Feature extraction via similarity search: application to atom finding and denoising in electron and scanning probe microscopy imaging
Not Available
47 OTHER INSTRUMENTATION↗
Engineering topics
Jesse, Stephen
Publications and source records attributed to Jesse, Stephen.
Multi-purposed Ar gas cluster ion beam processing for graphene engineering
Graphene, with unique mechanical and electrical properties, offers diverse application opportunities from beyond Moore’s nano-electronics to water filtration. However, accomplishing these relies on cleaning and processing large areas of supported and suspended graphene sheets. Here in this paper, we demonstrate the use of an Ar cluster ion beam as a versatile tool for graphene cleaning, defect engineering, and nanopore fabrication. In-situ and ex-situ characterization techniques were utilized in combination with first principles molecular dynamics, to highlight the differences in processing of the supported and suspended graphene samples. In this work, we monitor interaction of the Ar cluster ion beam with graphene as a function of ion dose with in-situ secondary ion mass spectrometry (SIMS), as well as ex-situ Raman spectroscopy measurements. Scanning transmission electron microscopy (STEM) results confirm that the Ar cluster ion beam can form nanopores in the suspended graphene; while the basal plane of graphene remains intact maintaining the lattice structure. Finally, Scanning Electron Microscopy (SEM) image analysis of the irradiated samples allows quantitative tracking of pore areas and their distribution as a function of ion dose. This study highlights the flexibility of the Ar cluster ion beam in 2D material processing, and offers insights into Ar beam interaction with graphene.
36 MATERIALS SCIENCE↗
Deep Learning of Atomically Resolved Scanning Transmission Electron Microscopy Images: Chemical Identification and Tracking Local Transformations
Recent advances in scanning transmission electron and scanning probe microscopies have opened unprecedented opportunities in probing the materials structural parameters and various functional properties in real space with an angstrom-level precision. This progress has been accompanied by exponential increase in the size and quality of datasets produced by microscopic and spectroscopic experimental techniques. These developments necessitate adequate methods for extracting relevant physical and chemical information from the large datasets, for which a priori information on the structures of various atomic configurations and lattice defects is limited or absent. Here we demonstrate an application of deep neural networks to extracting information from atomically resolved images including location of the atomic species and type of defects. We develop a “weakly-supervised” approach that uses information on the coordinates of all atomic species in the image, extracted via a deep neural network, to identify a rich variety of defects that are not part of an initial training set. We further apply our approach to interpret complex atomic and defect transformation, including switching between different coordination of silicon dopants in graphene as a function of time, formation of peculiar silicon dimer with mixed 3-fold and 4-fold coordination, and the motion of molecular “rotor”. In conclusion, this deep learning based approach resembles logic of a human operator, but can be scaled leading to significant shift in the way of extracting and analyzing information from raw experimental data.
36 MATERIALS SCIENCE↗
Automated Interpretation and Extraction of Topographic Information from Time of Flight Secondary Ion Mass Spectrometry Data
Time of flight secondary ion mass spectrometry (ToF SIMS) is one of the most powerful characterization tools allowing imaging of the chemical properties of various systems and materials. It allows precise studies of the chemical composition with sub-100-nm lateral and nanometer depth spatial resolution. However, comprehensive interpretation of ToF SIMS results is challengeable, because of the data volume and its multidimensionality. Furthermore, investigation of the samples with pronounced topographical features are complicated by the spectral shift. In this work we developed approach for the comprehensive ToF SIMS data interpretation based on the data analytics and automated extraction of the sample topography based on time of flight shift. We further applied this approach to investigate correlation between biological function and chemical composition in Arabidopsis roots.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Mitigating e-beam-induced hydrocarbon deposition on graphene for atomic-scale scanning transmission electron microscopy studies
Chemical vapor deposition (CVD) grown graphene used in (scanning) transmission electron microscopy [(S)TEM] studies must undergo a careful transfer of the one-atom-thick membrane from the growth surface (typically a Cu foil) to the TEM grid. During this transfer process, the graphene invariably becomes contaminated with foreign materials. This contamination proves to be very problematic in the (S)TEM because often >95% of the graphene is obscured, and imaging of the pristine areas results in e-beam-induced hydrocarbon deposition which further acts to obscure the desired imaging area. In this article, the authors examine two cleaning techniques for CVD grown graphene that mitigate both aspects of the contamination problem: visible contamination covering the graphene, and “invisible” contamination that deposits onto the graphene under e-beam irradiation. Furthermore, the visible contamination may be removed quickly by a rapid thermal annealing to 1200 °C in situ and the invisible e-beam-deposited contamination may be removed through an Ar/O 2 annealing procedure prior to imaging in the (S)TEM.
