arXiv subjects

Robert Hovden

Publications and source records attributed to Robert Hovden.

At least 55 records · Page 3Linked to original sources

arXiv2020

The Limits of Resolution and Dose for Aberration-Corrected Electron Tomography

Aberration-corrected electron microscopy can resolve the smallest atomic bond-lengths in nature. However, the high-convergence angles that enable spectacular resolution in 2D have unknown 3D resolution limits for all but the smallest objects ($< \sim$8nm). We show aberration-corrected electron tomography offers new limits for 3D imaging by measuring several focal planes at each specimen tilt. We present a theoretical foundation for aberration-corrected electron tomography by establishing analytic descriptions for resolution, sampling, object size, and dose---with direct analogy to the Crowther-Klug criterion. Remarkably, aberration-corrected scanning transmission electron tomography can measure complete 3D specimen structure of unbounded object sizes up to a specified cutoff resolution. This breaks the established Crowther limit when tilt increments are twice the convergence angle or smaller. Unprecedented 3D resolution is achievable across large objects. Atomic 3D imaging (1$\unicode{xC5}$) is allowed across extended objects larger than depth-of-focus (e.g. $>$ 20nm) using available microscopes and modest specimen tilting ($<$ 3$^\circ$). Furthermore, aberration-corrected tomography follows the rule of dose-fractionation where a specified total dose can be divided among tilts and defoci.

cond-mat.mtrl-sci↗

arXiv2020

Electron tomography for functional nanomaterials

Modern nanomaterials contain complexity that spans all three dimensions - from multigate semiconductors to clean energy nanocatalysts to complex block copolymers. For nanoscale characterization, it has been a long-standing goal to observe and quantify the three-dimensional (3D) structure - not just surfaces, but the entire internal volume and the chemical arrangement. Electron tomography estimates the complete 3D structure of nanomaterials from a series of two-dimensional projections taken across many viewing angles. Since its first introduction in 1968, electron tomography has progressed substantially in resolution, dose, and chemical sensitivity. In particular, scanning transmission electron microscope tomography has greatly enhanced the study of 3D nanomaterials by providing quantifiable internal morphology and spectroscopic detection of elements. Combined with recent innovations in computational reconstruction algorithms and 3D visualization tools, scientists can interactively dissect volumetric representations and extract meaningful statistics of specimens. This article highlights the maturing field of electron tomography and the widening scientific applications that utilize 3D structural, chemical, and functional imaging at the nanometer and subnanometer length scales.

physics.app-ph↗

arXiv2020

Imaging Polarity in Two Dimensional Materials by Breaking Friedel's Law

Friedel's law guarantees an inversion-symmetric diffraction pattern for thin, light materials where a kinematic approximation or a single-scattering model holds. Typically, breaking Friedel symmetry is ascribed to multiple scattering events within thick, non-centrosymmetric crystals. However, two-dimensional (2D) materials such as a single monolayer of MoS$_2$ can also violate Friedel's law, with unexpected contrast between conjugate Bragg peaks. We show analytically that retaining higher order terms in the power series expansion of the scattered wavefunction can describe the anomalous contrast between $hkl$ and $\overline{hkl}$ peaks that occurs in 2D crystals with broken in-plane inversion symmetry. These higher-order terms describe multiple scattering paths starting from the same atom in an atomically thin material. Furthermore, 2D materials containing heavy elements, such as WS$_2$, always act as strong phase objects, violating Friedel's law no matter how high the energy of the incident electron beam. Experimentally, this understanding can enhance diffraction-based techniques to provide rapid imaging of polarity, twin domains, in-plane rotations, or other polar textures in 2D materials.

cond-mat.mtrl-sci↗

arXiv2020

Dynamic Compressed Sensing for Real-Time Tomographic Reconstruction

Electron tomography has achieved higher resolution and quality at reduced doses with recent advances in compressed sensing. Compressed sensing (CS) theory exploits the inherent sparse signal structure to efficiently reconstruct three-dimensional (3D) volumes at the nanoscale from undersampled measurements. However, the process bottlenecks 3D reconstruction with computation times that run from hours to days. Here we demonstrate a framework for dynamic compressed sensing that produces a 3D specimen structure that updates in real-time as new specimen projections are collected. Researchers can begin interpreting 3D specimens as data is collected to facilitate high-throughput and interactive analysis. Using scanning transmission electron microscopy (STEM), we show that dynamic compressed sensing accelerates the convergence speed by 3-fold while also reducing its error by 27% for an Au/SrTiO3 nanoparticle specimen. Before a tomography experiment is completed, the 3D tomogram has interpretable structure within 33% of completion and fine details are visible as early as 66%. Upon completion of an experiment, a high-fidelity 3D visualization is produced without further delay. Additionally, reconstruction parameters that tune data fidelity can be manipulated throughout the computation without rerunning the entire process.

