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A promising architecture for next-generation, low energy spintronic devices uses skyrmions -- nanoscale whirlpools of magnetic moment -- as information carriers. Notably, schemes for racetrack memory have been proposed in which skyrmions and antiskyrmions, their antiparticle, serve as the logical bits 1 and 0. However, major challenges exist to designing skyrmion-antiskyrmion based computing. The presence of both particles in one material is often mutually exclusive such that few systems have been identified in which they coexist, and in these systems their appearance is stochastic rather than deterministic. Here, we create a tunable skyrmion-antiskyrmion system in FeGe films through ion-irradiation and annealing, and detail the structural properties of the films under these various conditions. Specifically, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au$^{4+}$ ions, showing evidence that the amorphized regions preferentially host antiskyrmions at densities controlled by the irradiation fluence. In this work, we focus on a subsequent, systematic electron diffraction study with in-situ annealing, demonstrating the ability to recrystallize controllable fractions of the material at temperatures ranging from approximately 150$^{\circ}$ C to 250$^{\circ}$ C, enabling further tunability of skyrmion/antiskyrmion populations. We describe the crystallization kinetics using the Johnson-Mehl-Avrami-Kolmogorov model, finding that growth of crystalline grains is consistent with diffusion-controlled one-to-two dimensional growth with a decreasing nucleation rate. The procedures developed here can be applied towards creation of skyrmion-antiskyrmion systems for energy-efficient, high-density data storage, spin wave emission produced by skyrmion-antiskyrmion pair annihilation, and more generally testbeds for research on skyrmion-antiskyrmion liquids and crystals.

Sodium niobate, a lead-free ferroic material, hosts delicately-balanced, competing order parameters, including ferroelectric states that can be stabilized by epitaxial strain. Here, we show that the resulting macroscopic ferroelectricity exhibits an unconventional microscopic structure using multislice electron ptychography. This technique overcomes multiple scattering artifacts limiting conventional electron microscopy, enabling both lateral spatial resolution beyond the diffraction limit and recovery of three-dimensional structural information. These imaging capabilities allow us to separate the ferroelectric interior of the sample from the relaxed surface structure and identify the soft phonon mode and related structural distortions with picometer precision. Unlike conventional ferroelectric perovskites, we find that the polar distortion in this material involves minimal distortions of the cation sublattices and is instead dominated by anion displacements. We establish limits on film thickness for interfacial octahedral rotation engineering and directly visualize an incommensurate octahedral rotation pattern, arising from the flat dispersion of the associated phonon mode., Comment: 63 pages, 5 figures, 17 supplementary figures

Doping impurity atoms is a strategy commonly used to tune the functionality of materials including catalysts, semiconductors, and quantum emitters. The location of dopants and their interaction with surrounding atoms could significantly modulate the transport, optical, or magnetic properties of materials. However, directly imaging individual impurity atoms inside materials remains a generally unaddressed need. Here, we demonstrate how single atoms can be detected and located in three dimensions via multislice electron ptychography.Interstitial atoms in a complex garnet oxide heterostructure are resolved with a depth resolution better than 2.7 nm, together with a deep-sub-{\AA}ngstrom lateral resolution. Single-scan atomic-layer depth resolution should be possible using strongly divergent electron probe illumination. Our results provide a new approach to detecting individual atomic defects and open doors to characterize the local environments and spatial distributions that underlie a broad range of systems such as single-atom catalysts, nitrogen-vacancy centers, and other atomic-scale quantum sensors., Comment: 28 pages, 5 figures, 10 supplementary figures

Unlike non-polar semiconductors such as silicon, the broken inversion symmetry of the wide bandgap semiconductor gallium nitride leads to a large electronic polarization along a unique crystal axis. This makes the two surfaces of the semiconductor wafer perpendicular to the polar axis dramatically different in their physical and chemical properties. In the last three decades, the cation (gallium) face of gallium nitride has been used for photonic devices such as LEDs and lasers. Though the cation face has also been predominantly used for electronic devices, the anion (nitrogen) face has recently shown promise for high electron mobility transistors due to favorable polarization discontinuities. In this work we introduce dualtronics, showing that it is possible to make photonic devices on the cation face, and electronic devices on the anion face, of the same semiconductor wafer. This opens the possibility for leveraging both faces of polar semiconductors in a single structure, where electronic, photonic, and acoustic properties can be implemented on opposite faces of the same wafer, dramatically enhancing the functional capabilities of this revolutionary semiconductor family.

