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Increasing Spatial Fidelity and SNR of 4D-STEM using Multi-frame Data Fusion

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 Added by Lewys Jones
 Publication date 2021
  fields Physics
and research's language is English




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4D-STEM, in which the 2D diffraction plane is captured for each 2D scan position in the scanning transmission electron microscope (STEM) using a pixelated detector, is complementing and increasingly replacing existing imaging approaches. However, at present the speed of those detectors, although having drastically improved in the recent years, is still 100 to 1,000 times slower than the current PMT technology operators are used to. Regrettably, this means environmental scanning-distortion often limits the overall performance of the recorded 4D data. Here we present an extension of existing STEM distortion correction techniques for the treatment of 4D-data series. Although applicable to 4D-data in general, we use electron ptychography and electric-field mapping as model cases and demonstrate an improvement in spatial-fidelity, signal-to-noise ratio (SNR), phase-precision and spatial-resolution.

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The recent development of electron sensitive and pixelated detectors has attracted the use of four-dimensional scanning transmission electron microscopy (4D-STEM). Here, we present a precession electron diffraction assisted 4D-STEM technique for automated orientation mapping using diffraction spot patterns directly captured by an in-column scintillator based complementary metal-oxide-semiconductor (CMOS) detector. We compare the results to a conventional approach, which utilizes a fluorescent screen filmed by an external CCD camera. The high dynamic range and signal-to-noise characteristics of the detector largely improve the image quality of the diffraction patterns, especially the visibility of diffraction spots at high scattering angles. In the orientation maps reconstructed via the template matching process, the CMOS data yields a significant reduction of false indexing and higher reliability compared to the conventional approach. The angular resolution of misorientation measurement could also be improved by masking reflections close to the direct beam. This is because the orientation sensitive, weak and small diffraction spots at high scattering angle are more significant. The results show that fine details such as nanograins, nanotwins and sub-grain boundaries can be resolved with a sub-degree angular resolution which is comparable to orientation mapping using Kikuchi diffraction patterns.
Four dimensional scanning transmission electron microscopy (4D STEM) records the scattering of electrons in a material in great detail. The benefits offered by 4D STEM are substantial, with the wealth of data it provides facilitating for instance high precision, high electron dose efficiency phase imaging via center of mass or ptychography based analysis. However the requirement for a 2D image of the scattering to be recorded at each probe position has long placed a severe bottleneck on the speed at which 4D STEM can be performed. Recent advances in camera technology have greatly reduced this bottleneck, with the detection efficiency of direct electron detectors being especially well suited to the technique. However even the fastest frame driven pixelated detectors still significantly limit the scan speed which can be used in 4D STEM, making the resulting data susceptible to drift and hampering its use for low dose beam sensitive applications. Here we report the development of the use of an event driven Timepix3 direct electron camera that allows us to overcome this bottleneck and achieve 4D STEM dwell times down to 100~ns; orders of magnitude faster than what has been possible with frame based readout. We characterise the detector for different acceleration voltages and show that the method is especially well suited for low dose imaging and promises rich datasets without compromising dwell time when compared to conventional STEM imaging.
There is an increasing need to reconstruct objects in four or more dimensions corresponding to space, time and other independent parameters. The best 4D reconstruction algorithms use regularized iterative reconstruction approaches such as model based iterative reconstruction (MBIR), which depends critically on the quality of the prior modeling. Recently, Plug-and-Play methods have been shown to be an effective way to incorporate advanced prior models using state-of-the-art denoising algorithms designed to remove additive white Gaussian noise (AWGN). However, state-of-the-art denoising algorithms such as BM4D and deep convolutional neural networks (CNNs) are primarily available for 2D and sometimes 3D images. In particular, CNNs are difficult and computationally expensive to implement in four or more dimensions, and training may be impossible if there is no associated high-dimensional training data. In this paper, we present Multi-Slice Fusion, a novel algorithm for 4D and higher-dimensional reconstruction, based on the fusion of multiple low-dimensional denoisers. Our approach uses multi-agent consensus equilibrium (MACE), an extension of Plug-and-Play, as a framework for integrating the multiple lower-dimensional prior models. We apply our method to the problem of 4D cone-beam X-ray CT reconstruction for Non Destructive Evaluation (NDE) of moving parts. This is done by solving the MACE equations using lower-dimensional CNN denoisers implemented in parallel on a heterogeneous cluster. Results on experimental CT data demonstrate that Multi-Slice Fusion can substantially improve the quality of reconstructions relative to traditional 4D priors, while also being practical to implement and train.
105 - C. F. Majkrzak 2019
In the analysis of neutron scattering measurements of condensed matter structure, it normally suffices to treat the incident and scattered neutron beams as if composed of incoherent distributions of plane waves with wavevectors of different magnitudes and directions which are taken to define an instrumental resolution. However, despite the wide-ranging applicability of this conventional treatment, there are cases in which the wave function of an individual neutron in the beam must be described more accurately by a spatially localized packet, in particular with respect to its transverse extent normal to its mean direction of propagation. One such case involves the creation of orbital angular momentum (OAM) states in a neutron via interaction with a material device of a given size. It is shown in the work reported here that there exist two distinct measures of coherence of special significance and utility for describing neutron beams in scattering studies of materials in general. One measure corresponds to the coherent superposition of basis functions and their wavevectors which constitute each individual neutron packet state function whereas the other measure can be associated with an incoherent distribution of mean wavevectors of the individual neutron packets in a beam. Both the distribution of the mean wavevectors of individual packets in the beam as well as the wavevector components of the superposition of basis functions within an individual packet can contribute to the conventional notion of instrumental resolution. However, it is the transverse spatial extent of packet wavefronts alone that determines the area within which a coherent scattering process can occur in the first place. This picture is shown to be consistent with standard quantum theory. It is also demonstrated that these two measures of coherence can be distinguished from one another experimentally.
We present a detailed study of the spatial resolution of our time-resolved neutron imaging detector utilizing a new neutron position reconstruction method that improves both spatial resolution and event reconstruction efficiency. Our prototype detector system, employing a micro-pattern gaseous detector known as the micro-pixel chamber ({mu}PIC) coupled with a field-programmable-gate-array-based data acquisition system, combines 100{mu}m-level spatial and sub-{mu}s time resolutions with excellent gamma rejection and high data rates, making it well suited for applications in neutron radiography at high-intensity, pulsed neutron sources. From data taken at the Materials and Life Science Experimental Facility within the Japan Proton Accelerator Research Complex (J-PARC), the spatial resolution was found to be approximately Gaussian with a sigma of 103.48 +/- 0.77 {mu}m (after correcting for beam divergence). This is a significant improvement over that achievable with our previous reconstruction method (334 +/- 13 {mu}m), and compares well with conventional neutron imaging detectors and with other high-rate detectors currently under development. Further, a detector simulation indicates that a spatial resolution of less than 60 {mu}m may be possible with optimization of the gas characteristics and {mu}PIC structure. We also present an example of imaging combined with neutron resonance absorption spectroscopy.
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