Engineering topics

Jesse, Stephen

Publications and source records attributed to Jesse, Stephen.

At least 163 records · Page 9

DOE OSTI2016

Phases and interfaces from real space atomically resolved data: Physics-based deep data image analysis

Advances in electron and scanning probe microscopies have led to a wealth of atomically resolved structural and electronic data, often with ~1–10 pm precision. However, knowledge generation from such data requires the development of a physics-based robust framework to link the observed structures to macroscopic chemical and physical descriptors, including single phase regions, order parameter fields, interfaces, and structural and topological defects. Here, we develop an approach based on a synergy of sliding window Fourier transform to capture the local analog of traditional structure factors combined with blind linear unmixing of the resultant 4D data set. This deep data analysis is ideally matched to the underlying physics of the problem and allows reconstruction of the a priori unknown structure factors of individual components and their spatial localization. We demonstrate the principles of this approach using a synthetic data set and further apply it for extracting chemical and physically relevant information from electron and scanning tunneling microscopy data. Furthermore, this method promises to dramatically speed up crystallographic analysis in atomically resolved data, paving the road toward automatic local structure–property determinations in crystalline and quasi-ordered systems, as well as systems with competing structural and electronic order parameters.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Full data acquisition in Kelvin Probe Force Microscopy: Mapping dynamic electric phenomena in real space

Kelvin probe force microscopy (KPFM) has provided deep insights into the role local electronic, ionic and electrochemical processes play on the global functionality of materials and devices, even down to the atomic scale. Conventional KPFM utilizes heterodyne detection and bias feedback to measure the contact potential difference (CPD) between tip and sample. This measurement paradigm, however, permits only partial recovery of the information encoded in bias- and time-dependent electrostatic interactions between the tip and sample and effectively down-samples the cantilever response to a single measurement of CPD per pixel. This level of detail is insufficient for electroactive materials, devices, or solid-liquid interfaces, where non-linear dielectrics are present or spurious electrostatic events are possible. Here, we simulate and experimentally validate a novel approach for spatially resolved KPFM capable of a full information transfer of the dynamic electric processes occurring between tip and sample. General acquisition mode, or G-Mode, adopts a big data approach utilising high speed detection, compression, and storage of the raw cantilever deflection signal in its entirety at high sampling rates (> 4 MHz), providing a permanent record of the tip trajectory. We develop a range of methodologies for analysing the resultant large multidimensional datasets involving classical, physics-based and information-based approaches. Physics-based analysis of G-Mode KPFM data recovers the parabolic bias dependence of the electrostatic force for each cycle of the excitation voltage, leading to a multidimensional dataset containing spatial and temporal dependence of the CPD and capacitance channels. We use multivariate statistical methods to reduce data volume and separate the complex multidimensional data sets into statistically significant components that can then be mapped onto separate physical mechanisms. Overall, G-Mode KPFM offers a new paradigm to study dynamic electric phenomena in electroactive interfaces as well as offer a promising approach to extend KPFM to solid-liquid interfaces.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

Direct-write liquid phase transformations with a scanning transmission electron microscope

The highly energetic electron beam from a scanning transmission electron microscope (STEM) can induce local changes in the state of matter, ranging from local knock-out and atomic movement, to amorphization/crystallization, and chemical/electrochemical reactions occuring at localized liquid-solid and gas-solid interfaces. To date, fundamental studies of e-beam induced phenomena and practical applications have been limited by conventional e-beam rastering modes that allow only for uniform e-beam exposures. Here we develop an automated liquid phase nanolithography method that is capable of directly writing nanometer scaled features within silicon nitride encapsulated liquid cells. An external beam control system, connected to the scan coils of an aberration-corrected STEM, is used to precisely control the position, dwell time, and scan velocity of a sub-nanometer STEM probe. Site-specific locations in a sealed liquid cell containing an aqueous solution of H 2 PdCl 4 are irradiated to controllably deposit palladium onto silicon nitride membranes. We determine the threshold electron dose required for the radiolytic deposition of metallic palladium, explore the influence of electron dose on the feature size and morphology of nanolithographically patterned nanostructures, and propose a feedback-controlled monitoring method for active control of the nanofabricated structures through STEM detector signal monitoring. As a result, this approach enables both fundamental studies of electron beam induced interactions with matter, as well as opens a pathway to fabricate nanostructures with tailored architectures and chemistries via shape-controlled nanolithographic patterning from liquid phase precursors.