Progress in the study of infinite-layer nickelates has always been highly linked to materials advances. In particular, the recent development of superconductivity via hole-doping was predicated on the controlled synthesis of Ni in a very high oxidation state, and subsequent topotactic reduction to a very low oxidation state, currently limited to epitaxial thin films. Here we demonstrate a process to combine these steps with a heterostructure which includes an epitaxial soluble buffer layer, enabling the release of freestanding membranes of (Nd,Sr)NiO2 encapsulated in SrTiO3, which serves as a protective layer. The membranes have comparable structural and electronic properties to that of optimized thin films, and range in lateral dimensions from millimeters to ~100 micron fragments, depending on the degree of strain released with respect to the initial substrate. The changes in the superconducting transition temperature associated with membrane release are quite similar to those reported for substrate and pressure variations, suggestive of a common underlying mechanism. These membranes structures should provide a versatile platform for a range of experimental studies and devices free from substrate constraints.

Skyrmions and antiskyrmions are nanoscale swirling textures of magnetic moments formed by chiral interactions between atomic spins in magnetic non-centrosymmetric materials and multilayer films with broken inversion symmetry. These quasiparticles are of interest for use as information carriers in next-generation, low-energy spintronic applications. To develop skyrmion-based memory and logic, we must understand skyrmion-defect interactions with two main goals -- determining how skyrmions navigate intrinsic material defects and determining how to engineer disorder for optimal device operation. Here, we introduce a tunable means of creating a skyrmion-antiskyrmion system by engineering the disorder landscape in FeGe using ion irradiation. Specifically, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au$^{4+}$ ions at varying fluences, inducing amorphous regions within the crystalline matrix. Using low-temperature electrical transport and magnetization measurements, we observe a strong topological Hall effect with a double-peak feature that serves as a signature of skyrmions and antiskyrmions. These results are a step towards the development of information storage devices that use skyrmions and anitskyrmions as storage bits and our system may serve as a testbed for theoretically predicted phenomena in skyrmion-antiskyrmion crystals.

Square net tellurides host an array of electronic ground states and commonly exhibit charge-density-wave ordering. Here we report the epitaxy of DyTe$_{2-\delta}$ on atomically flat MgO (001) using molecular beam epitaxy. The films are single phase and highly oriented as evidenced by transmission electron microscopy and X-ray diffraction measurements. Epitaxial strain is evident in films and is relieved as the thickness increases up to a value of approximately 20 unit cells. Diffraction features associated with a supercell in the films are resolved which is coupled with Te-deficiency. First principles calculations attribute the formation of this defect lattice to nesting conditions in the Fermi surface, which produce a periodic occupancy of the conducting Te square-net, and opens a band gap at the chemical potential. This work establishes the groundwork for exploring the role of strain in tuning electronic and structural phases of epitaxial square-net tellurides and related compounds.

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature ($T_C$) in thin film Fe$_3$GeTe$_2$/Bi$_2$Te$_3$ from bulk-like values ($\sim$220 K) to above room temperature by increasing the growth temperature from 300 $^\circ$C to 375 $^\circ$C. For samples grown at 375 $^\circ$C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe$_m$Ge$_n$Te$_2$ compositions (e.g. Fe$_5$Ge$_2$Te$_2$ and Fe$_7$Ge$_6$Te$_2$) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. This observation paves the way for developing various Fe$_m$Ge$_n$Te$_2$/TI heterostructures with novel properties., Comment: 8 pages, 4 figures

Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the two-dimensional limit. Here, we report studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe3GeTe2 (FGT). The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plane anisotropy of the FGT, inducing a strongly tilted magnetic configuration in the FGT. Furthermore, the in-plane exchange bias provides sufficient symmetry breaking to allow deterministic spin-orbit torque switching of the FGT in CrSBr/FGT/Pt samples at zero applied magnetic field. A minimum thickness of the CrSBr greater than 10 nm is needed to provide a non-zero exchange bias at 30 K.