physics.comp-ph↗

arXiv2019

Nanoscale deformation mechanics reveal resilience in nacre of Pinna nobilis shell

The combination of soft nanoscale organic components with inorganic nanograins hierarchically designed by natural organisms results in highly ductile structural materials that can withstand mechanical impact and exhibit high resilience on the macro- and nano-scale. Our investigation of nacre deformation reveals the underlying nanomechanics that govern the structural resilience and absorption of mechanical energy. Using high-resolution scanning/transmission electron microscopy (S/TEM) combined with in situ indentation, we observe nanoscale recovery of heavily deformed nacre that restores its mechanical strength on external stimuli up to 80% of its yield strength. Under compression, nacre undergoes deformation of nanograins and non-destructive locking across organic interfaces such that adjacent inorganic tablets structurally join. The locked tablets respond to strain as a continuous material, yet the organic boundaries between them still restrict crack propagation. Remarkably, the completely locked interface recovers its original morphology without any noticeable deformation after compressive contact stresses as large as 1.2 GPa.

cond-mat.mtrl-sci↗

arXiv2019

Stacking, Strain, & Twist in 2D Materials Quantified by 3D Electron Diffraction

The field of two-dimensional (2D) materials has expanded to multilayered systems where electronic, optical, and mechanical properties change-often dramatically-with stacking order, thickness, twist, and interlayer spacing [1-5]. For transition metal dichalcogenides (TMDs), bond coordination within a single van der Waals layer changes the out-of-plane symmetry that can cause metal-insulator transitions [1, 6] or emergent quantum behavior [7]. Discerning these structural order parameters is often difficult using real-space measurements, however, we show 2D materials have distinct, conspicuous three-dimensional (3D) structure in reciprocal space described by near infinite oscillating Bragg rods. Combining electron diffraction and specimen tilt we probe Bragg rods in all three dimensions to identify multilayer structure with sub-Angstrom precision across several 2D materials-including TMDs (MoS2, TaSe2, TaS2) and multilayer graphene. We demonstrate quantitative determination of key structural parameters such as surface roughness, inter- & intra-layer spacings, stacking order, and interlayer twist using a rudimentary transmission electron microscope (TEM). We accurately characterize the full interlayer stacking order of multilayer graphene (1-, 2-, 6-, 12-layers) as well the intralayer structure of MoS2 and extract a chalcogen-chalcogen layer spacing of 3.07 +/- 0.11 Angstrom. Furthermore, we demonstrate quick identification of multilayer rhombohedral graphene.

cond-mat.mtrl-sci↗

arXiv2019

Sampling Limits for Electron Tomography with Sparsity-exploiting Reconstructions

Electron tomography (ET) has become a standard technique for 3D characterization of materials at the nano-scale. Traditional reconstruction algorithms such as weighted back projection suffer from disruptive artifacts with insufficient projections. Popularized by compressed sensing, sparsity-exploiting algorithms have been applied to experimental ET data and show promise for improving reconstruction quality or reducing the total beam dose applied to a specimen. Nevertheless, theoretical bounds for these methods have been less explored in the context of ET applications. Here, we perform numerical simulations to investigate performance of l_1-norm and total-variation (TV) minimization under various imaging conditions. From 36,100 different simulated structures, our results show specimens with more complex structures generally require more projections for exact reconstruction. However, once sufficient data is acquired, dividing the beam dose over more projections provides no improvements - analogous to the traditional dose-fraction theorem. Moreover, a limited tilt range of +-75 or less can result in distorting artifacts in sparsity-exploiting reconstructions. The influence of optimization parameters on reconstructions is also discussed.

cs.CV↗

arXiv2019

Removing Stripes, Scratches, and Curtaining with Non-Recoverable 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-to reliably restore images corrupted by stripe like features. Our approach removes beam instability, ion mill curtaining, mechanical scratches, or any stripe features and remains robust at low signal-to-noise. The success of this approach is achieved by exploiting compressed sensings inability to recover directional structures that are highly localized and missing in Fourier Space.

cs.CV↗

arXiv2018

Atomic and electronic reconstruction at van der Waals interface in twisted bilayer graphene