36 MATERIALS SCIENCE↗
Chemical Changes in Layered Ferroelectric Semiconductors Induced by Helium Ion Beam
Transitioning to multi-material systems as either interfaced 2D materials or 3D heterostructures can lead to the next generation multi-functional device architectures. Combined direct physical and chemical nanoscale control of these systems offers a new way to tailor material and device functionality as functional structures reach their physical limit. Transition metal thiophosphate (TPS), Cu 1-x In 1+x/3 P 2 S 6 , that have ferroelectric polarization behavior as layered crystals at room temperature and above make them attractive candidates for direct material sculpting of both chemical and functional properties. The bulk material exhibits stable ferroelectric polarization corroborated by domain structures, rewritable polarization, and hysteresis loops. Our previous studies have demonstrated that ferroic order persists on the surface and that spinoidal decomposition of ferroelectric and paraelectric phases occurs in non-stoichiometric Cu/In ratio formulations. Here, we elucidate the chemical changes induced through helium ion irradiation in the TPS family library with varying Cu/In ratio formulations using correlated AFM and ToF-SIMS imaging. We correlate nano- and micro- structures that scale, in area and volume, to the total dose of the helium ion beam, as well as the overall copper concentration in the sample. Furthermore, our ToF-SIMS results show that ion irradiation leads to oxygen penetration as a function of Cu concentration, and proceeds along the Cu domains to the stopping distance of the helium ions in the TPS material. These results opens up new opportunities to understand and implement ferroicly coupled van der Waal devices into an existing framework of 2D heterostructures by locally tuning material chemistry and functionality.
36 MATERIALS SCIENCE↗
Metal/Ion Interactions Induced p–i–n Junction in Methylammonium Lead Triiodide Perovskite Single Crystals
Hybrid perovskites, as emerging multifunctional semiconductors, have demonstrated dual electronic/ionic conduction properties. Here, we report a metal/ion interaction induced p-i-n junction across slightly n-type doped MAPbI 3 single crystals with Au/MAPbI 3 /Ag configuration based on interface dependent Seebeck effect, Hall effect and time-of-flight secondary ion mass spectrometry analysis. The organic cations (MA + ) interact with Au atoms, forming positively charged coordination complexes at Au/MAPbI 3 interface, whereas iodine anions (I – ) can react with Ag contacts, leading to interfacial ionic polarization. Such metal/ion interactions establish a p-doped region near the Au/MAPbI 3 interface due to the formation of MA + vacancies, and an n-doped region near the Ag/MAPbI 3 interface due to formation of I – vacancies, consequently forming a p-i-n junction across the crystal in Au/MAPbI 3 /Ag configuration. Therefore, the metal/ion interaction plays a role in determining the surface electronic structure and semiconducting properties of hybrid perovskites.
36 MATERIALS SCIENCE↗
Direct Probing of Polarization Charge at Nanoscale Level
Ferroelectric materials possess spontaneous polarization that can be used for multiple applications. Owing to a long-term development of reducing the sizes of devices, the preparation of ferroelectric materials and devices is entering the nanometer-scale regime. In order to evaluate the ferroelectricity, there is a need to investigate the polarization charge at the nanoscale. Nonetheless, it is generally accepted that the detection of polarization charges using a conventional conductive atomic force microscopy (CAFM) without a top electrode is not feasible because the nanometer-scale radius of an atomic force microscopy (AFM) tip yields a very low signal-to-noise ratio. But, the detection is unrelated to the radius of an AFM tip and, in fact, a matter of the switched area. In this work, the direct probing of the polarization charge at the nanoscale is demonstrated using the positive-up-negative-down method based on the conventional CAFM approach without additional corrections or circuits to reduce the parasitic capacitance. The polarization charge densities of 73.7 and 119.0 µC cm -2 are successfully probed in ferroelectric nanocapacitors and thin films, respectively. The results we obtained show the feasibility of the evaluation of polarization charge at the nanoscale and provide a new guideline for evaluating the ferroelectricity at the nanoscale.
