Deep Learning Approach for High-accuracy Electron Counting of Monolithic Active Pixel Sensor-type Direct Electron Detectors at Increased Electron Dose.

Electron counting can be performed algorithmically for monolithic active pixel sensor direct electron detectors to eliminate readout noise and Landau noise arising from the variability in the amount of deposited energy for each electron. Errors in existing counting algorithms include mistakenly counting a multielectron strike as a single electron event, and inaccurately locating the incident position of the electron due to lateral spread of deposited energy and dark noise. Here, we report a supervised deep learning (DL) approach based on Faster region-based convolutional neural network (R-CNN) to recognize single electron events at varying electron doses and voltages. The DL approach shows high accuracy according to the near-ideal modulation transfer function (MTF) and detector quantum efficiency for sparse images. It predicts, on average, 0.47 pixel deviation from the incident positions for 200 kV electrons versus 0.59 pixel using the conventional counting method. The DL approach also shows better robustness against coincidence loss as the electron dose increases, maintaining the MTF at half Nyquist frequency above 0.83 as the electron density increases to 0.06 e-/pixel. Thus, the DL model extends the advantages of counting analysis to higher dose rates than conventional methods.

Ultrahigh Carrier Mobilities in Ferroelectric Domain Wall Corbino Cones at Room Temperature.

Recently, electrically conducting heterointerfaces between dissimilar band insulators (such as lanthanum aluminate and strontium titanate) have attracted considerable research interest. Charge transport and fundamental aspects of conduction have been thoroughly explored. Perhaps surprisingly, similar studies on conceptually much simpler conducting homointerfaces, such as domain walls, are not nearly so well developed. Addressing this disparity, magnetoresistance is herein reported in approximately conical 180° charged domain walls, in partially switched ferroelectric thin-film single-crystal lithium niobate. This system is ideal for such measurements: first, the conductivity difference between domains and domain walls is unusually large (a factor of 1013 ) and hence currents driven through the thin film, between planar top and bottom electrodes, are overwhelmingly channeled along the walls; second, when electrical contact is made to the top and bottom of the domain walls and a magnetic field is applied along their cone axes, then the test geometry mirrors that of a Corbino disk: a textbook arrangement for geometric magnetoresistance measurement. Data imply carriers with extremely high room-temperature Hall mobilities of up to ≈3700 cm2 V-1 s-1 . This is an unparalleled value for oxide interfaces (and for bulk oxides) comparable to mobilities in other systems seen at cryogenic, rather than at room, temperature.

TopoTEM: A Python Package for Quantifying and Visualizing Scanning Transmission Electron Microscopy Data of Polar Topologies.

The exotic internal structure of polar topologies in multiferroic materials offers a rich landscape for materials science research. As the spatial scale of these entities is often subatomic in nature, aberration-corrected transmission electron microscopy (TEM) is the ideal characterization technique. Software to quantify and visualize the slight shifts in atomic placement within unit cells is of paramount importance due to the now routine acquisition of images at such resolution. In the previous ~decade since the commercialization of aberration-corrected TEM, many research groups have written their own code to visualize these polar entities. More recently, open-access Python packages have been developed for the purpose of TEM atomic position quantification. Building on these packages, we introduce the TEMUL Toolkit: a Python package for analysis and visualization of atomic resolution images. Here, we focus specifically on the TopoTEM module of the toolkit where we show an easy to follow, streamlined version of calculating the atomic displacements relative to the surrounding lattice and thus plotting polarization. We hope this toolkit will benefit the rapidly expanding field of topology-based nano-electronic and quantum materials research, and we invite the electron microscopy community to contribute to this open-access project.

Charged Domain Wall and Polar Vortex Topologies in a Room-Temperature Magnetoelectric Multiferroic Thin Film.

Multiferroic topologies are an emerging solution for future low-power magnetic nanoelectronics due to their combined tuneable functionality and mobility. Here, we show that in addition to being magnetoelectric multiferroic at room temperature, thin-film Aurivillius phase Bi6TixFeyMnzO18 is an ideal material platform for both domain wall and vortex topology-based nanoelectronic devices. Utilizing atomic-resolution electron microscopy, we reveal the presence and structure of 180°-type charged head-to-head and tail-to-tail domain walls passing throughout the thin film. Theoretical calculations confirm the subunit cell cation site preference and charged domain wall energetics for Bi6TixFeyMnzO18. Finally, we show that polar vortex-type topologies also form at out-of-phase boundaries of stacking faults when internal strain and electrostatic energy gradients are altered. This study could pave the way for controlled polar vortex topology formation via strain engineering in other multiferroic thin films. Moreover, these results confirm that the subunit cell topological features play an important role in controlling the charge and spin state of Aurivillius phase films and other multiferroic heterostructures.