43 PARTICLE ACCELERATORS↗

DOE OSTI2016

Nanoforging Single Layer MoSe 2 Through Defect Engineering with Focused Helium Ion Beams

Development of devices and structures based on the layered 2D materials critically hinges on the capability to induce, control, and tailor the electronic, transport, and optoelectronic properties via defect engineering, much like doping strategies have enabled semiconductor electronics and forging enabled introduction of iron age. Here, we demonstrate the use of a scanning helium ion microscope (HIM) for tailoring the functionality of single layer MoSe 2 locally, and decipher associated mechanisms at atomic level. We demonstrate He + beam bombardment that locally creates vacancies, shifts the Fermi energy landscape and thereby increases the Young s modulus of elasticity. Furthermore, we observe for the first time, an increase in the B-exciton photoluminescence signal from the nanoforged regions at room temperature. In conclusion, the approach for precise defect engineering demonstrated here opens opportunities for creating functional 2D optoelectronic devices with a wide range of customizable properties that include operating in the visible region.

42 ENGINEERING↗

DOE OSTI2016

Decoupling indirect topographic cross-talk in band excitation piezoresponse force microscopy imaging and spectroscopy

Here, all scanning probe microscopies are subjected to topographic cross-talk, meaning the topography-related contrast in functional images. Here, we investigate the signatures of indirect topographic cross-talk in piezoresponse force microscopy (PFM) imaging and spectroscopy and its decoupling using band excitation (BE) method in ferroelectric BaTiO 3 deposited on the Si substrates with free standing nanopillars of diameter 50 nm. Comparison between the single-frequency PFM and BE-PFM results shows that the measured signal can be significantly distorted by topography-induced shifts in the contact resonance frequency and cantilever transfer function. However, with proper correction, such shifts do not affect PFM imaging and hysteresis loop measurements. This suggests the necessity of an advanced approach, such as BE-PFM, for detection of intrinsic sample piezoresponse on the topographically non-uniform surfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Dynamic scan control in STEM: spiral scans

Abstract Scanning transmission electron microscopy (STEM) has emerged as one of the foremost techniques to analyze materials at atomic resolution. However, two practical difficulties inherent to STEM imaging are: radiation damage imparted by the electron beam, which can potentially damage or otherwise modify the specimen and slow-scan image acquisition, which limits the ability to capture dynamic changes at high temporal resolution. Furthermore, due in part to scan flyback corrections, typical raster scan methods result in an uneven distribution of dose across the scanned area. A method to allow extremely fast scanning with a uniform residence time would enable imaging at low electron doses, ameliorating radiation damage and at the same time permitting image acquisition at higher frame-rates while maintaining atomic resolution. The practical complication is that rastering the STEM probe at higher speeds causes significant image distortions. Non-square scan patterns provide a solution to this dilemma and can be tailored for low dose imaging conditions. Here, we develop a method for imaging with alternative scan patterns and investigate their performance at very high scan speeds. A general analysis for spiral scanning is presented here for the following spiral scan functions: Archimedean, Fermat, and constant linear velocity spirals, which were tested for STEM imaging. The quality of spiral scan STEM images is generally comparable with STEM images from conventional raster scans, and the dose uniformity can be improved.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

BEAM: A Computational Workflow System for Managing and Modeling Material Characterization Data in HPC Environments