36 MATERIALS SCIENCE↗
Basic Energy Sciences Roundtable: Opportunities for Basic Research for Next-Generation Quantum Systems
For decades, scientists have predicted that devices based on “quantum phenomena” will be able to store and manipulate information to provide radical new approaches for computing, communication, and sensing. However, only recently have quantum phenomena been incorporated into technologies for next-generation computers, sensors, and detectors that demonstrate performance characteristics rivaling those of their conventional counterparts. These devices clearly demonstrate the enormous potential for future quantum-based technologies. The novel quantum device capabilities currently envisioned include enhanced resolution in imaging, sensors, and detectors; advanced cryptography for more secure communication; and significantly larger computational capabilities at speeds far greater than those possible in classical computing. However, realizing these advances requires a detailed understanding of how quantum systems (including quantum materials or assemblies of trapped ions and electrons) behave, accurate knowledge of how to integrate the components into complex systems, and precise control of the structures. In this context, creating and controlling quantum states within molecules and materials offer exciting scientific opportunities for fundamental research, as well as for enabling next-generation quantum-based technologies. Numerous questions remain, ranging from how quantum interactions may enable innovation through the creation of novel quantum systems, to how these new quantum technologies can advance our understanding of matter and chemistry at the most fundamental levels. To address these questions and identify priority research opportunities (PROs), the US Department of Energy (DOE) Office of Basic Energy Sciences (BES) convened a roundtable of experts in quantum materials and quantum systems encompassing the fields of physics, chemistry, materials synthesis science, device engineering, detector technology, and atomic-scale characterization techniques. This group of experimentalists and theorists met on October 30–31, 2017, to explore scientific research opportunities in this rapidly moving field, in which BES support can play a key role in advancing and utilizing quantum information science (QIS). The goals of this roundtable were to define the unique roles for BES in this active research field and to provide input on future research directions, forming the basis for a coordinated, long-term research effort that will enable major advances in quantum-based science and technology. BES is uniquely positioned to advance this field because of its long history of fundamental research support for both materials and chemical sciences, along with its construction and operation of world-class scientific user facilities. Fundamental research in this area is strongly coupled to DOE efforts in scientific computing, high-energy physics, and accelerator/detector research and related to activities in “Beyond Moore’s Law” computing, next-generation semiconductor materials, and exascale computing.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Placing single atoms in graphene with a scanning transmission electron microscope
We demonstrate that the sub-atomically focused beam of a scanning transmission electron microscope (STEM) can be used to controllably manipulate individual dopant atoms in a 2D graphene lattice. We demonstrate the manipulation of adsorbed source materials and the graphene lattice with the electron beam such that individual vacancy defects can be controllably passivated by Si substitutional atoms. We further demonstrate that these Si defects may be directed through the lattice via e-beam control or modified (as yet, uncontrollably) to form new defects which can incorporate new atoms into the graphene lattice. Furthermore, these studies demonstrate the potential of STEM for atom-by-atom nanofabrication and fundamental studies of chemical reactions in 2D materials on the atomic level.
36 MATERIALS SCIENCE↗
Breaking the Time Barrier in Kelvin Probe Force Microscopy: Fast Free Force Reconstruction Using the G-Mode Platform
The atomic force microscope (AFM) offers unparalleled insight into structure and material functionality across nanometer length scales. However, the spatial resolution afforded by the AFM tip is counterpoised by slow detection speeds compared to other common microscopy techniques (e.g. optical, scanning electron microscopy etc.). In this work, we develop an AFM imaging approach allowing ultrafast reconstruction of the tip-sample forces having ~2 orders of magnitude higher time resolution than standard detection methods. Fast free force recovery (F3R) overcomes the widely-viewed temporal bottleneck in AFM, i.e. the mechanical bandwidth of the cantilever, enabling time-resolved imaging at sub-bandwidth speeds. We demonstrate quantitative recovery of electrostatic forces with ~10 µs temporal resolution, free from cantilever ring-down effects. We further apply the F3R method to Kelvin probe force microscopy (KPFM) measurements. F3R-KPFM is an open loop imaging approach (i.e. no bias feedback), allowing ultrafast surface potential measurements (e.g. < 20 µs) to be performed at regular KPFM scan speeds. F3R-KPFM is demonstrated for exploration of ion migration in organometallic halide perovskites materials and shown to allow spatio-temporal imaging of positively charged ion migration under applied electric field, as well as subsequent formation of accumulated charges at the perovskite/electrode interface. In this work we demonstrate quantitative F3R-KPFM measurements – however, we fully expect the F3R approach to be valid for all modes of non-contact AFM operation, including non-invasive probing of ultrafast electrical and magnetic dynamics.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
G-mode - Full Information Capture Applied to Scanning Probe Microscopy
Explore the source record for details and available documents.