Surface strain plays a key role in enhancing the activity of Pt-alloy nanoparticle oxygen reduction catalysts. However, the details of strain effects in real fuel cell catalysts are not well-understood, in part due to a lack of strain characterization techniques that are suitable for complex supported nanoparticle catalysts. This work investigates these effects using strain mapping with nanobeam electron diffraction and a continuum elastic model of strain in simple core-shell particles. We find that surface strain is relaxed both by lattice defects at the core-shell interface and by relaxation across particle shells caused by Poisson expansion in the spherical geometry. The continuum elastic model finds that in the absence of lattice dislocations, geometric relaxation results in a surface strain that scales with the average composition of the particle, regardless of the shell thickness. We investigate the impact of these strain effects on catalytic activity for a series of Pt-Co catalysts treated to vary their shell thickness and core-shell lattice mismatch. For catalysts with the thinnest shells, the activity is consistent with an Arrhenius dependence on the surface strain expected for coherent strain in dislocation-free particles, while catalysts with thicker shells showed greater activity losses indicating strain relaxation caused by dislocations as well., Comment: 23 pages,7 figures, includes appendix

Using low-temperature cathodoluminescence spectroscopy, we study the properties of N- and Al-polar AlN layers grown by molecular beam epitaxy on bulk AlN{0001}. Compared to the bulk AlN substrate, layers of both polarities feature a suppression of deep-level luminescence, a total absence of the prevalent donor with an exciton binding energy of 28 meV, and a much increased intensity of the emission from free excitons. The dominant donor in these layers is characterized by an associated exciton binding energy of 13 meV. The observation of excited exciton states up to the exciton continuum allows us to directly extract the $\Gamma_{5}$ free exciton binding energy of 57 meV.

Intermetallic Nb3Sn alloys have long been believed to form through Sn diffusion into Nb. However, our observations of significant oxygen content in Nb3Sn prompted an investigation of alternative formation mechanisms. Through experiments involving different oxide interfaces (clean HF-treated, native oxidized, and anodized), we demonstrate a thermodynamic route that fundamentally challenges the conventional Sn diffusion mechanism for Nb3Sn nucleation. Our results highlight the critical involvement of a SnOx intermediate phase. This new nucleation mechanism identifies the principles for growth optimization and new synthesis of high-quality Nb3Sn superconductors.

Surface structures on radio-frequency (RF) superconductors are crucially important in determining their interaction with the RF field. Here we investigate the surface compositions, structural profiles, and valence distributions of oxides, carbides, and impurities on niobium (Nb) and niobium-tin (Nb3Sn) in situ under different processing conditions. We establish the underlying mechanisms of vacuum baking and nitrogen processing in Nb and demonstrate that carbide formation induced during high-temperature baking, regardless of gas environment, determines subsequent oxide formation upon air exposure or low-temperature baking, leading to modifications of the electron population profile. Our findings support the combined contribution of surface oxides and second-phase formation to the outcome of ultra-high vacuum baking (oxygen processing) and nitrogen processing. Also, we observe that vapor-diffused Nb3Sn contains thick metastable oxides, while electrochemically synthesized Nb3Sn only has a thin oxide layer. Our findings reveal fundamental mechanisms of baking and processing Nb and Nb3Sn surface structures for high-performance superconducting RF and quantum applications

The nature of superconductivity and its interplay with strong spin-orbit coupling at the KTaO3(111) interfaces remains a subject of debate. To address this problem, we grew epitaxial LaMnO3/KTaO3(111) heterostructures. We show that superconductivity is robust against the in-plane magnetic field, with the critical field of superconductivity reaching 25 T in optimally doped heterostructures. The superconducting order parameter is highly sensitive to carrier density. We argue that spin-orbit coupling drives the formation of anomalous quasiparticles with vanishing magnetic moment, providing the condensate significant immunity against magnetic fields beyond the Pauli paramagnetic limit. These results offer design opportunities for superconductors with extreme resilience against magnetic field.

Superconducting radio-frequency (SRF) resonators are critical components for particle accelerator applications, such as free-electron lasers, and for emerging technologies in quantum computing. Developing advanced materials and their deposition processes to produce RF superconductors that yield nanoohms surface resistances is a key metric for the wider adoption of SRF technology. Here we report ZrNb(CO) RF superconducting films with high critical temperatures (Tc) achieved for the first time under ambient pressure. The attainment of a Tc near the theoretical limit for this material without applied pressure is promising for its use in practical applications. A range of Tc, likely arising from Zr doping variation, may allow a tunable superconducting coherence length that lowers the sensitivity to material defects when an ultra-low surface resistance is required. Our ZrNb(CO) films are synthesized using a low-temperature (100 - 200 C) electrochemical recipe combined with thermal annealing. The phase transformation as a function of annealing temperature and time is optimized by the evaporated Zr-Nb diffusion couples. Through phase control, we avoid hexagonal Zr phases that are equilibrium-stable but degrade Tc. X-ray and electron diffraction combined with photoelectron spectroscopy reveal a system containing cubic ZrNb mixed with rocksalt NbC and low-dielectric-loss ZrO2. We demonstrate proof-of-concept RF performance of ZrNb(CO) on an SRF sample test system. BCS resistance trends lower than reference Nb, while quench fields occur at approximately 35 mT. Our results demonstrate the potential of ZrNb(CO) thin films for particle accelerator and other SRF applications.

