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At least 667 records · Page 37

An extended trajectory-mechanics approach for calculating two-phase flow paths

A technique originating in quantum dynamics is used to derive a trajectory-based, semi-analytical solution for two-phase flow. The partial differential equation governing the evolution of the aqueous phase is equivalent to a family of ordinary differential equations defined along a path through the porous medium. The trajectories may be found by solving the differential equations directly or by post-processing the output of a numerical solution to the full set of governing equations. The trajectories, which differ from conventional streamlines, are found to bend downward in response to gravitational forces. The curvature is more pronounced as the dip of the porous layer containing the flow increases. Subtle changes in the relative permeability curve can lead to significant variations in the trajectories. The ordinary differential equation for the trajectory provides an expression for the travel time along the path. The expression produces a semi-analytical approximation to the model parameter sensitivities, the partial derivatives of the travel times with respect to changes in the permeability model. The semi-analytical trajectory-based sensitivities generally agree with those computed using a numerical reservoir simulator and a perturbation approach. The sensitivities are useful in tomographic imaging algorithms designed to estimate the spatial variation in permeability within a porous medium using multiphase observations.

58 GEOSCIENCES↗

Functional Imaging of Hybrid Nanostructures: Visualization of Mechanisms for Solar Energy Utilization

The report describes advances in understanding the interaction of light with hybrid nanostructured materials, and the influence of physical and electronic structure on the flow of excess energetic charge carriers to support the design and optimization of new materials for photoelectrical and photoelectrochemical energy conversion. Raman scattering, multi-wavelength optical excitation, and numerical modeling are combined with electrical transport measurements on model hybrid materials structures and devices to resolve, in energy and space, the absorption of light, the generation of excess energetic charge carriers, and the efficiency of their separation to generate electrical and chemical energy. Appropriate combinations of spatially-resolved, time-resolved, and spectrally-resolved measurements are used to isolate and quantify various steps in the energy conversion process, including geometrically and plasmonically enhanced absorption, the generation of carriers with excess energy, and the efficiency with which the carriers can move to and perform useful chemistry at interfaces.

14 SOLAR ENERGY↗

Optical detection of spin Hall effect in metals

Optical techniques have been widely used to probe the spin Hall effect in semiconductors. In metals, however, only electrical methods such as nonlocal spin valve transport, ferromagnetic resonance, or spin torque transfer experiments have been successful. These methods require complex processing techniques and measuring setups. We show here that the spin Hall effect can be observed in non-magnetic metals such as Pt and β-W, using a standard bench top magneto-optical Kerr system with very little sample preparation. Applying a square wave current and using Fourier analysis significantly improve our detection level. One can readily determine the angular dependence of the induced polarization on the bias current direction (very difficult to do with voltage detection), the orientation of the spin Hall induced polarization, and the sign of the spin Hall angle. This optical approach is free from the complications of various resistive effects, which can compromise voltage measurements. This opens up the study of spin Hall effect in metals to a variety of spin dynamic and spatial imaging experiments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dielectric resonator method for determining gap symmetry of superconductors through anisotropic nonlinear Meissner effect

We present a new measurement method which can be used to image the gap nodal structure of superconductors whose pairing symmetry is under debate. This technique utilizes a high quality factor microwave resonance involving the sample of interest. While supporting a circularly symmetric standing wave current pattern, the sample is perturbed by a scanned laser beam, creating a photoresponse that was previously shown to reveal the superconducting gap anisotropy. Simulation and the measurement of the photoresponse of an unpatterned Nb film show less than 8% anisotropy, as expected for a superconductor with a nearly isotropic energy gap along with expected systematic uncertainty. On the other hand, measurement of a YBa 2 Cu 3 O 7- δ thin film shows a clear 4-fold symmetric image with ~12.5% anisotropy, indicating the well-known 4-fold symmetric d x 2 - y 2 gap nodal structure in the ab -plane. The deduced gap nodal structure can be further cross-checked by low temperature surface impedance data, which are simultaneously measured. The important advantage of the presented method over the previous spiral resonator method is that it does not require a complicated lithographic patterning process which limits one from testing various kinds of materials due to photoresponse arising from patterning defects. This advantage of the presented technique, and the ability to measure unpatterned samples such as planar thin films and single crystals, enables one to survey the pairing symmetry of a wide variety of unconventional superconductors.

47 OTHER INSTRUMENTATION↗

Facile and high spatial resolution ratio-metric luminescence thermal mapping in microfluidics by near infrared excited upconversion nanoparticles

A local area temperature monitor is important for precise control of chemical and biological processes in microfluidics. In this work, we developed a facile method to realize micron spatial resolution of temperature mapping in a microfluidic channel quickly and cost effectively. Based on the temperature dependent fluorescence emission of NaYF{sub 4}:Yb{sup 3+}, Er{sup 3+} upconversion nanoparticles (UCNPs) under near-infrared irradiation, ratio-metric imaging of UCNPs doped polydimethylsiloxane can map detailed temperature distribution in the channel. Unlike some reported strategies that utilize temperature sensitive organic dye (such as Rhodamine) to achieve thermal sensing, our method is highly chemically inert and physically stable without any performance degradation in long term operation. Moreover, this method can be easily scaled up or down, since the spatial and temperature resolution is determined by an optical imaging system. Our method supplied a simple and efficient solution for temperature mapping on a heterogeneous surface where usage of an infrared thermal camera was limited.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Thin-Entrance Window Process for Soft X-Ray Sensors

