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All sources NASA NTRS DOE OSTI

DOE OSTI2021

Explaining an unusual electromigration behavior—A comprehensive experimental and theoretical analysis using finite element method

In metallic interconnects, it is generally assumed that electromigration (EM) failure location is independent of the applied electrical current and always occurs at the highest-current-density area. Our experiments show otherwise. We designed an Al interconnect that alters its failure location by only varying the applied current density. The failure occurs near the high for a current above 2 × 10 7 A/cm 2 , but at a location with 59% of the maximum for lower current densities. Thermoreflectance thermal imaging is employed to gather time-dependent high-resolution spatial temperature distributions of the Al interconnect during EM. More importantly, we propose a computationally inexpensive 2D finite element method that tracks EM evolution in time and matches well with the observations from different experimental conditions. A detailed analysis covering the major driving forces of EM is carried out to understand the complex physics behind EM. The atomic depletion rate contributed by each force is quantitatively studied. By examining the results from every tested experimental condition, the model reveals that the temperature gradient is the key reason causing atomic depletion near the failure location. Graphical illustrations and qualitative analysis are provided to intuitively show the key findings of our work.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Thermodynamic and Kinetic Transitions of Liquids in Nanoconfinement

Core principles of chemistry are ubiquitously invoked to shed light on the nature of molecular level interactions in nanoconfined fluids, which play a pivotal role in a wide range of processes in geochemistry, biology, and engineering. A detailed understanding of the physicochemical processes involved in the flow, structural transitions, and freezing or melting behavior of fluids confined within nanometer-sized pores of solid materials is thus of enormous importance for both basic research and technological applications. This Account provides a perspective on new insights into the thermodynamic and kinetic transitions of nanoconfined fluids in their stable and metastable forms. After briefly introducing the unique properties of mesoporous silicas from the SBA, MCM, and FDU families that serve as the confinement matrices, combining highly ordered single and bimodal mesopore architectures with tunable pore sizes in the ~2-15 nm range and narrow size distributions, recent studies on melting/freezing behavior of water confined in these host matrices are reviewed. While differential scanning calorimetry (DSC) reveals a linear relationship between melting point depression and pore size (independent of the pore shape), as predicted by the Gibbs-Thomson relation, variable temperature 2 H wide-line nuclear magnetic resonance (NMR) spectroscopy studies confirm the core-shell model of water and give evidence for a layer-by-layer freezing mechanism, which gives rise to an apparent fragile-to-strong transition in the solidification dynamics. In contrast to the freezing/melting behavior of water, the effect of nanoconfinement on the glass transition of supercooled liquids is nonuniversal and the glass transition temperature T g can either increase or decrease with the dimensionality and extent of confinement. This nonuniversal behavior is exemplified by the two glass-forming molecular liquids, glycerol and ortho-terphenyl (OTP). While glycerol shows an increase in T g and a pronounced slowdown of the rotational dynamics of the constituent molecules due to a change in the molecular packing between the bulk and the confined liquid, OTP displays a linear and confining-media-dependent depression of T g with increased confinement that is strongly influenced by the pore-liquid interface characteristics. This Account concludes with a focus on recent experimental evidence of extreme spatial and dynamical heterogeneity in both freezing and glass transition processes. This discovery was enabled by the unique mesoporous structures of SBA-16 and FDU-5, possessing bimodal architectures with two interconnected pore types of different size and shape (spherical and cylindrical). For the very first time, two melting points for water and two glass transitions for supercooled OTP, corresponding to a specific pore type, were observed. Collectively, these observations strongly suggest a close mechanistic connection between the local fluctuations in the structure and dynamics of nanoconfined liquids. Finally, while the findings reviewed in this Account provide new insights into thermodynamic and kinetic transitions of fluids, there remain many unanswered questions regarding the effects of nanoconfinement on the fundamental properties of fluids, which offer exciting future opportunities in chemical research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2010