Workbench-size particle accelerators, enabled by Nb3Sn-based superconducting radio-frequency (SRF) cavities, hold the potential of driving scientific discovery by offering a widely accessible and affordable source of high-energy electrons and X-rays. Thin-film Nb3Sn RF superconductors with high quality factors, high operation temperatures, and high-field potentials are critical for these devices. However, surface roughness, non-stoichiometry, and impurities in Nb3Sn deposited by conventional Sn-vapor diffusion prevent them from reaching their theoretical capabilities. Here we demonstrate a seed-free electrochemical synthesis that pushes the limit of chemical and physical properties in Nb3Sn. Utilization of electrochemical Sn pre-deposits reduces the roughness of converted Nb3Sn by five times compared to typical vapor-diffused Nb3Sn. Quantitative mappings using chemical and atomic probes confirm improved stoichiometry and minimized impurity concentrations in electrochemically synthesized Nb3Sn. We have successfully applied this Nb3Sn to the large-scale 1.3 GHz SRF cavity and demonstrated ultra-low BCS surface resistances at multiple operation temperatures, notably lower than vapor-diffused cavities. Our smooth, homogeneous, high-purity Nb3Sn provides the route toward high efficiency and high fields for SRF applications under helium-free cryogenic operations.

Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high quality KTaO3 thin films by molecular-beam epitaxy. Tantalum was provided by both a suboxide source emanating a TaO2 flux from Ta2O5 contained in a conventional effusion cell as well as an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10 \% O3 + 90 \% O2) were simultaneously supplied with the TaO$_2$ (or tantalum) molecular beams to grow the KTaO$_3$ films. Laue fringes suggest that the films are smooth with an abrupt film/substrate interface. Cross-sectional scanning transmission electron microscopy does not show any extended defects and confirms that the films have an atomically abrupt interface with the substrate. Atomic force microscopy reveals atomic steps at the surface of the grown films. Reciprocal space mapping demonstrates that the films, when sufficiently thin, are coherently strained to the SrTiO$_3$ (001) and GdScO$_3$ (110) substrates.

We complete measurements of interconversions among the full triad of thermal gradients, charge currents, and spin currents in the topological insulator Bi$_2$Se$_3$ by quantifying the efficiency with which thermal gradients can generate transverse spin currents. We accomplish this by comparing the spin Nernst magneto-thermopower to the spin Hall magnesistance for bilayers of Bi$_2$Se$_3$/CoFeB. We find that Bi$_2$Se$_3$ does generate substantial thermally-driven spin currents. A lower bound for the ratio of spin current to thermal gradient is $J_s/\nabla_x T$ = (4.9 $\pm$ 0.9) $\times$ 10$^{6}$ ($\hbar/2e$) A m$^{-2}$ / K $\mu$m$^{-1}$, and a lower bound for the magnitude of the spin Nernst ratio is $-$0.61 $\pm$ 0.11. The spin Nernst ratio for Bi$_2$Se$_3$ is the largest among all materials measured to date, 2-3 times larger compared to previous measurements for the heavy metals Pt and W.

Niobium-zirconium (Nb-Zr) alloy is an old superconductor that is a promising new candidate for superconducting radio-frequency (SRF) cavity applications. Using density-functional and Eliashberg theories, we show that addition of Zr to a Nb surface in small concentrations increases the critical temperature $T_c$ and improves other superconducting properties. Furthermore, we calculate $T_c$ for Nb-Zr alloys across a broad range of Zr concentrations, showing good agreement with the literature for disordered alloys as well as the potential for significantly higher $T_c$ in ordered alloys near 75%Nb/25%Zr composition. We provide experimental verification on Nb-Zr alloy samples and SRF sample test cavities prepared with either physical vapor or our novel electrochemical deposition recipes. These samples have the highest measured $T_c$ of any Nb-Zr superconductor to date and indicate a reduction in BCS resistance compared to the conventional Nb reference sample; they represent the first steps along a new pathway to greatly enhanced SRF performance. Finally, we use Ginzburg-Landau theory to show that the addition of Zr to a Nb surface increases the superheating field $B_{sh}$, a key figure of merit for SRF which determines the maximum accelerating gradient at which cavities can operate., Comment: 7 pages, 5 figures, submitted to Physical Review Letters

