Detecting charge transfer at defects in 2D materials with electron ptychography

Charge transfer between atoms is fundamental to chemical bonding but has remained very challenging to detect directly in real space. Atomic-resolution imaging of charge density is not sufficient by itself, as the change in the density due to bonding is subtle compared to the total local charge density. Both sufficiently high sensitivity and accuracy are required, which we demonstrate here for the detection of charge transfer at defects in two-dimensional WS\textsubscript{2} via high-speed electron ptychography and its ability to correct errors due to residual lens aberrations

Efficient first principles simulation of electron scattering factors for transmission electron microscopy

Electron microscopy is a powerful tool for studying the properties of materials down to their atomic structure. In many cases, the quantitative interpretation of images requires simulations based on atomistic structure models. These typically use the independent atom approximation that neglects bonding effects, which may, however, be measurable and of physical interest. Since all electrons and the nuclear cores contribute to the scattering potential, simulations that go beyond this approximation have relied on computationally highly demanding all-electron calculations. Here, we describe a new method to generate ab initio electrostatic potentials when describing the core electrons by projector functions. Combined with an interface to quantitative image simulations, this implementation enables an easy and fast means to model electron microscopy images. We compare simulated transmission electron microscopy images and diffraction patterns to experimental data, showing an accuracy equivalent to earlier all-electron calculations at a much lower computational cost.Comment: 10 pages, 5 figures, 2 table

High On/Off ratio memristive switching of manganite/cuprate bilayer by interfacial magnetoelectricity

Memristive switching serves as the basis for a new generation of electronic devices. Memristors are two-terminal devices in which the current is turned on and off by redistributing point defects, e.g., vacancies, which is difficult to control. Memristors based on alternative mechanisms have been explored, but achieving both the high On/Off ratio and the low switching energy desirable for use in electronics remains a challenge. Here we report memristive switching in a La_(0.7)Ca_(0.3)MnO_(3)/PrBa_(2)Cu_(3)O_(7) bilayer with an On/Off ratio greater than 103 and demonstrate that the phenomenon originates from a new type of interfacial magnetoelectricity. Using results from firstprinciples calculations, we show that an external electric-field induces subtle displacements of the interfacial Mn ions, which switches on/off an interfacial magnetic “dead” layer, resulting in memristive behavior for spin-polarized electron transport across the bilayer. The interfacial nature of the switching entails low energy cost about of a tenth of atto Joule for write/erase a “bit”. Our results indicate new opportunities for manganite/cuprate systems and other transition-metal-oxide junctions in memristive applications

Direct Imaging of Charge Redistribution due to Bonding at Atomic Resolution via Electron Ptychography

Phase imaging in electron microscopy is sensitive to the local potential including charge redistribution from bonding. We demonstrate that electron ptychography provides the necessary sensitivity to detect this subtle effect by directly imaging the charge redistribution in single layer boron nitride. Residual aberrations can be measured and corrected post-collection, and simultaneous atomic number contrast imaging provides unambiguous sub-lattice identification. Density functional theory calculations confirm the detection of charge redistribution

Effect of maghemization on the magnetic properties of nonstoichiometric pseudo-single-domain magnetite particles

The effect of maghemization on the magnetic properties of magnetite (Fe3O4) grains in the pseudo-single-domain (PSD) size range is investigated as a function of annealing temperature. X-ray diffraction and transmission electron microscopy confirm the precursor grains as Fe3O4 ranging from ∼150 to ∼250 nm in diameter, whilst Mössbauer spectrometry suggests the grains are initially near-stoichiometric. The Fe3O4 grains are heated to increasing reaction temperatures of 120–220°C to investigate their oxidation to maghemite (γ-Fe2O3). High-angle annular dark field imaging and localized electron-energy loss spectroscopy reveal slightly oxidized Fe3O4 grains, heated to 140°C, exhibit higher oxygen content at the surface. Off-axis electron holography allows for construction of magnetic induction maps of individual Fe3O4 and γ-Fe2O3 grains, revealing their PSD (vortex) nature, which is supported by magnetic hysteresis measurements, including first-order reversal curve analysis. The coercivity of the grains is shown to increase with reaction temperature up to 180°C, but subsequently decreases after heating above 200°C; this magnetic behavior is attributed to the growth of a γ-Fe2O3 shell with magnetic properties distinct from the Fe3O4 core. It is suggested there is exchange coupling between these separate components that results in a vortex state with reduced vorticity. Once fully oxidized to γ-Fe2O3, the domain states revert back to vortices with slightly reduced coercivity. It is argued that due to a core/shell coupling mechanism during maghemization, the directional magnetic information will still be correct; however, the intensity information will not be retained