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Ophus, Colin

Publications and source records attributed to Ophus, Colin.

160 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Non-spectroscopic composition measurements of SrTiO 3 -La 0.7 Sr 0.3 MnO 3 multilayers using scanning convergent beam electron diffraction

The local atomic structure of a crystalline sample aligned along a zone axis can be probed with a focused electron probe, which produces a convergent beam electron diffraction pattern. The introduction of high speed direct electron detectors has allowed for experiments that can record a full diffraction pattern image at thousands of probe positions on a sample. By incoherently summing these patterns over crystalline unit cells, we demonstrate in this paper that in addition to crystal structure and thickness, we can also estimate the local composition of a perovskite superlattice sample. This is achieved by matching the summed patterns to a library of simulated diffraction patterns. Finally, this technique allows for atomic-scale chemical measurements without requiring a spectrometer or hardware aberration correction.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Deciphering chemical order/disorder and material properties at the single-atom level

Perfect crystals are rare in nature. Real materials often contain crystal defects and chemical order/disorder such as grain boundaries, dislocations, interfaces, surface reconstructions and point defects. Such disruption in periodicity strongly affects material properties and functionality. Despite rapid development of quantitative material characterization methods, correlating three-dimensional (3D) atomic arrangements of chemical order/disorder and crystal defects with material properties remains a challenge. On a parallel front, quantum mechanics calculations such as density functional theory (DFT) have progressed from the modelling of ideal bulk systems to modelling ‘real’ materials with dopants, dislocations, grain boundaries and interfaces; but these calculations rely heavily on average atomic models extracted from crystallography. To improve the predictive power of first-principles calculations, there is a pressing need to use atomic coordinates of real systems beyond average crystallographic measurements. Here we determine the 3D coordinates of 6,569 iron and 16,627 platinum atoms in an iron-platinum nanoparticle, and correlate chemical order/disorder and crystal defects with material properties at the single-atom level. We identify rich structural variety with unprecedented 3D detail including atomic composition, grain boundaries, anti-phase boundaries, anti-site point defects and swap defects. We show that the experimentally measured coordinates and chemical species with 22 picometre precision can be used as direct input for DFT calculations of material properties such as atomic spin and orbital magnetic moments and local magnetocrystalline anisotropy. The work presented here combines 3D atomic structure determination of crystal defects with DFT calculations, which is expected to advance our understanding of structure–property relationships at the fundamental level.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Optimizing disk registration algorithms for nanobeam electron diffraction strain mapping

Scanning nanobeam electron diffraction strain mapping is a technique by which the positions of diffracted disks sampled at the nanoscale over a crystalline sample can be used to reconstruct a strain map over a large area. However, it is important that the disk positions are measured accurately, as their positions relative to a reference are directly used to calculate strain. Here in this study, we compare several correlation methods using both simulated and experimental data in order to directly probe susceptibility to measurement error due to non-uniform diffracted disk illumination structure. We found that prefiltering the diffraction patterns with a Sobel filter before performing cross correlation or performing a square-root magnitude weighted phase correlation returned the best results when inner disk structure was present. Lastly, we have tested these methods both on simulated datasets, and experimental data from unstrained silicon as well as a twin grain boundary in 304 stainless steel.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Development of a fast framing detector for electron microscopy

A high frame rate detector system is described that enables fast real-time data analysis of scanning diffraction experiments in scanning transmission electron microscopy (STEM). This is an end-to-end development that encompasses the data producing detector, data transportation, and real-time processing of data. The detector will consist of a central pixel sensor that is surrounded by annular silicon diodes. Both components of the detector system will synchronously capture data at almost 100 kHz frame rate, which produces an approximately 400 Gb/s data stream. Low-level preprocessing will be implemented in firmware before the data is streamed from the National Center for Electron Microscopy (NCEM) to the National Energy Research Scientific Computing Center (NERSC). Live data processing, before it lands on disk, will happen on the Cori supercomputer and aims to present scientists with prompt experimental feedback. This online analysis will provide rough information of the sample that can be utilized for sample alignment, sample monitoring and verification that the experiment is set up correctly. Only a compressed version of the relevant data is then selected for more in-depth processing.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Enhanced phase contrast transfer using ptychography combined with a pre-specimen phase plate in a scanning transmission electron microscope

We report the ability to image light elements in both crystalline and noncrystalline materials at near atomic resolution with an enhanced contrast is highly advantageous to understand the structure and properties of a wide range of beam sensitive materials including biological specimens and molecular hetero-structures. This requires the imaging system to have an efficient phase contrast transfer at both low and high spatial frequencies. Here, we introduce a new phase contrast imaging method in a scanning transmission electron microscope (STEM) using a pre-specimen phase plate in the probe forming aperture, combined with a fast pixelated detector to record diffraction patterns at every probe position, and phase reconstruction using ptychography. The phase plate significantly enhances the contrast transfer of low spatial frequency information, and ptychography maximizes the extraction of the phase information at all spatial frequencies. In addition, the STEM probe with the presence of the phase plate retains its atomic resolution, allowing simultaneous incoherent Z-contrast imaging to be obtained along with the ptychographic phase image. An experimental image of Au nanoparticles on a carbon support shows high contrast for both materials. Multislice image simulations of a DNA molecule shows the capability of imaging soft matter at low dose conditions, which implies potential applications of low dose imaging of a wide range of beam sensitive materials.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), A n+1 B n O 3n+1 , thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Sr n+1 Ti n O 3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Nanomaterial datasets to advance tomography in scanning transmission electron microscopy