Planar Submillimeter-Wave Mixer Technology with Integrated Antenna

High-performance mixers at terahertz frequencies require good matching between the coupling circuits such as antennas and local oscillators and the diode embedding impedance. With the availability of amplifiers at submillimeter wavelengths and the need to have multi-pixel imagers and cameras, planar mixer architecture is required to have an integrated system. An integrated mixer with planar antenna provides a compact and optimized design at terahertz frequencies. Moreover, it leads to a planar architecture that enables efficient interconnect with submillimeter-wave amplifiers. In this architecture, a planar slot antenna is designed on a thin gallium arsenide (GaAs) membrane in such a way that the beam on either side of the membrane is symmetric and has good beam profile with high coupling efficiency. A coplanar waveguide (CPW) coupled Schottky diode mixer is designed and integrated with the antenna. In this architecture, the local oscillator (LO) is coupled through one side of the antenna and the RF from the other side, without requiring any beam sp litters or diplexers. The intermediate frequency (IF) comes out on a 50-ohm CPW line at the edge of the mixer chip, which can be wire-bonded to external circuits. This unique terahertz mixer has an integrated single planar antenna for coupling both the radio frequency (RF) input and LO injection without any diplexer or beamsplitters. The design utilizes novel planar slot antenna architecture on a 3- mthick GaAs membrane. This work is required to enable future multi-pixel terahertz receivers for astrophysics missions, and lightweight and compact receivers for planetary missions to the outer planets in our solar system. Also, this technology can be used in tera hertz radar imaging applications as well as for testing of quantum cascade lasers (QCLs).

Chattopadhyay, Gautam↗

DOE OSTI2024

Neutrons in Structural Biology: Challenges and Opportunities (Workshop Report)

Gaining a thorough understanding of biological systems requires building our knowledge about biological processes from the level of atoms and electrons, and up to whole organisms. Such comprehensive knowledge will allow for a predictive understanding of complex biological systems behavior. It will guide us in the design and development of novel therapeutics and vaccines to tackle existing health threats and to prepare for future pandemics, and it will provide information necessary to create new biomaterials and bio-inspired technologies through manipulation of biological macromolecules, their assemblies, single cells and even microorganisms. Reaching these goals will require a synergistic combination of multiple experimental techniques with molecular calculations and predictive simulations, and the design and development of new techniques and capabilities that bridge current knowledge and technology gaps. Neutron scattering provides unique information about the biomacromolecular structure and function and can play a major role in achieving these goals. A workshop was held to engage the scientific community in identifying pressing challenges in biochemistry, structural biology, enzymology and structure-guided drug design not solved with the current neutron scattering technologies or utilizing other structural biology techniques such as X-ray crystallography, NMR, and cryo-EM. The workshop brought together structural biology, biochemistry and computational experts, as well as early career researchers and students, creating a forum for discussing scientific advancement and collaboration. The workshop included a one-day satellite training workshop where graduate students and postdoctoral researchers were educated in the application of neutron crystallography and small-angle scattering in structural biology. Furthermore, the Instrument Scientific Advisory Board (ISAB) for the development of a macromolecular neutron diffractometer at ORNL’s Second Target Station was introduced at the workshop. The major outcome was that neutrons can provide atomic-level understanding of biomacromolecular structure, function and dynamics which is of paramount importance for addressing the identified challenges. Neutron crystallography, in particular, can resolve long-standing biochemical issues regarding enzyme function by delineating the underlying chemistry and can have a major impact on the design of small-molecule therapeutics, especially in combination with molecular computation (quantum chemistry and molecular dynamics simulations) and the emerging artificial intelligence (AI)-assisted drug design technologies. The unique properties of neutrons, including their high sensitivity to hydrogen and their non-destructive nature, make them ideal probes of biological matter. There is a palpable need in the scientific community to expand and enhance the impact of neutron sciences on biology. Neutron crystallography is the only structural biology method capable of determining positions of all hydrogen atoms in proteins, nucleic acids and their complexes at near-physiological temperatures and of unstable species at cryogenic temperatures. Moreover, neutron analysis is non-ionizing, non-destructive and does not perturb the structure or redox chemistry of active site metal centers and clusters in proteins, which can be invaluable for studying radiation-sensitive metalloprotein complexes. Further, neutron energies used in scattering applications are similar to atomic motions, permitting neutron spectroscopies to characterize the dynamics of biomacromolecules on the picosecond to microsecond timescales. The different sensitivities of neutrons to protium (H) and deuterium (D) isotopes of hydrogen allow enhanced visibility of specific parts of biological complexes through isotopic labeling. The impact of neutrons will be most powerful when neutron scattering is combined with complementary experimental techniques that use photons and electrons, and with high-performance computing. The interconnection and mutuality of the experimental and theoretical capabilities will drive discoveries in biological and health sciences to generate more complete picture of complex biological systems. The major limitation in the field of biological neutron crystallography has been signal-to-noise, demanding large samples that are difficult to produce for the majority of biomacromolecules and limiting the applicability of this technique in biological sciences. A neutron crystallography instrument at the Second Target Station will revolutionize biological science with neutrons by engaging a large scientific community of structural biologists, enabling successful neutron diffraction experiments from radically smaller biomacromolecular crystals, resolving unanswered biochemical questions, and meaningfully contributing to rational drug design. The meeting highlighted 10 grand challenges that will be addressed with this advanced capability over the next decade and beyond, and the recommendations required to help address them are given below.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Oxide-Free Three-Dimensional Germanium/Silicon Core–Shell Metalattice Made by High-Pressure Confined Chemical Vapor Deposition

