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  1. Physics-based reward driven image analysis in microscopy

    The rise of electron microscopy has expanded our ability to acquire nanometer and atomically resolved images of complex materials. The resulting vast datasets are typically analyzed by human operators, an intrinsically challenging process due to the multiple possible analysis steps and the corresponding need to build and optimize complex analysis workflows. We present a methodology based on the concept of a Reward Function coupled with Bayesian Optimization, to optimize image analysis workflows dynamically. The Reward Function is engineered to closely align with the experimental objectives and broader context and is quantifiable upon completion of the analysis. Here, cross-section, high-angle annularmore » dark field (HAADF) images of ion-irradiated (Y, Dy)Ba2Cu3O7–δ thin-films were used as a model system. The reward functions were formed based on the expected materials density and atomic spacings and used to drive multi-objective optimization of the classical Laplacian-of-Gaussian (LoG) method. These results can be benchmarked against the DCNN segmentation. This optimized LoG* compares favorably against DCNN in the presence of the additional noise. We further extend the reward function approach towards the identification of partially-disordered regions, creating a physics-driven reward function and action space of high-dimensional clustering. We pose that with correct definition, the reward function approach allows real-time optimization of complex analysis workflows at much higher speeds and lower computational costs than classical DCNN-based inference, ensuring the attainment of results that are both precise and aligned with the human-defined objectives.« less
  2. Revealing unprecedented cathode interface behavior in all-solid-state batteries with oxychloride solid electrolytes

    The superionic conductor, lithium tantalum oxychloride (LTOC), exhibits unprecedented stability with Co-lean and Ni-rich cathodes, while lowering the working temperature proves effective in regulating the Co-rich cathode interface with LTOC.
  3. Using solenoid as multipurpose tool for measuring beam parameters

    Solenoids are frequently used for focusing low-energy beams. In this paper, we show how they can serve as multipurpose diagnostics tools to measure various beam parameters, including energy, emittance, the second moments of the transverse distribution, and the beam position and angle with respect to the solenoid’s axis. The energy measurement is based on rotation of the plane of the transverse motion, as opposed to generating dispersion with a dipole. Measurement of the beam trajectory with respect to the solenoid axis is done by analyzing the beam orbit downstream of the solenoid while varying its current. The second moments aremore » calculated by analyzing the beam image on a profile monitor while accounting for the beam rotation caused by the solenoid. We describe in detail the corresponding procedures and the experimental results of these measurements.« less
  4. 4D Imaging of ZnO-Coated Nanoporous Al2O3 Aerogels by Chemically Sensitive Ptychographic Tomography: Implications for Designer Catalysts

    The 3D chemical structure (4D spectromicroscopy) of nanoporous Al2O3 aerogels coated with ZnO by atomic layer deposition (ALD) was studied by multienergy scanning transmission X-ray microscopy. These materials are representative of a class of designer catalysts in which the nanoporous support is prepared separately from the active catalyst material, which is subsequently introduced by ALD, thereby allowing independent optimization of the morphology, chemistry, and spatial distribution of the support and catalyst. The samples studied were prepared by Ga ion and Xe plasma focused ion beam (FIB) milling as well as drop casting from water suspension. Zn L and Al Kmore » edge spectra of six samples with three different ZnO loadings were measured to investigate how loading and different sample preparation methods affect the 3D distribution of the ZnO and Al2O3. Scanning transmission X-ray microscopy (STXM) and ptychographic imaging at two energies each at the Zn L3 and Al K edge were measured. The ptychography data were analyzed by using the SHARP reconstruction code to generate quantitative 2D chemical maps of the Al2O3 and the ZnO. The STXM and ptychography maps were then measured at a sequence of tilt angles, covering up to 160° of rotation. The 3D structure of the ZnO and Al2O3 was derived from the tilt series data by tomographic reconstruction using a compressed sensing algorithm. A twodimensional spatial resolution (half-period) of 6 nm, measured by Fourier ring correlation, and a 3D spatial resolution (half-period) of 9 nm, measured by Fourier shell correlation, were achieved when using the COSMIC beamline at the Advanced Light Source (ALS). The results show that for all of the ZnO loadings studied there is nonuniform coverage of the ZnO on the Al2O3 aerogel framework. In addition, we found that both FIB methods create sample artifacts, although the distortion was less with Xe plasma than Ga ion FIB.« less
  5. Low-energy high-brightness electron beam dynamics based on slice beam matrix method