Improvements in scientific instrumentation allow imaging at mesoscopic to atomic length scales, many spectroscopic modes, and now—with the rise of multimodal acquisition systems and the associated processing capability—the era of multidimensional, informationally dense data sets has arrived. Technical issues in these combinatorial scientific fields are exacerbated by computational challenges best summarized as a necessity for drastic improvement in the capability to transfer, store, and analyze large volumes of data. The Bellerophon Environment for Analysis of Materials (BEAM) platform provides material scientists the capability to directly leverage the integrated computational and analytical power of High Performance Computing (HPC) to perform scalable data analysis and simulation via an intuitive, cross-platform client user interface. This framework delivers authenticated, “push-button” execution of complex user workflows that deploy data analysis algorithms and computational simulations utilizing the converged compute-and-data infrastructure at Oak Ridge National Laboratory's (ORNL) Compute and Data Environment for Science (CADES) and HPC environments like Titan at the Oak Ridge Leadership Computing Facility (OLCF). In this work we address the underlying HPC needs for characterization in the material science community, elaborate how BEAM's design and infrastructure tackle those needs, and present a small sub-set of user cases where scientists utilized BEAM across a broad range of analytical techniques and analysis modes.

96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗

DOE OSTI2016

pyCroscopy

Suite of Python Libraries that implement structure data format processing, multivariate analysis, and interactive visualization of microscopy data and other spectral imaging modalities, including scanning probe microscopy, electron microscopy, Bragg diffraction microscopy, and chemical imaging.

Jesse, Stephen↗

DOE OSTI2016

Unraveling the Mechanism of Nanoscale Mechanical Reinforcement in Glassy Polymer Nanocomposites

The mechanical reinforcement of polymer nanocomposites (PNCs) above the glass transition temperature, T g , has been extensively researched. However, not much is known about the origin of this effect below T g . In this paper, we unravel the mechanism of PNC reinforcement within the glassy state by directly probing nanoscale mechanical properties with atomic force microscopy and macroscopic properties with Brillouin light scattering. Our results unambiguously show that the "glassy" Young's modulus in the interfacial polymer layer of PNCs is two-times higher than in the bulk polymer, which results in significant reinforcement below T g . We ascribe this phenomenon to a high stretching of the chains within the interfacial layer. Since the interfacial chain packing is essentially temperature independent, these findings provide a new insight into the mechanical reinforcement of PNCs also above T g .

36 MATERIALS SCIENCE↗

DOE OSTI2016

Directing Matter: Toward Atomic-Scale 3D Nanofabrication

Here we report that enabling memristive, neuromorphic, and quantum based computing as well as efficient mainstream energy storage and conversion technologies requires next generation of materials customized at the atomic scale. This requires full control of atomic arrangement and bonding in three dimensions. The last two decades witnessed substantial industrial, academic, and government research efforts directed towards this goal through various lithographies and scanning probe based methods. These technologies emphasize 2D surface structures, with some limited 3D capability. Recently, a range of focused electron and ion based methods have demonstrated compelling alternative pathways to achieving atomically precise manufacturing of 3D structures in solids, liquids, and at interfaces. Electron and ion microscopies offer a platform that can simultaneously observe dynamic and static structures at the nano and atomic scales, and also induce structural rearrangements and chemical transformation. The addition of predictive modeling or rapid image analytics and feedback enables guiding these in a controlled manner. Here, we review the recent results that used focused electron and ion beams to create free-standing nanoscale 3D structures, radiolysis and the fabrication potential with liquid precursors, epitaxial crystallization of amorphous oxides with atomic layer precision, as well as visualization and control of individual dopant motion within a 3D crystal lattice. These works lay the foundation for new approaches to directing nanoscale level architectures and offer a potential roadmap to full 3D atomic control in materials. Lastly, in this perspective we lay out the gaps that currently constrain the processing range of these platforms, reflect on indirect requirements, such as the integration of large scale data analysis with theory, and discuss future prospects of these technologies.