Somnath, Suhas↗
Pycroscopy - An Open Source Approach to Microscopy and Microanalysis in the Age of Big Data and Open Science
Explore the source record for details and available documents.
Somnath, Suhas↗
Three-State Ferroelastic Switching and Large Electromechanical Responses in PbTiO 3 Thin Films
Leveraging competition between energetically degenerate states to achieve large field-driven responses is a hallmark of functional materials, but routes to such competition are limited. Here, a new route to such effects involving domain-structure competition is demonstrated, which arises from straininduced spontaneous partitioning of PbTiO 3 thin films into nearly energetically degenerate, hierarchical domain architectures of coexisting c/a and a 1 /a 2 domain structures. Using band-excitation piezoresponse force microscopy, this study manipulates and acoustically detects a facile interconversion of different ferroelastic variants via a two-step, three-state ferroelastic switching process (out-of-plane polarized c+ → in-plane polarized a → out-of-plane polarized c- state), which is concomitant with large nonvolatile electromechanical strains (≈1.25%) and tunability of the local piezoresponse and elastic modulus (>23%). It is further demonstrated that deterministic, nonvolatile writing/erasure of large-area patterns of this electromechanical response is possible, thus showing a new pathway to improved function and properties.
36 MATERIALS SCIENCE↗
Multi-Modal Processing of Graphene Towards Precisely Controlled Fabrication of a Nanoelectronic Device Using the Helium Ion Microscope and the TOF SIMS
Explore the source record for details and available documents.
Kim, Songkil↗
Enhancing Ion Migration in Grain Boundaries of Hybrid Organic-Inorganic Perovskites by Chlorine
Ionicity plays an important role in determining material properties, as well as optoelectronic performance of organometallic trihalide perovskites (OTPs). Ion migration in OTP films has recently been under intensive investigation by various scanning probe microscopy (SPM) techniques. Controversial findings regarding the role of grain boundaries (GBs) associated with ion migration are often encountered, likely as a result of feedback errors and topographic effects common in to SPM. In this work, electron microscopy and spectroscopy (scanning transmission electron microscopy/electron energy loss spectroscopy) are combined with a novel, open-loop, band-excitation, (contact) Kelvin probe force microscopy (BE-KPFM and BE-cKPFM), in conjunction with ab initio molecular dynamics simulations to examine the ion behavior in the GBs of CH 3 NH 3 PbI 3 perovskite films. Furthermore, this combination of diverse techniques provides a deeper understanding of the differences between ion migration within GBs and interior grains in OTP films. Our work demonstrates that ion migration can be significantly enhanced by introducing additional mobile Cl - ions into GBs. The enhancement of ion migration may serve as the first step toward the development of high-performance electrically and optically tunable memristors and synaptic devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Mixed electrochemical–ferroelectric states in nanoscale ferroelectrics
Ferroelectricity on the nanoscale has been the subject of much fascination in condensed-matter physics for over half a century. In recent years, multiple reports claiming ferroelectricity in ultrathin ferroelectric films based on the formation of remnant polarization states, local electromechanical hysteresis loops, and pressure-induced switching were made. But, similar phenomena were reported for traditionally non-ferroelectric materials, creating a significant level of uncertainty in the field. We show that in nanoscale systems the ferroelectric state is fundamentally inseparable from the electrochemical state of the surface, leading to the emergence of a mixed electrochemical–ferroelectric state. We explore the nature, thermodynamics, and thickness evolution of such states, and demonstrate the experimental pathway to establish its presence. Our analysis reconciles multiple prior studies, provides guidelines for studies of ferroelectric materials on the nanoscale, and establishes the design paradigm for new generations of ferroelectric-based devices.
36 MATERIALS SCIENCE↗
Ferroelectric or non-ferroelectric: Why so many materials exhibit “ferroelectricity” on the nanoscale
Here, ferroelectric materials have remained one of the major focal points of condensed matter physics and materials science for over 50 years. In the last 20 years, the development of voltage-modulated scanning probe microscopy techniques, exemplified by Piezoresponse force microscopy (PFM) and associated time- and voltage spectroscopies, opened a pathway to explore these materials on a single-digit nanometer level. Consequently, domain structures and walls and polarization dynamics can now be imaged in real space. More generally, PFM has allowed studying electromechanical coupling in a broad variety of materials ranging from ionics to biological systems.
36 MATERIALS SCIENCE↗