New free electron lasers, such as SLAC’s LCLS-II, will provide unique scientific imaging opportunities. In order to fully utilize these facilities, we need to develop detectors with shallow entrance windows that will enable detection of soft x-rays from 250 eV to 1.5 KeV. Achieving adequately shallow entrance windows is challenging because the high temperature anneal needed to activate the dopant also drives the dopant profile deeper, growing the region that is insensitive to soft x-rays. A new microwave annealing technology provides an efficient way to achieve shallow entrance windows in fully depleted high-resistivity silicon sensors. The microwave anneal technique can activate dopants at low substrate temperature, with minimal dopant diffusion, and can be used to fabricate both n-type and p-type entrance windows. SRP and SIMS measurements were used to verify dopant activation with negligible dopant diffusion. We then applied the microwave anneal process to a planar sensor wafer, using the new process to create the backside diode contact. Electrical test of the resulting sensors shows good reverse bias characteristics. The sensors have been bump-bonded to a read-out ASIC and used successfully to measure an Fe-55 x-ray spectrum. Process and device simulations were performed to characterize the quantum efficiency of the entrance window for soft x-rays. This technique is useful for other sensor applications requiring a shallow entrance window, including detectors for UV photons, low energy ions and low energy electrons.

47 OTHER INSTRUMENTATION↗

Two-phase accurate multiplexed structured image capture (2pAc-MUSIC)

Multiplexed Structural Image Capture (MUSIC) technique uses modulation of light from a scene prior to imaging to encode the temporal evolution of target into spatial frequency shifts, with each shift corresponding to a unique time and resulting in individual distinct snapshots. Computational-processing of the multiplexed single-shot image can recover the nanosecond-resolution scene evolution. One of the limitations is the loss of spatial resolution of the recovered image due to limitations of the low-pass spatial frequency filtering depth. Here we demonstrated that two images with complementary spatial phases can be used to enhance the spatial resolutions. For this application, 2 Phase Accurate (2pAc)-MUSIC is implemented that a scene is encoded with two complementary phases. The increased spatial information captured reduces the lower frequency noise in the Fourier domain found in single-phase MUSIC. A recovery algorithm combines the 180-degree spatial frequency shifted images into a single scene and applies a spatial filter in the Fourier domain that has a larger depth than previously possible to achieve a scene with increased spatial resolution. The 2pAc-MUSIC can effectively enhance the spatial resolution by removing the overlapping zero-order spatial frequencies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Resolution enhancement in nonlinear photoacoustic imaging

Nonlinear processes can be exploited to gain access to more information than is possible in the linear regime. Nonlinearity modifies the spectra of the excitation signals through harmonic generation, frequency mixing, and spectral shifting, so that features originally outside the detector range can be detected. Here, we present an experimental study of resolution enhancement for photoacoustic imaging of thin metal layers immersed in water. In this case, there is a threshold in the excitation below which no acoustic signal is detected. Above threshold, the nonlinearity reduces the width of the active area of the excitation beam, resulting in a narrower absorption region and thus improved spatial resolution. This gain is limited only by noise, as the active area of the excitation can be arbitrarily reduced when the fluence becomes closer to the threshold. Here, we demonstrate a two-fold improvement in resolution and quantify the image quality as the excitation fluence goes through threshold.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spectrum-per-Pixel Cathodoluminescence Imaging of CdTe Thin-Film Bevels

We conduct T=6 K cathodoluminescence (CL) spectrum imaging with a nano-scale electron beam on beveled surfaces of CdTe thin-films at different critical stages of standard CdTe device fabrication. The through-thickness total CL intensity profiles are consistent with a reduction in grain boundary recombination due to the CdCl2 treatment. Color-coded maps of the low-temperature luminescence transition energies reveal that CdTe thin films have remarkably non-uniform opto-electronic properties, which depend strongly on sample processing history. The grain-to-grain S content in the interdiffused CdTe/CdS region is estimated from a sample size of thirty-five grains, and the S content in adjacent grains varies significantly in CdCl2-treated samples. A low-temperature luminescence model is developed to interpret spectral behavior at grain boundaries and grain interiors.