36 MATERIALS SCIENCE↗

DOE OSTI2016

G-mode magnetic force microscopy: Separating magnetic and electrostatic interactions using big data analytics

In this work, we develop a full information capture approach for Magnetic Force Microscopy (MFM), referred to as generalized mode (G-Mode) MFM. G-Mode MFM acquires and stores the full data stream from the photodetector, captured at sampling rates approaching the intrinsic photodiode limit. The data can be subsequently compressed, denoised, and analyzed, without information loss. Here, G-Mode MFM is implemented and compared to the traditional heterodyne-based MFM on model systems, including domain structures in ferromagnetic Yttrium Iron Garnet and the electronically and magnetically inhomogeneous high entropy alloy, CoFeMnNiSn. We investigate the use of information theory to mine the G-Mode MFM data and demonstrate its usefulness for extracting information which may be hidden in traditional MFM modes, including signatures of nonlinearities and mode-coupling phenomena. Finally, we demonstrate detection and separation of magnetic and electrostatic tip-sample interactions from a single G-Mode image, by analyzing the entire frequency response of the cantilever. G-Mode MFM is immediately implementable on any atomic force microscopy platform and as such is expected to be a useful technique for probing spatiotemporal cantilever dynamics and mapping material properties, as well as their mutual interactions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Correlation between piezoresponse nonlinearity and hysteresis in ferroelectric crystals at nanoscale

Here, the nonlinear response of a ferroic to external fields has been studied for decades, garnering interest for both understanding fundamental physics, as well as technological applications such as memory devices. Yet, the behavior of ferroelectrics at mesoscopic regimes remains poorly understood, and the scale limits of theories developed for macroscopic regimes are not well tested experimentally. Here, we test the link between piezo-nonlinearity and local piezoelectric strain hysteresis, via AC-field dependent measurements in conjunction with first order reversal curve (FORC) measurements on (K,Na)NbO 3 crystals with band-excitation piezoelectric force microscopy. The correlation coefficient between nonlinearity amplitude and the FORC of the polarization switching shows a clear decrease in correlation with increasing AC bias, suggesting the impact of domain wall clamping on the DC measurement case. Further, correlation of polynomial fitting terms from the nonlinear measurements with the hysteresis loop area reveals that the largest correlations are reserved for the quadratic terms, which is expected for irreversible domain wall motion contributions that impact both piezoelectric behavior as well as minor loop formation. These confirm the link between local piezoelectric nonlinearity, domain wall motion and minor loop formation, and suggest that existing theories (such as Preisach) are applicable at these length scales, with associated implications for future nanoscale devices.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Solid-state electrochemistry on the nanometer and atomic scales: the scanning probe microscopy approach

Energy technologies of the 21st century require an understanding and precise control over ion transport and electrochemistry at all length scales – from single atoms to macroscopic devices. Our short review provides a summary of recent studies dedicated to methods of advanced scanning probe microscopy for probing electrochemical transformations in solids at the meso-, nano- and atomic scales. In this discussion we present the advantages and limitations of several techniques and a wealth of examples highlighting peculiarities of nanoscale electrochemistry.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2016

The Center for Nanophase Materials Sciences

The Center for Nanophase Materials Sciences (CNMS) at Oak Ridge National Laboratory (ORNL) integrates nanoscale science with neutron science; synthesis science; and theory, modeling, and simulation. Operating as a national user facility, the CNMS supports a multidisciplinary environment for research to understand nanoscale materials and phenomena.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Polarization Control via He-Ion Beam Induced Nanofabrication in Layered Ferroelectric Semiconductors

Rapid advanced in nanoscience rely on continuous improvements of matter manipulation at near atomic scales. Currently, well characterized, robust, resist-based lithography carries the brunt of the nanofabrication process. However, use of local electron, ion and physical probe methods is also expanding, driven largely by their ability to fabricate without the multi-step preparation processes that can result in contamination from resists and solvents. Furthermore, probe based methods extend beyond nanofabrication to nanomanipulation and imaging, vital ingredients to rapid transition to prototyping and testing of layered 2D heterostructured devices. In this work we demonstrate that helium ion interaction, in a Helium Ion Microscope (HIM), with the surface of bulk copper indium thiophosphate CuM III P 2 X 6 (M = Cr, In; X= S, Se), (CITP) results in the control of ferroelectric domains, and growth of cylindrical nanostructures with enhanced conductivity; with material volumes scaling with the dosage of the beam. The nanostructures are oxygen rich, sulfur poor, and with the copper concentration virtually unchanged as confirmed by Energy Dispersive X-ray (EDX). Scanning Electron Microscopy (SEM) imaging contrast as well as Scanning Microwave Microscopy (SMM) measurements suggest enhanced conductivity in the formed particle, whereas Atomic Force Microscopy (AFM) measurements indicate that the produced structures have lower dissipation and a lower Young s modulus.