The demand for high-throughput electron tomography is rapidly increasing in biological and material sciences. However, this 3D imaging technique is computationally bottlenecked by alignment and reconstruction which runs from hours to days. We demonstrate real-time tomography with dynamic 3D tomographic visualization to enable rapid interpretation of specimen structure immediately as data is collected on an electron microscope. Using geometrically complex chiral nanoparticles, we show volumetric interpretation can begin in less than 10 minutes and a high quality tomogram is available within 30 minutes. Real time tomography is integrated into tomviz, an open source and cross platform 3D analysis tool that contains intuitive graphical user interfaces (GUI) to enable any scientist to characterize biological and material structure in 3D.

We demonstrate advantages of samples made by mechanical stacking of exfoliated van der Waals materials for controlling the topological surface state of a 3-dimensional topological insulator (TI) via interaction with an adjacent magnet layer. We assemble bilayers with pristine interfaces using exfoliated flakes of the TI BiSbTeSe2 and the magnet Cr2Ge2Te6, thereby avoiding problems caused by interdiffusion that can affect interfaces made by top-down deposition methods. The samples exhibit an anomalous Hall effect (AHE) with abrupt hysteretic switching. For the first time in samples composed of a TI and a separate ferromagnetic layer, we demonstrate that the amplitude of the AHE can be tuned via gate voltage with a strong peak near the Dirac point. This is the signature expected for the AHE due to Berry curvature associated with an exchange gap induced by interaction between the topological surface state and an out-of-plane-oriented magnet., Comment: submitted version

Efficient manipulation of antiferromagnetically coupled materials that are integration-friendly and have strong perpendicular magnetic anisotropy (PMA) is of great interest for low-power, fast, dense magnetic storage and computing. Here, we report a distinct, giant bulk damping-like spin-orbit torque in strong-PMA ferrimagnetic Fe100-xTbx single layers that are integration-friendly (composition-uniform, amorphous, sputter-deposited). For sufficiently-thick layers, this bulk torque is constant in the efficiency per unit layer thickness, {\xi}_DL^j/t, with a record-high value of 0.036nm-1, and the dampinglike torque efficiency {\xi}_DL^j achieves very large values for thick layers, up to 300% for 90 nm layers. This giant bulk torque by itself switches tens of nm thick Fe100-xTbx layers that have very strong PMA and high coercivity at current densities as low as a few MA/cm2. Surprisingly, for a given layer thickness, {\xi}_DL^j shows strong composition dependence and becomes negative for composition where the total angular momentum is oriented parallel to the magnetization rather than antiparallel. Our findings of giant bulk spin torque efficiency and intriguing torque-compensation correlation will stimulate study of such unique spin-orbit phenomena in a variety of ferrimagnetic hosts. This work paves a promising avenue for developing ultralow-power, fast, dense ferrimagnetic storage and computing devices., Comment: To appear in Applied Physics Reviews

The existence of long range magnetic order in low dimensional magnetic systems, such as the quasi-two-dimensional (2D) van der Waals (vdW) magnets, has attracted intensive studies of new physical phenomena. The vdW Fe$_N$GeTe$_2$ ($N$ = 3, 4, 5; FGT) family is exceptional owing to its vast tunability of magnetic properties. Particularly, a ferromagnetic ordering temperature ($T_{\text{C}}$) above room temperature at $N$ = 5 (F5GT) is observed. Here, our study shows that, by nickel (Ni) substitution of iron (Fe) in F5GT, a record high $T_{\text{C}}$ = 478(6) K is achieved. Importantly, pervasive, beyond-room-temperature ferromagnetism exists in almost the entire doping range of the phase diagram of Ni-F5GT. We argue that this striking observation in Ni-F5GT can be possibly due to several contributing factors, in which the structural alteration enhanced 3D magnetic couplings might be critical for enhancing the ferromagnetic order., Comment: Submitted on 06-Dec-2021; Now online