Metalattices are crystalline arrays of uniform particles in which the period of the crystal is close to some characteristic physical length scale of the material. In this work, we explore the synthesis and properties of a germanium metalattice in which the similar to 70 nm periodicity of a silica colloidal crystal template is close to the similar to 24 nm Bohr exciton radius of the nanocrystalline Ge replica. The problem of Ge surface oxidation can be significant when exploring quantum confinement effects or designing electronically coupled nanostructures because of the high surface area to volume ratio at the nanoscale. To eliminate surface oxidation, we developed a coreshell synthesis in which the Ge metalattice is protected by an oxide-free Si interfacial layer, and we explore its properties by transmission electron microscopy (TEM), Raman spectroscopy, and electron energy loss spectroscopy (EELS). The interstices of a colloidal crystal film grown from 69 nm diameter spherical silica particles were filled with polycrystalline Ge by high-pressure confined chemical vapor deposition (HPcCVD) from GeH4. After the SiO2 template was etched away with aqueous HF, the Ge replica was uniformly coated with an amorphous Si shell by HPcCVD as confirmed by TEM-EDS (energy-dispersive X-ray spectroscopy) and Raman spectroscopy. Formation of the shell prevents oxidation of the Ge core within the detection limit of XPS. The electronic properties of the core-shell structure were studied by accessing the Ge 3d edge onset using STEM-EELS. A blue shift in the edge onset with decreasing size of Ge sites in the metalattices suggests quantum confinement of the Ge core. The degree of quantum confinement of the Ge core depends on the void sizes in the template, which is tunable by using silica particles of varying size. The edge onset also shows a shift to higher energy near the shell in comparison with the Ge core. This shift along with the observation of Ge-Si vibrational modes in the Raman spectrum indicate interdiffusion of Ge and Si. Both the size of the voids in the template and core-shell interdiffusion of Si and Ge can in principle be tuned to modify the electronic properties of the Ge metalattice.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2011

