mdl-37749738

ABSTRACT

When using the unit cell average of first moment data from four-dimensional scanning transmission electron microscopy (4D-STEM) to characterize ferroelectric materials, a variety of sources of systematic errors needs to be taken into account. In particular, these are the magnitude of the acceleration voltage, STEM probe semi-convergence angle, sample thickness, and sample tilt out of zone axis. Simulations show that a systematic error of calculated electric fields using the unit cell averaged momentum transfer originates from violation of point symmetry within the unit cells. Thus, values can easily exceed those of potential polarization-induced electric fields in ferroelectrics. Importantly, this systematic error produces deflection gradients between different domains seemingly representing measured fields. However, it could be shown that for PbZr0.2Ti0.8O3, many adjacent domains exhibit a relative crystallographic mistilt and in-plane rotation. The experimental results show that the method gives qualitative domain contrast. Comparison of the calculated electric field with the systematic error showed that the domain contrast of the unit cell averaged electric fields is mainly caused by dynamical scattering effects and the electric field plays only a minor role, if present at all.

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