Control of the interlayer twist angle in two-dimensional (2D) van der Waals (vdW) heterostructures enables one to engineer a quasiperiodic moiré superlattice of tunable length scale. In twisted bilayer graphene (TBG), the simple moiré superlattice band description suggests that the electronic band width can be tuned to be comparable to the vdW interlayer interaction at a 'magic angle', exhibiting strongly correlated behavior. However, the vdW interlayer interaction can also cause significant structural reconstruction at the interface by favoring interlayer commensurability, which competes with the intralayer lattice distortion. Here we report the atomic scale reconstruction in TBG and its effect on the electronic structure. We find a gradual transition from incommensurate moiré structure to an array of commensurate domain structures as we decrease the twist angle across the characteristic crossover angle, $θ_c$ ~1°. In the twist regime smaller than $θ_c$ where the atomic and electronic reconstruction become significant, a simple moiré band description breaks down. Upon applying a transverse electric field, we observe electronic transport along the network of one-dimensional (1D) topological channels that surround the alternating triangular gapped domains, providing a new pathway to engineer the system with continuous tunability.

cond-mat.mtrl-sci↗

arXiv2017

Image registration of low signal-to-noise cryo-STEM data

Combining multiple fast image acquisitions to mitigate scan noise and drift artifacts has proven essential for picometer precision, quantitative analysis of atomic resolution scanning transmission electron microscopy (STEM) data. For very low signal-to-noise ratio (SNR) image stacks - frequently required for undistorted imaging at liquid nitrogen temperatures - image registration is particularly delicate, and standard approaches may either fail, or produce subtly specious reconstructed lattice images. We present an approach which effectively registers and averages image stacks which are challenging due to their low-SNR and propensity for unit cell misalignments. Registering all possible image pairs in a multi-image stack leads to significant information surplus. In combination with a simple physical picture of stage drift, this enables identification of incorrect image registrations, and determination of the optimal image shifts from the complete set of relative shifts. We demonstrate the effectiveness of our approach on experimental, cryogenic STEM datasets, highlighting subtle artifacts endemic to low-SNR lattice images and how they can be avoided. High-SNR average images with information transfer out to 0.72 A are achieved at 300 kV and with the sample cooled to near liquid nitrogen temperature.

eess.SP↗

arXiv2017

Commensurate Stripes and Phase Coherence in Manganites Revealed with Cryogenic Scanning Transmission Electron Microscopy

Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map at atomic resolution the nature of incommensurate order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature ($\sim$ 93K). In diffraction, the ordering wavevector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the underlying ordered state is lattice-commensurate at both temperatures. The cations undergo picometer-scale ($\sim $6-11 pm) transverse displacements, which suggests that charge-lattice coupling is strong and hence favors lattice-locked modulations. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93K. Such local phase variations not only govern the long range correlations of the charge-ordered state, but also results in apparent shifts in the ordering wavevector. These atomically-resolved observations underscore the importance of lattice coupling and provide a microscopic explanation for putative "incommensurate" order in hole-doped oxides.

cond-mat.str-el↗

arXiv2017

Bending and Breaking of Stripes in a Charge-Ordered Manganite

In complex electronic materials, coupling between electrons and the atomic lattice gives rise to remarkable phenomena, including colossal magnetoresistance and metal-insulator transitions. Charge-ordered phases are a prototypical manifestation of charge-lattice coupling, in which the atomic lattice undergoes periodic lattice displacements (PLDs). Here we directly map the picometer scale PLDs at individual atomic columns in the room temperature charge-ordered manganite Bi$_{0.35}$Sr$_{0.18}$Ca$_{0.47}$MnO$_3$ using aberration corrected scanning transmission electron microscopy (STEM). We measure transverse, displacive lattice modulations of the cations, distinct from existing manganite charge-order models. We reveal locally unidirectional striped PLD domains as small as $\sim$5 nm, despite apparent bidirectionality over larger length scales. Further, we observe a direct link between disorder in one lattice modulation, in the form of dislocations and shear deformations, and nascent order in the perpendicular modulation. By examining the defects and symmetries of PLDs near the charge-ordering phase transition, we directly visualize the local competition underpinning spatial heterogeneity in a complex oxide.

cond-mat.str-el↗

arXiv2016

Atomic Lattice Disorder in Charge Density Wave Phases of Exfoliated Dichalcogenides (1T-TaS2)

Charge density waves (CDW) and their concomitant periodic lattice distortions (PLD) govern the electronic properties in many layered transition-metal dichalcogenides. In particular, 1T-TaS2 undergoes a metal-to-insulator phase transition as the PLD becomes commensurate with the crystal lattice. Here we directly image PLDs of the nearly-commensurate (NC) and commensurate (C) phases in thin exfoliated 1T-TaS2 using atomic resolution scanning transmission electron microscopy at room and cryogenic temperature. At low temperatures, we observe commensurate PLD superstructures, suggesting ordering of the CDWs both in- and out-of-plane. In addition, we discover stacking transitions in the atomic lattice that occur via one bond length shifts. Interestingly, the NC PLDs exist inside both the stacking domains and their boundaries. Transitions in stacking order are expected to create fractional shifts in the CDW between layers and may be another route to manipulate electronic phases in layered dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2016