Miniaturized Airborne Imaging Central Server System

In recent years, some remote-sensing applications require advanced airborne multi-sensor systems to provide high performance reflective and emissive spectral imaging measurement rapidly over large areas. The key or unique problem of characteristics is associated with a black box back-end system that operates a suite of cutting-edge imaging sensors to collect simultaneously the high throughput reflective and emissive spectral imaging data with precision georeference. This back-end system needs to be portable, easy-to-use, and reliable with advanced onboard processing. The innovation of the black box backend is a miniaturized airborne imaging central server system (MAICSS). MAICSS integrates a complex embedded system of systems with dedicated power and signal electronic circuits inside to serve a suite of configurable cutting-edge electro- optical (EO), long-wave infrared (LWIR), and medium-wave infrared (MWIR) cameras, a hyperspectral imaging scanner, and a GPS and inertial measurement unit (IMU) for atmospheric and surface remote sensing. Its compatible sensor packages include NASA s 1,024 1,024 pixel LWIR quantum well infrared photodetector (QWIP) imager; a 60.5 megapixel BuckEye EO camera; and a fast (e.g. 200+ scanlines/s) and wide swath-width (e.g., 1,920+ pixels) CCD/InGaAs imager-based visible/near infrared reflectance (VNIR) and shortwave infrared (SWIR) imaging spectrometer. MAICSS records continuous precision georeferenced and time-tagged multisensor throughputs to mass storage devices at a high aggregate rate, typically 60 MB/s for its LWIR/EO payload. MAICSS is a complete stand-alone imaging server instrument with an easy-to-use software package for either autonomous data collection or interactive airborne operation. Advanced multisensor data acquisition and onboard processing software features have been implemented for MAICSS. With the onboard processing for real time image development, correction, histogram-equalization, compression, georeference, and data organization, fast aerial imaging applications, including the real time LWIR image mosaic for Google Earth, have been realized for NASA fs LWIR QWIP instrument. MAICSS is a significant improvement and miniaturization of current multisensor technologies. Structurally, it has a complete modular and solid-state design. Without rotating hard drives and other moving parts, it is operational at high altitudes and survivable in high-vibration environments. It is assembled from a suite of miniaturized, precision-machined, standardized, and stackable interchangeable embedded instrument modules. These stackable modules can be bolted together with the interconnection wires inside for the maximal simplicity and portability. Multiple modules are electronically interconnected as stacked. Alternatively, these dedicated modules can be flexibly distributed to fit the space constraints of a flying vehicle. As a flexibly configurable system, MAICSS can be tailored to interface a variety of multisensor packages. For example, with a 1,024x1,024 pixel LWIR and a 8,984x6,732 pixel EO payload, the complete MAICSS volume is approximately 7x9x11 in. (=18x23x28 cm), with a weight of 25 lb (=11.4 kg).

Sun, Xiuhong↗

DOE OSTI2021

Propagation of atmospheric pressure plasmas through interconnected pores in dielectric materials

We report the propagation of atmospheric pressure plasmas (APPs) on and through porous dielectric materials is being investigated for plasma-catalysis and functionalizing biomedical materials for tissue scaffolding and bone regeneration. Such plasma functionalization improves wettability and cell attachment, and so uniformity of the treatment of the pore surfaces is important. The method of propagation of APPs through porous media is not well characterized. In this paper, we discuss results from a computational investigation of humid air APPs propagating through short fully interconnected pore-chains in a dielectric substrate. The properties of the dielectric and pores (diameter 150 μm) were chosen to resemble bone scaffolding. We found that photoionization is an important feature in plasma propagation through pore-chains to seed electrons in the following pore in the chain. This seeding of electrons in regions of high electric field allows for the formation of micro-streamers and surface ionization waves. This is particularly important when the openings between pores are small. The orientation of the pore-chain with respect to the applied electric field has a significant impact on plasma generation, mode of propagation, and fluences of short-lived, reactive species to the surfaces of the pores. The uniformity of fluences of charged and short-lived neutral species to the pore surfaces decreases as the angle of the pore chain deviates from being aligned with the applied electric field. Diffusion within pores

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Using Dissipative Particle Dynamics to Model Effects of Chemical Reactions Occurring within Hydrogels

Computational models that reveal the structural response of polymer gels to changing, dissolved reactive chemical species would provide useful information about dynamically evolving environments. However, it remains challenging to devise one computational approach that can capture all the interconnected chemical events and responsive structural changes involved in this multi-stage, multi-component process. Here, we augment the dissipative particle dynamics (DPD) method to simulate the reaction of a gel with diffusing, dissolved chemicals to form kinetically stable complexes, which in turn cause concentration-dependent deformation of the gel. Using this model, we also examine how the addition of new chemical stimuli and subsequent reactions cause the gel to exhibit additional concentration-dependent structural changes. Through these DPD simulations, we show that the gel forms multiple latent states (not just the “on/off”) that indicate changes in the chemical composition of the fluidic environment. Hence, the gel can actuate a range of motion within the system, not just movements corresponding to the equilibrated swollen or collapsed states. Moreover, the system can be used as a sensor, since the structure of the layer effectively indicates the presence of chemical stimuli.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Perspectives of active Si photonics devices for data communication and optical sensing