    Preserving the phase space quality has been of crucial importance to high-brightness electron beam transport. Any driving source of beam performance limitations in such a transport system must be carefully examined in order to preserve the beam phase space quality. It is found that in the low beam energy, high bunch charge regime, space charge effect on the charged particle beam evolution can be complicated. It may be insufficient to analyze the beam properties through the envelope or lower order moments for the mere bulk of the beam. In this work we will study the space-charge-dominated, low-energy, high-brightness electron beammore » dynamics based on the slice beam matrix method. The slice beam matrix method, extended from the existing bulk beam analysis, is applicable to an arbitrary longitudinal bunch distribution and can thus take the nonlinear RF curvature into account. The semi-analytical sliced beam space charge model is constructed and assumes an axisymmetric beam in the presence of perfect conducting cylindrical pipe with circular cross section. We present in this paper the theoretical formulation, starting from single-particle dynamics, space charge field calculation, followed by the moment description of a collection of particles, based on beam sigma matrix and longitudinal slice decomposition. We prove the equivalence between the beam matrix method and the envelope formalism in the presence of space charge effect, in both the transverse and longitudinal dimensions. Two examples are then demonstrated, one for a unit cell of superconducting radio-frequency (RF) cavity and the other for a 1.5-cell RF gun system. The semi-analytical results from beam matrix calculation are discussed and compared with particle tracking simulation using ASTRA. In conclusion, we expect that the analysis based on the slice beam matrix method shall serve as an efficient and advanced tool to further investigate the low-energy high-brightness electron beam dynamics.« less
  6. Removing Stripes, Scratches, and Curtaining with Nonrecoverable Compressed Sensing

    Highly-directional image artifacts such as ion mill curtaining, mechanical scratches, or image striping from beam instability degrade the interpretability of micrographs. These unwanted, aperiodic features extend the image along a primary direction and occupy a small wedge of information in Fourier space. Deleting this wedge of data replaces stripes, scratches, or curtaining, with more complex streaking and blurring artifacts—known within the tomography community as “missing wedge” artifacts. Here, we overcome this problem by recovering the missing region using total variation minimization, which leverages image sparsity-based reconstruction techniques—colloquially referred to as compressed sensing (CS)—to reliably restore images corrupted by stripe-like features.more » Our approach removes beam instability, ion mill curtaining, mechanical scratches, or any stripe features and remains robust at low signal-to-noise. In conclusion, the success of this approach is achieved by exploiting CS's inability to recover directional structures that are highly localized and missing in Fourier Space.« less
  7. Anomalous vibrational modes in few layer WTe2 revealed by polarized Raman scattering and first-principles calculations

    When layered transition-metal dichalcogenides (TMDs) are scaled down from a three- to a two-dimensional geometry, electronic and structural transitions occur, leading to the emergence of properties not usually found in the bulk. Here, we report a systematic Raman study of exfoliated semi-metallic WTe2 flakes with thickness ranging from few layers down to a single layer. A dramatic change in the Raman spectra occurs between the monolayer and few-layer WTe2 as a vibrational mode centered at ~86.9 cm-1 in the monolayer splits into two active modes at 82.9 and 89.6 cm-1 in the bilayer. Davydov splitting of these two modes ismore » found in the bilayer, as further evidenced by polarized Raman measurements. Strong angular dependence of Raman modes on the WTe2 film thickness reflects that the existence of directional interlayer interaction, rather than isotropic van der Waals (vdw) coupling, is playing an essential role affecting the phonon modes, especially in anisotropic 2D WTe2 material. Therefore, the strong evolution of Raman modes with thickness and polarization direction, can not only be a reliable fingerprint for the determination of the thickness and the crystallographic orientation, but can also be an ideal probe for such strong and directional interlayer interaction.« less
  8. Magnetic field-induced Fermi surface reconstruction and quantum criticality in CeRhIn5

    Here, we present detailed results of the field evolution of the de Haas–van Alphen (dHvA) effect in CeRhIn5. A magnetic field-induced reconstruction of the Fermi surface is clearly shown to occur inside the antiferromagnetic state, in an applied field of around B* ≃ 30 T, which is evidenced by the appearance of several new dHvA branches. The angular dependence of the dHvA frequencies reveals that the Fermi surfaces of CeRhIn5 at B > B* and CeCoIn5 are similar. The results suggest that the Ce-4f electrons in become itinerant at B > B* due to the Kondo effect, prior to themore » field-induced quantum critical point (QCP) at Bc0 ≃ 50 T. The electronic states at the field-induced QCP are therefore different from that of the pressure-induced QCP where a dramatic Fermi surface reconstruction occurs exactly at the critical pressure, indicating that multiple types of QCP may exist in CeRhIn5.« less

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"Yuan, Hui"

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