In condensed-matter systems, competition between ground states at phase boundaries can lead to significant changes in material properties under external stimuli, particularly when these ground states have different crystal symmetries. A key scientific and technological challenge is to stabilize and control coexistence of symmetry-distinct phases with external stimuli. Using BiFeO3 (BFO) layers confined between layers of the dielectric TbScO3 as a model system, we stabilize the mixed-phase coexistence of centrosymmetric and non-centrosymmetric BFO phases with antipolar, insulating and polar, semiconducting behavior, respectively at room temperature. Application of in-plane electric (polar) fields can both remove and introduce centrosymmetry from the system resulting in reversible, nonvolatile interconversion between the two phases. This interconversion between the centrosymmetric insulating and non-centrosymmetric semiconducting phases coincides with simultaneous changes in the non-linear optical response of over three orders of magnitude, a change in resistivity of over five orders of magnitude, and a change in the polar order. Our work establishes a materials platform allowing for novel cross-functional devices which take advantage of changes in optical, electrical, and ferroic responses., Comment: L Caretta and Y-T Shao contributed equally. 64 pages, 4 figures, 25 supplemental figures, 1 supplemental table

We observe a catalytic mechanism during the growth of III-O and IV-O materials by suboxide molecular-beam epitaxy ($S$-MBE). By supplying the molecular catalysts In$_2$O and SnO we increase the growth rates of Ga$_2$O$_3$ and In$_2$O$_3$. This catalytic action is explained by a metastable adlayer $A$, which increases the reaction probability of the reactants Ga$_2$O and In$_2$O with active atomic oxygen, leading to an increase of the growth rates of Ga$_2$O$_3$ and In$_2$O$_3$. We derive a model for the growth of binary III-O and IV-O materials by $S$-MBE and apply these findings to a generalized catalytic description for metal-oxide catalyzed epitaxy (MOCATAXY), applicable to elemental and molecular catalysts. We derive a mathematical description of $S$-MBE and MOCATAXY providing a computational framework to set growth parameters in previously inaccessible kinetic and thermodynamic growth regimes when using the aforementioned catalysis. Our results indicate MOCATAXY takes place with a suboxide catalyst rather than with an elemental catalyst. As a result of the growth regimes achieved, we demonstrate a Ga$_2$O$_3$/Al$_2$O$_3$ heterostructure with unrivaled crystalline quality, paving the way to the preparation of oxide device structures with unprecedented perfection.

Understanding lattice deformations is crucial in determining the properties of nanomaterials, which can become more prominent in future applications ranging from energy harvesting to electronic devices. However, it remains challenging to reveal unexpected deformations that crucially affect material properties across a large sample area. Here, we demonstrate a rapid and semi-automated unsupervised machine learning approach to uncover lattice deformations in materials. Our method utilizes divisive hierarchical clustering to automatically unveil multi-scale deformations in the entire sample flake from the diffraction data using four-dimensional scanning transmission electron microscopy (4D-STEM). Our approach overcomes the current barriers of large 4D data analysis and enables extraction of essential features even without a priori knowledge of the sample. Using this purely data-driven analysis, we have uncovered different types of material deformations, such as strain, lattice distortion, bending contour, etc., which can significantly impact the band structure and subsequent performance of nanomaterials-based devices. We envision that this data-driven procedure will provide insight into the intrinsic structures and accelerate the discovery of novel materials.

Precision and accuracy of quantitative scanning transmission electron microscopy (STEM) methods such as ptychography, and the mapping of electric, magnetic and strain fields depend on the dose. Reasonable acquisition time requires high beam current and the ability to quantitatively detect both large and minute changes in signal. A new hybrid pixel array detector (PAD), the second-generation Electron Microscope Pixel Array Detector (EMPAD-G2), addresses this challenge by advancing the technology of a previous generation PAD, the EMPAD. The EMPAD-G2 images continuously at a frame-rates up to 10 kHz with a dynamic range that spans from low-noise detection of single electrons to electron beam currents exceeding 180 pA per pixel, even at electron energies of 300 keV. The EMPAD-G2 enables rapid collection of high-quality STEM data that simultaneously contain full diffraction information from unsaturated bright field disks to usable Kikuchi bands and higher-order Laue zones. Test results from 80 to 300 keV are presented, as are first experimental results demonstrating ptychographic reconstructions, strain and polarization maps. We introduce a new information metric, the Maximum Usable Imaging Speed (MUIS), to identify when a detector becomes electron-starved, saturated or its pixel count is mismatched with the beam current.