Electron tomography in materials science has flourished with the demand to characterize nanoscale materials in three dimensions (3D). Access to experimental data is vital for developing and validating reconstruction methods that improve resolution and reduce radiation dose requirements. This work presents five high-quality scanning transmission electron microscope (STEM) tomography datasets in order to address the critical need for open access data in this field. The datasets represent the current limits of experimental technique, are of high quality, and contain materials with structural complexity. Included are tomographic series of a hyperbranched Co 2 P nanocrystal, platinum nanoparticles on a carbon nanofibre imaged over the complete 180° tilt range, a platinum nanoparticle and a tungsten needle both imaged at atomic resolution by equal slope tomography, and a through-focal tilt series of PtCu nanoparticles. A volumetric reconstruction from every dataset is provided for comparison and development of post-processing and visualization techniques. Researchers interested in creating novel data processing and reconstruction algorithms will now have access to state of the art experimental test data.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Orientation mapping of semicrystalline polymers using scanning electron nanobeam diffraction

Here, we demonstrate a scanning electron nanobeam diffraction technique that can be used for mapping the size and distribution of nanoscale crystalline regions in a polymer blend. In addition, it can map the relative orientation of crystallites and the degree of crystallinity of the material. The model polymer blend is a 50:50 w/w mixture of semicrystalline poly(3-hexylthiophene-2,5-diyl) (P3HT) and amorphous polystyrene (PS). The technique uses a scanning electron beam to raster across the sample and acquires a diffraction image at each probe position. Through image alignment and filtering, the diffraction image dataset enables mapping of the crystalline regions within the scanned area and construction of an orientation map.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Efficient linear phase contrast in scanning transmission electron microscopy with matched illumination and detector interferometry

The ability to image light elements in soft matter at atomic resolution enables unprecedented insight into the structure and properties of molecular heterostructures and beam-sensitive nanomaterials. In this study, we introduce a scanning transmission electron microscopy technique combining a pre-specimen phase plate designed to produce a probe with structured phase with a high-speed direct electron detector to generate nearly linear contrast images with high efficiency. We demonstrate this method by using both experiment and simulation to simultaneously image the atomic-scale structure of weakly scattering amorphous carbon and strongly scattering gold nanoparticles. Our method demonstrates strong contrast for both materials, making it a promising candidate for structural determination of heterogeneous soft/hard matter samples even at low electron doses comparable to traditional phase-contrast transmission electron microscopy. Ultimately, simulated images demonstrate the extension of this technique to the challenging problem of structural determination of biological material at the surface of inorganic crystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2016

Identifying different stacking sequences in few-layer CVD-grown Mo S 2 by low-energy atomic-resolution scanning transmission electron microscopy

We present that atomically thin MoS 2 grown by chemical vapor deposition (CVD) is a promising candidate for next-generation electronics due to inherent CVD scalability and controllability. However, it is well known that the stacking sequence in few-layer MoS 2 can significantly impact electrical and optical properties. Herein we report different intrinsic stacking sequences in CVD-grown few-layer MoS 2 obtained by atomic-resolution annular-dark-field imaging in an aberration-corrected scanning transmission electron microscope operated at 50 keV. Trilayer MoS 2 displays a new stacking sequence distinct from the commonly observed 2H and 3R phases of MoS 2 . Finally, density functional theory is used to examine the stability of different stacking sequences, and the findings are consistent with our experimental observations.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Correcting nonlinear drift distortion of scanning probe and scanning transmission electron microscopies from image pairs with orthogonal scan directions

Unwanted motion of the probe with respect to the sample is a ubiquitous problem in scanning probe and scanning transmission electron microscopies, causing both linear and nonlinear artifacts in experimental images. We have designed a procedure to correct these artifacts by using orthogonal scan pairs to align each measurement line-by-line along the slow scan direction, by fitting contrast variation along the lines. We demonstrate the accuracy of our algorithm on both synthetic and experimental data and provide an implementation of our method.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Unravelling structural ambiguities in lithium- and manganese-rich transition metal oxides

Although Li- and Mn-rich transition metal oxides have been extensively studied as high-capacity cathode materials for Li-ion batteries, the crystal structure of these materials in their pristine state is not yet fully understood. Here we apply complementary electron microscopy and spectroscopy techniques at multi-length scale on well-formed Li1.2(Ni0.13Mn0.54Co0.13)O2 crystals with two different morphologies as well as two commercially available materials with similar compositions, and unambiguously describe the structural make-up of these samples. Systematically observing the entire primary particles along multiple zone axes reveals that they are consistently made up of a single phase, save for rare localized defects and a thin surface layer on certain crystallographic facets. Finally and more specifically, we show the bulk of the oxides can be described as an aperiodic crystal consisting of randomly stacked domains that correspond to three variants of monoclinic structure, while the surface is composed of a Co- and/or Ni-rich spinel with antisite defects.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Three-dimensional coordinates of individual atoms in materials revealed by electron tomography

Crystallography, the primary method for determining the 3D atomic positions in crystals, has been fundamental to the development of many fields of science. However, the atomic positions obtained from crystallography represent a global average of many unit cells in a crystal. In this paper, we report, for the first time, the determination of the 3D coordinates of thousands of individual atoms and a point defect in a material by electron tomography with a precision of ~19 pm, where the crystallinity of the material is not assumed. From the coordinates of these individual atoms, we measure the atomic displacement field and the full strain tensor with a 3D resolution of ~1 nm 3 and a precision of ~10 -3 , which are further verified by density functional theory calculations and molecular dynamics simulations. Finally, the ability to precisely localize the 3D coordinates of individual atoms in materials without assuming crystallinity is expected to find important applications in materials science, nanoscience, physics, chemistry and biology.

74 ATOMIC AND MOLECULAR PHYSICS↗