Si photonics has made rapid progress in research and commercialization in the past two decades. While it started with electronic–photonic integration on Si to overcome the interconnect bottleneck in data communications, Si photonics has now greatly expanded into optical sensing, light detection and ranging (LiDAR), optical computing, and microwave/RF photonics applications. From an applied physics point of view, this perspective discusses novel materials and integration schemes of active Si photonics devices for a broad range of applications in data communications, spectrally extended complementary metal–oxide–semiconductor (CMOS) image sensing, as well as 3D imaging for LiDAR systems. We also present a brief outlook of future synergy between Si photonic integrated circuits and Si CMOS image sensors toward ultrahigh capacity optical I/O, ultrafast imaging systems, and ultrahigh sensitivity lab-on-chip molecular biosensing.

electronic band structure↗

DOE OSTI2022

Multiphysics simulation of microscale copper printing by confined electrodeposition using a nozzle array

3D printing of metals at the microscale and nanoscale is crucial to produce high-density interconnects and intricate structures in electronic devices. Conventional melting and sintering processes are not suitable for these scales due to a reliance on individual metal particles in the size range of tens of micrometers. Confined electrodeposition (CED) is an established alternative to conventional metal 3D printing processes in which an electrolyte is used to selectively induce deposition of the metal on the printing surface. However, commercialization and efficiency of this process have been limited due to a reliance on sub-micrometer nozzles to achieve desirable deposition rates and single nozzle to achieve uniformity of printed structures. Here, we address these challenges by computationally analyzing an array of microscale nozzles. We tailor the convection within the electrolyte to alter both deposition rate and geometric uniformity of the printed structures. The results show that for large nozzles the evaporation alone is not sufficient to obtain high deposition rates, yet an external pressure can be used to increase deposition and alter uniformity (thickness) of printed structures. Our results can be used to design and analyze new experiments toward parallel multi-nozzle deposition using CED toward high-throughput metal printing.

3D printing↗

DOE OSTI2022

Room Temperature Lasing from Semiconducting Single-Walled Carbon Nanotubes

Miniaturized near-infrared semiconductor lasers that are able to generate coherent light with low energy consumption have widespread applications in fields such as optical interconnects, neuromorphic computing, and deep-tissue optogenetics. With optical transitions at near-infrared wavelengths, diameter-tunable electronic structures, and superlative optoelectronic properties, semiconducting single-walled carbon nanotubes (SWCNTs) are promising candidates for nanolaser applications. However, despite significant efforts in this direction and recent progress toward enhancing spontaneous emission from SWCNTs through Purcell effects, SWCNT-based excitonic lasers have not yet been demonstrated. Leveraging an optimized cavity-emitter integration scheme enabled by a self-assembly process, here we couple SWCNT emission to the whispering gallery modes supported by polymer microspheres, resulting in room temperature excitonic lasing with an average lasing threshold of 4.5 kW/cm 2 . The high photostability of SWCNTs allows stable lasing for prolonged duration with minimal degradation. Finally, this experimental realization of excitonic lasing from SWCNTs, combined with their versatile electronic and optical properties that can be further controlled by chemical modification, offers far-reaching opportunities for tunable near-infrared nanolasers that are applicable for optical signal processing, in vivo biosensing, and optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Physics Division Strategic Plan Fiscal Years 2020-2024