Anomalous Motion of Charged Domain Walls and Associated Negative Capacitance in Copper-Chlorine Boracite.

During switching, the microstructure of a ferroelectric normally adapts to align internal dipoles with external electric fields. Favorably oriented dipolar regions (domains) grow at the expense of those in unfavorable orientations and this is manifested in a predictable field-induced motion of the walls that separate one domain from the next. Here, the discovery that specific charged 90°domain walls in copper-chlorine boracite move in the opposite direction to that expected, increasing the size of the domain in which polarization is anti-aligned with the applied field, is reported. Polarization-field (P-E) hysteresis loops, inferred from optical imaging, show negative gradients and non-transient negative capacitance, throughout the P-E cycle. Switching currents (generated by the relative motion between domain walls and sensing electrodes) confirm this, insofar as their signs are opposite to those expected conventionally. For any given bias, the integrated switching charge due to this anomalous wall motion is directly proportional to time, indicating that the magnitude of the negative capacitance component should be inversely related to frequency. This passes Jonscher's test for the misinterpretation of positive inductance and gives confidence that field-induced motion of these specific charged domain walls generates a measurable negative capacitance contribution to the overall dielectric response.

Metal-ferroelectric supercrystals with periodically curved metallic layers.

Simultaneous manipulation of multiple boundary conditions in nanoscale heterostructures offers a versatile route to stabilizing unusual structures and emergent phases. Here, we show that a stable supercrystal phase comprising a three-dimensional ordering of nanoscale domains with tailored periodicities can be engineered in PbTiO3-SrRuO3 ferroelectric-metal superlattices. A combination of laboratory and synchrotron X-ray diffraction, piezoresponse force microscopy, scanning transmission electron microscopy and phase-field simulations reveals a complex hierarchical domain structure that forms to minimize the elastic and electrostatic energy. Large local deformations of the ferroelectric lattice are accommodated by periodic lattice modulations of the metallic SrRuO3 layers with curvatures up to 107 m-1. Our results show that multidomain ferroelectric systems can be exploited as versatile templates to induce large curvatures in correlated materials, and present a route for engineering correlated materials with modulated structural and electronic properties that can be controlled using electric fields.

Quantifying the Transverse-Electric-Dominant 260 nm Emission from Molecular Beam Epitaxy-Grown GaN-Quantum-Disks Embedded in AlN Nanowires: A Comprehensive Optical and Morphological Characterization.

There has been a relentless pursuit of transverse electric (TE)-dominant deep ultraviolet (UV) optoelectronic devices for efficient surface emitters to replace the environmentally unfriendly mercury lamps. To date, the use of the ternary AlGaN alloy inevitably has led to transverse magnetic (TM)-dominant emission, an approach that is facing a roadblock. Here, we take an entirely different approach of utilizing a binary GaN compound semiconductor in conjunction with ultrathin quantum disks (QDisks) embedded in AlN nanowires (NWs). The growth of GaN QDisks is realized on a scalable and low-cost Si substrate using plasma-assisted molecular beam epitaxy as a highly controllable monolayer growth platform. We estimated an internal quantum efficiency of ∼81% in a wavelength regime of ∼260 nm for these nanostructures. Additionally, strain mapping obtained by high-angle annular dark-field scanning transmission electron microscopy is studied in conjunction with the TE and TM modes of the carrier recombination. Moreover, for the first time, we quantify the TE and TM modes of the PL emitted by GaN QDisks for deep-UV emitters. We observed nearly pure TE-polarized photoluminescence emission at a polarization angle of ∼5°. This work proposes highly quantum-confined ultrathin GaN QDisks as a promising candidate for deep-UV vertical emitters.

Ferroelectric Domain Wall Memristor.

