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Register a new userIn-situ real-space imaging of crystal surface reconstruction dynamics via electron microscopy
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Crystal surfaces are sensitive to the surrounding environment, where atoms left with broken bonds reconstruct to minimize surface energy. In many cases, the surface can exhibit chemical properties unique from the bulk. These differences are important as they control reactions and mediate thin film growth. This is particularly true for complex oxides where certain terminating crystal planes are polar and have a net dipole moment. For polar terminations, reconstruction of atoms on the surface is the central mechanism to avoid the so called polar catastrophe. This adds to the complexity of the reconstruction where charge polarization and stoichiometry govern the final surface in addition to standard thermodynamic parameters such as temperature and partial pressure. Here we present direct, in-situ determination of polar SrTiO3 (110) surfaces at temperatures up to 900 C using cross-sectional aberration corrected scanning transmission electron microscopy (STEM). Under these conditions, we observe the coexistence of various surface structures that change as a function of temperature. As the specimen temperature is lowered, the reconstructed surface evolves due to thermal mismatch with the substrate. Periodic defects, similar to dislocations, are found in these surface structures and act to relieve stress due to mismatch. Combining STEM observations and electron spectroscopy with density functional theory, we find a combination of lattice misfit and charge compensation for stabilization. Beyond the characterization of these complex reconstructions, we have developed a general framework that opens a new pathway to simultaneously investigate the surface and near surface regions of single crystals as a function of environment.
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Understanding the fundamental dynamics of topological vortex and antivortex naturally formed in micro/nanoscale ferromagnetic building blocks under external perturbations is crucial to magnetic vortex based information processing and spintronic devices. All previous studies have focused on magnetic vortex-core switching via external magnetic fields, spin-polarized currents, or spin waves, which have largely prohibited the investigation of novel spin configurations that could emerge from the ground states in ferromagnetic disks and their underlying dynamics. Here, we report in situ visualization of femtosecond laser quenching induced magnetic vortex change in various symmetric ferromagnetic Permalloy disks by Lorentz phase imaging using 4D electron microscopy. Besides the switching of magnetic vortex chirality and polarity, we observed with distinct occurrence frequencies a plenitude of complex magnetic structures that have never been observed by magnetic field or current assisted switching. These complex magnetic structures consist of a number of newly created topological magnetic defects (vortex and antivortex) strictly conserving the topological winding number, demonstrating the direct impact of topological invariant on the magnetization dynamics in ferromagnetic disks. Their spin configurations show mirror or rotation symmetry due to the geometrical confinement of the disks. Combined micromagnetic simulations with the experimental observations reveal the underlying magnetization dynamics and formation mechanism of the optical quenching induced complex magnetic structures. Their distinct occurrence rates are pertinent to their formation-growth energetics and pinning effects at the disk edge. Based on these findings, we propose a paradigm of optical-quenching-assisted fast switching of vortex cores for the control of magnetic vortex based information recording and spintronic devices.
Effects of the Verwey transition on the (100) surface of magnetite were studied using scanning tunelling microscopy and spin polarized low-energy electron microsccopy. On cooling through the transition temperature Tv, the initially flat surface undergoes a roof-like distortion with a periodicity of ~0.5 um due to ferroelastic twinning within monoclinic domains of the low-temperature monoclinic structure. The monoclinic c axis orients in the surface plane, along the [001]c directions. At the atomic scale, the charge-ordered sqrt2xsqrt2R45 reconstruction of the (100) surface is unperturbed by the bulk transition, and is continuous over the twin boundaries. Time resolved low-energy electron microscopy movies reveal the structural transition to be first-order at the surface, indicating that the bulk transition is not an extension of the Verwey-like sqrt2xsqrt2R45 reconstruction. Although conceptually similar, the charge-ordered phases of the (100) surface and sub-Tv bulk of magnetite are unrelated phenomena.
An anisotropic charge distribution on individual atoms, such as e.g. {sigma}-hole, may strongly affect material and structural properties of systems. Nevertheless, subatomic resolution of such anisotropic charge distributions represents a long-standing experimental challenge. In particular, the existence of the {sigma}-hole on halogen atoms has been demonstrated only indirectly through determination of crystal structures of organic molecules containing halogens or via theoretical calculations. Nevertheless, its direct experimental visualization has not been reported yet. Here we demonstrate that Kelvin probe force microscopy, with a properly functionalized probe, can reach subatomic resolution imaging the {sigma}-hole or a quadrupolar charge of carbon monoxide molecule. This achievement opens new way to characterize biological and chemical systems where anisotropic atomic charges play decisive role.
To visualize the topography of thin oxide films during growth, thereby enabling to study its growth behavior quasi real-time, we have designed and integrated an atomic force microscope (AFM) in a pulsed laser deposition (PLD) vacuum setup. The AFM scanner and PLD target are integrated in a single support frame, combined with a fast sample transfer method, such that in-situ microscopy can be utilized after subsequent deposition pulses. The in-situ microscope can be operated from room temperature (RT) up to 700$^circ$C and at (process) pressures ranging from the vacuum base pressure of 10$^{-6}$ mbar up to 1 mbar, typical PLD conditions for the growth of oxide films. The performance of this instrument is demonstrated by resolving unit cell height surface steps and surface topography under typical oxide PLD growth conditions.
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