The vision of the Physics Division (PHY) at Argonne National Laboratory is to continue enhancing its role as a world-leading institution in basic nuclear physics research and its applications. Key to this vision is for PHY to continue to safely and effectively operate and evolve the capabilities of the Argonne Tandem Linac Accelerator System (ATLAS) facility to best serve its users. ATLAS is the Department of Energy (DOE) accelerator facility for low-energy nuclear physics research. The research carried out by PHY covers many themes in contemporary science but can be distilled into five areas of focus. These themes are interconnected, with continuously evolving synergies between the various groups and facilities in PHY and the broader Laboratory. This five-year strategic plan serves to illustrate our current capabilities and new directions related to these five areas of focus (ATLAS also develops an independent strategic plan): Accelerator research and design. The goal of this theme is to design, fabricate, test, and implement novel accelerator systems, with a focus on high-intensity ion and electron systems. These R&D activities have led to enhancements in the ATLAS accelerator system. Among others, the division’s accelerator systems are in use or planned for use at Fermilab, the Advanced Photon Source, and in a broad variety of applications at the Facility for Rare Isotope Beams (FRIB). Atom trapping and fundamental symmetries. The goal of this theme is to explore and exploit the uses of advanced laser cooling and trapping techniques to manipulate atoms. There are three main areas of focus. First is in the application of the atom trap trace analysis (ATTA) technique for age determination of groundwater and ice by using radio-krypton dating. The next two trapping-based programs involve tests of fundamental symmetries in nature: the cooling and trapping of radium-225 with the aim of determining limits on an observation of its electric dipole moment and precision measurements of the beta decay properties of helium-6 to set limits on the tensor coupling constant. This is complemented by measurements of similar properties in lithium-8 and boron-8. Nuclear astrophysics. The goal of this theme is to enhance our understanding of how elements are created in the universe via explosive nucleosynthesis and how stars evolve. To meet the challenges of this theme, many of the capabilities of ATLAS are being enhanced, including the development of new beams through a new in-flight separator (RAISOR) and the anticipated neutron-generator upgrade of the Californium Rare Isotope Breeder Upgrade facility (nuCARIBU). These are coupled to state-of-the-art instruments such as the Canadian Penning Trap, Helical Orbit Spectrometer, Gammasphere, GRETINA, Multi-Sampling Ionization Chamber, the Fragment Mass Analyzer, and Argonne Gas-filled Fragment Analyzer, and a new low-background experimental area for decay studies. Nuclear structure. The goal of this theme is to understand the structure of nuclei, both stable and radioactive, in terms of single-particle properties, their shapes, and the dynamics governing reactions between them. These include questions such as what are the limits of nuclear stability and what are the properties of super heavy nuclei. As with the nuclear astrophysics theme, the capabilities of ATLAS, guided by the ATLAS user community, are continuously being enhanced to this end. The Division has strategic initiatives to play a leading role in the development of instrumentation and research programs at the FRIB. Quantum chromodynamics (QCD) and hadron physics. The goal of this theme is to lead major research programs focused on revealing the quark and gluon structure of protons, neutrons, nuclei, and short-lived mesons and baryons. These involve major programs at Jefferson Lab, Fermilab, and smaller facilities. They are complemented by theoretical endeavors centered on the question of how hadrons and their properties emerge from QCD. Out of these activities arise strategic initiatives to play a major role in the forthcoming Electron-Ion Collider (EIC).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Suppression of neutral-pion production in deep-inelastic scattering off nuclei with the CLAS detector

We present the first threefold differential measurement for neutral-pion multiplicity ratios produced in semi-inclusive deep-inelastic electron scattering on carbon, iron, and lead nuclei normalized to deuterium from CLAS at Jefferson Lab. We found that the neutral-pion multiplicity ratio is maximally suppressed for the leading hadrons (energy fraction 𝑧 → 1), suppression varying from 25% in carbon up to 75% in lead. An enhancement of the multiplicity ratio at low 𝑧 and high 𝑝$^2_𝑇$ is observed, suggesting an interconnection between these two variables. This behavior is qualitatively similar to the previous twofold differential measurement of charged pions by the HERMES Collaboration and, recently, by CLAS Collaboration. The largest enhancement was observed at high 𝑝$^2_𝑇$ for heavier nuclei, namely, iron and lead, while the smallest enhancement was observed for the lightest nucleus, carbon. This behavior suggests a competition between partonic multiple scattering, which causes enhancement, and hadronic inelastic scattering, which causes suppression.

color confinement↗