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 Co2P 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.

cond-mat.mes-hall↗

arXiv2015

Nanoscale assembly processes revealed in the nacroprismatic transition zone of Pinna nobilis mollusc shells

Intricate biomineralization processes in molluscs engineer hierarchical structures with meso-, nano-, and atomic architectures that give the final composite material exceptional mechanical strength and optical iridescence on the macroscale. This multiscale biological assembly inspires new synthetic routes to complex materials. Our investigation of the prism-nacre interface reveals nanoscale details governing the onset of nacre formation using high-resolution scanning transmission electron microscopy. A wedge polishing technique provides unprecedented, large-area specimens required to span the entire interface. Within this region, we find a transition from nanofibrillar aggregation to irregular early-nacre layers, to well-ordered mature nacre suggesting the assembly process is driven by aggregation of nanoparticles (~50-80 nm) within an organic matrix that arrange in fiber-like polycrystalline configurations. The particle number increases successively and, when critical packing is reached, they merge into early-nacre platelets. These results give new insights into nacre formation and particle-accretion mechanisms that may be common to many calcareous biominerals.

cond-mat.mtrl-sci↗

arXiv2014

Breaking the Crowther Limit: Combining Depth-Sectioning and Tilt Tomography for High-Resolution, Wide-Field 3D Reconstructions

To date, high-resolution (< 1 nm) imaging of extended objects in three-dimensions (3D) has not been possible. A restriction known as the Crowther criterion forces a tradeoff between object size and resolution for 3D reconstructions by tomography. Further, the sub-Angstrom resolution of aberration-corrected electron microscopes is accompanied by a greatly diminished depth of field, causing regions of larger specimens (> 6 nm) to appear blurred or missing. Here we demonstrate a three-dimensional imaging method that overcomes both these limits by combining through-focal depth sectioning and traditional tilt-series tomography to reconstruct extended objects, with high-resolution, in all three dimensions. The large convergence angle in aberration corrected instruments now becomes a benefit and not a hindrance to higher quality reconstructions. A through-focal reconstruction over a 390 nm 3D carbon support containing over one hundred dealloyed and nanoporous PtCu catalyst particles revealed with sub-nanometer detail the extensive and connected interior pore structure that is created by the dealloying instability.

cond-mat.mtrl-sci↗

arXiv2013

Strain Solitons and Topological Defects in Bilayer Graphene

Spontaneous symmetry-breaking, where the ground state of a system has lower symmetry than the underlying Hamiltonian, is ubiquitous in physics. It leads to multiply-degenerate ground states, each with a different "broken" symmetry labeled by an order parameter. The variation of this order parameter in space leads to soliton-like features at the boundaries of different broken-symmetry regions and also to topological point defects. Bilayer graphene is a fascinating realization of this physics, with an order parameter given by its interlayer stacking coordinate. Bilayer graphene has been a subject of intense study because in the presence of a perpendicular electric field, a band gap appears in its electronic spectrum [1-3] through a mechanism that is intimately tied to its broken symmetry. Theorists have further proposed that novel electronic states exist at the boundaries between broken-symmetry stacking domains [4-5]. However, very little is known about the structural properties of these boundaries. Here we use electron microscopy to measure with nanoscale and atomic resolution the widths, motion, and topological structure of soliton boundaries and topological defects in bilayer graphene. We find that each soliton consists of an atomic-scale registry shift between the two graphene layers occurring over 6-11 nm. We infer the minimal energy barrier to interlayer translation and observe soliton motion during in-situ heating above 1000 °C. The abundance of these structures across a variety samples, as well as their unusual properties, suggests that they will have substantial effects on the electronic and mechanical properties of bilayer graphene.

cond-mat.mes-hall↗

arXiv2013

Bibliometrics for Internet Media: Applying the h-Index to YouTube

The h-index can be a useful metric for evaluating a person's output of Internet media. Here we advocate and demonstrate adaption of the h-index and the g-index to the top video content creators on YouTube. The h-index for Internet video media is based on videos and their view counts. The index h is defined as the number of videos with >= h*10^5 views. The index g is defined as the number of videos with >= g*10^5 views on average. When compared to a video creator's total view count, the h-index and g-index better capture both productivity and impact in a single metric.

cs.DL↗