2D crystals↗

DOE OSTI2016

Graphene engineering by neon ion beams

Achieving the ultimate limits of materials and device performance necessitates the engineering of matter with atomic, molecular, and mesoscale fidelity. While common for organic and macromolecular chemistry, these capabilities are virtually absent for 2D materials. In contrast to the undesired effect of ion implantation from focused ion beam (FIB) lithography with gallium ions, and proximity effects in standard e-beam lithography techniques, the shorter mean free path and interaction volumes of helium and neon ions offer a new route for clean, resist free nanofabrication. Furthermore, with the advent of scanning helium ion microscopy, maskless He + and Ne + beam lithography of graphene based nanoelectronics is coming to the forefront. Here, we will discuss the use of energetic Ne ions in engineering graphene devices and explore the mechanical, electromechanical and chemical properties of the ion-milled devices using scanning probe microscopy (SPM). By using SPM-based techniques such as band excitation (BE) force modulation microscopy, Kelvin probe force microscopy (KPFM) and Raman spectroscopy, we demonstrate that the mechanical, electrical and optical properties of the exact same devices can be quantitatively extracted. Additionally, the effect of defects inherent in ion beam direct-write lithography, on the overall performance of the fabricated devices is elucidated.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Highly mobile ferroelastic domain walls in compositionally graded ferroelectric thin films

Domains and domain walls are critical in determining the response of ferroelectrics, and the ability to controllably create, annihilate, or move domains is essential to enable a range of next-generation devices. Whereas electric-field control has been demonstrated for ferroelectric 180° domain walls, similar control of ferroelastic domains has not been achieved. Here, using controlled composition and strain gradients, we demonstrate deterministic control of ferroelastic domains that are rendered highly mobile in a controlled and reversible manner. Through a combination of thin-film growth, transmission-electron-microscopy-based nanobeam diffraction and nanoscale band-excitation switching spectroscopy, we show that strain gradients in compositionally graded PbZr 1-x Ti x O 3 heterostructures stabilize needle-like ferroelastic domains that terminate inside the film. These needle-like domains are highly labile in the out-of-plane direction under applied electric fields, producing a locally enhanced piezoresponse. This work demonstrates the efficacy of novel modes of epitaxy in providing new modalities of domain engineering and potential for as-yet-unrealized nanoscale functional devices.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Multifrequency spectrum analysis using fully digital G Mode-Kelvin probe force microscopy

Since its inception over two decades ago, Kelvin probe force microscopy (KPFM) has become the standard technique for characterizing electrostatic, electrochemical and electronic properties at the nanoscale. In this work, we present a purely digital, software-based approach to KPFM utilizing big data acquisition and analysis methods. General Mode (G-Mode) KPFM, works by capturing the entire photodetector data stream, typically at the sampling rate limit, followed by subsequent de-noising, analysis and compression of the cantilever response. We demonstrate that the G-Mode approach allows simultaneous multi-harmonic detection, combined with on-the-fly transfer function correction required for quantitative CPD mapping. The KPFM approach outlined in this work significantly simplifies the technique by avoiding cumbersome instrumentation optimization steps (i.e. lock in parameters, feedback gains etc.), while also retaining the flexibility to be implemented on any atomic force microscopy platform. We demonstrate the added advantages of G-Mode KPFM by allowing simultaneous mapping of CPD and capacitance gradient (C') channels as well as increased flexibility in data exploration across frequency, time, space, and noise domains. As a result, G-Mode KPFM is particularly suitable for characterizing voltage sensitive materials or for operation in conductive electrolytes, and will be useful for probing electrodynamics in photovoltaics, liquids and ionic conductors.

36 MATERIALS SCIENCE↗