A domain wall-enabled memristor is created, in thin film lithium niobate capacitors, which shows up to twelve orders of magnitude variation in resistance. Such dramatic changes are caused by the injection of strongly inclined conducting ferroelectric domain walls, which provide conduits for current flow between electrodes. Varying the magnitude of the applied electric-field pulse, used to induce switching, alters the extent to which polarization reversal occurs; this systematically changes the density of the injected conducting domain walls in the ferroelectric layer and hence the resistivity of the capacitor structure as a whole. Hundreds of distinct conductance states can be produced, with current maxima achieved around the coercive voltage, where domain wall density is greatest, and minima associated with the almost fully switched ferroelectric (few domain walls). Significantly, this "domain wall memristor" demonstrates a plasticity effect: when a succession of voltage pulses of constant magnitude is applied, the resistance changes. Resistance plasticity opens the way for the domain wall memristor to be considered for artificial synapse applications in neuromorphic circuits.

Titanium Carbide MXene Nucleation Layer for Epitaxial Growth of High-Quality GaN Nanowires on Amorphous Substrates.

Growing III-nitride nanowires on 2D materials is advantageous, as it effectively decouples the underlying growth substrate from the properties of the nanowires. As a relatively new family of 2D materials, MXenes are promising candidates as III-nitride nanowire nucleation layers capable of providing simultaneous transparency and conductivity. In this work, we demonstrate the direct epitaxial growth of GaN nanowires on Ti3C2 MXene films. The MXene films consist of nanoflakes spray coated onto an amorphous silica substrate. We observed an epitaxial relationship between the GaN nanowires and the MXene nanoflakes due to the compatibility between the triangular lattice of Ti3C2 MXene and the hexagonal structure of wurtzite GaN. The GaN nanowires on MXene show good material quality and partial transparency at visible wavelengths. Nanoscale electrical characterization using conductive atomic force microscopy reveals a Schottky barrier height of ∼330 meV between the GaN nanowire and the Ti3C2 MXene film. Our work highlights the potential of using MXene as a transparent and conductive preorienting nucleation layer for high-quality GaN growth on amorphous substrates.

Germanium tin alloy nanowires as anode materials for high performance Li-ion batteries.

The combination of two active Li-ion materials (Ge and Sn) can result in improved conduction paths and higher capacity retention. Here we report for the first time, the implementation of Ge1-x Sn x alloy nanowires as anode materials for Li-ion batteries. Ge1-x Sn x alloy nanowires have been successfully grown via vapor-liquid-solid technique directly on stainless steel current collectors. Ge1-x Sn x (x = 0.048) nanowires were predominantly seeded from the Au0.80Ag0.20 catalysts with negligible amount of growth was also directly catalyzed from stainless steel substrate. The electrochemical performance of the the Ge1-x Sn x nanowires as an anode material for Li-ion batteries was investigated via galvanostatic cycling and detailed analysis of differential capacity plots (DCPs). The nanowire electrodes demonstrated an exceptional capacity retention of 93.4% from the 2nd to the 100th charge at a C/5 rate, while maintaining a specific capacity value of ∼921 mAh g-1 after 100 cycles. Voltage profiles and DCPs revealed that the Ge1-x Sn x nanowires behave as an alloying mode anode material, as reduction/oxidation peaks for both Ge and Sn were observed, however it is clear that the reversible lithiation of Ge is responsible for the majority of the charge stored.

Electrical Tunability of Domain Wall Conductivity in LiNbO3 Thin Films.

Domain wall nanoelectronics is a rapidly evolving field, which explores the diverse electronic properties of the ferroelectric domain walls for application in low-dimensional electronic systems. One of the most prominent features of the ferroelectric domain walls is their electrical conductivity. Here, using a combination of scanning probe and scanning transmission electron microscopy, the mechanism of the tunable conducting behavior of the domain walls in the sub-micrometer thick films of the technologically important ferroelectric LiNbO3 is explored. It is found that the electric bias generates stable domains with strongly inclined domain boundaries with the inclination angle reaching 20° with respect to the polar axis. The head-to-head domain boundaries exhibit high conductance, which can be modulated by application of the sub-coercive voltage. Electron microscopy visualization of the electrically written domains and piezoresponse force microscopy imaging of the very same domains reveals that the gradual and reversible transition between the conducting and insulating states of the domain walls results from the electrically induced wall bending near the sample surface. The observed modulation of the wall conductance is corroborated by the phase-field modeling. The results open a possibility for exploiting the conducting domain walls as the electrically controllable functional elements in the multilevel logic nanoelectronics devices.