14 SOLAR ENERGY↗

Backscattering of Relativistic Electrons Incident on a Planar Foil at a Small Angle to Its Surface

Photographs of cross sections of an electron beam backscattered from a thin tungsten target have been obtained on a dosimetric film. The procession of images makes it possible to obtain the spatial distribution of backscattered particles. The angles of back reflection θ{sub br} of electron beams from foils have been measured. A 7.4-MeV microtron has been used as a source of electrons. The experiments have been performed with a tungsten foil 386 mg/cm{sup 2} (200 μm) thick and a tantalum foil 1328 mg/cm{sup 2} (800 μm) thick. Particles have been injected at an angle of α = 10° to the foil surface. The Monte Carlo simulation of the scattering of relativistic electrons incident on a planar target at small angles to its surface has been performed. The spatial and energy distributions of backscattered particle fluxes both transmitted through the target and reflected from it have been calculated. The dependences of fluxes on the direction of injection of particles and on the material and thickness of the target have been considered.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Non-resonant Nanoscale Extreme Light Confinement

A wide spectrum of photonics activities Sandia is engaged in such as solid state lighting, photovoltaics, infrared imaging and sensing, quantum sources, rely on nanoscale or ultrasubwavelength light-matter interactions (LMI). The fundamental understanding in confining electromagnetic power and enhancing electric fields into ever smaller volumes is key to creating next generation devices for these programs. The prevailing view is that a resonant interaction (e.g. in microcavities or surface-plasmon polaritions) is necessary to achieve the necessary light confinement for absorption or emission enhancement. Here we propose new paradigm that is non-resonant and therefore broadband and can achieve light confinement and field enhancement in extremely small areas [~(λ/500)^2 ]. The proposal is based on a theoretical work[1] performed at Sandia. The paradigm structure consists of a periodic arrangement of connected small and large rectangular slits etched into a metal film named double-groove (DG) structure. The degree of electric field enhancement and power confinement can be controlled by the geometry of the structure. The key operational principle is attributed to quasistatic response of the metal electrons to the incoming electromagnetic field that enables non-resonant broadband behavior. For this exploratory LDRD we have fabricated some test double groove structures to enable verification of quasistatic electronic response in the mid IR through IR optical spectroscopy. We have addressed some processing challenges in DG structure fabrication to enable future design of complex sensor and detector geometries that can utilize its non-resonant field enhancement capabilities.].

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Multi frame synchrotron radiography of pulsed power driven underwater single wire explosions

We present herein the first use of synchrotron-based phase contrast radiography to study pulsed-power driven high energy density physics experiments. Underwater electrical wire explosions have become of interest to the wider physics community due to their ability to study material properties at extreme conditions and efficiently couple stored electrical energy into intense shock waves in water. The latter can be shaped to provide convergent implosions, resulting in very high pressures (1-10 Mbar) produced on relatively small pulsed power facilities (100s of kA-MA). Multiple experiments have explored single-wire explosions in water, hoping to understand the underlying physics and better optimize this energy transfer process; however, diagnostics can be limited. Optical imaging diagnostics are usually obscured by the shock wave itself; and until now, diode-based X-ray radiography has been of relatively low resolution and rather a broad x-ray energy spectrum. Utilising phase contrast imaging capabilities of the ID19 beamline at the European Synchrotron Radiation Facility, we were able to image both the exploding wire and the shock wave. Probing radiation of 20-50 keV radiographed 200 μm tungsten and copper wires, in ~2-cm diameter water cylinders with resolutions of 8 μm and 32 μm. The wires were exploded by a ~30-kA, 500-ns compact pulser, and 128 radiographs, each with a 100-ps X-ray pulse exposure, spaced at 704 ns apart were taken in each experiment. Abel inversion was used to obtain the density profile of the wires, and the results are compared to two dimensional hydrodynamic and one dimensional magnetohydrodynamic simulations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The interplay between chromophore and protein determines the extended excited state dynamics in a single-domain phytochrome

Phytochromes are a diverse family of bilin-binding photoreceptors that regulate a wide range of physiological processes. Their photochemical properties make them attractive for applications in optogenetics and superresolution microscopy. Phytochromes undergo reversible photoconversion triggered by the Z ⇌ E photoisomerization about the double bond in the bilin chromophore. However, it is not fully understood at the molecular level how the protein framework facilitates the complex photoisomerization dynamics. In this work, we have studied a single-domain bilin-binding photoreceptor All2699g1 ( Nostoc sp. PCC 7120) that exhibits photoconversion between the red light-absorbing (P r ) and far red-absorbing (P fr ) states just like canonical phytochromes. We present the crystal structure and examine the photoisomerization mechanism of the P r form as well as the formation of the primary photoproduct Lumi-R using time-resolved spectroscopy and hybrid quantum mechanics/molecular mechanics simulations. We show that the unusually long excited state lifetime (broad lifetime distribution centered at ~300 picoseconds) is due to the interactions between the isomerizing pyrrole ring D and an adjacent conserved Tyr142. The decay kinetics shows a strongly distributed character which is imposed by the nonexponential protein dynamics. Our findings offer a mechanistic insight into how the quantum efficiency of the bilin photoisomerization is tuned by the protein environment, thereby providing a structural framework for engineering bilin-based optical agents for imaging and optogenetics applications.

59 BASIC BIOLOGICAL SCIENCES↗

Atomic Force Microscope Active Optical Probe for Single-Molecule Imaging and Time-Resolved Optical Spectroscopy (DOE SBIR Phase II/IIA Final Report)

Actoprobe LLC reports on the results of its DOE SBIR Phase II/IIA project on the development of Atomic Force Microscope Active Optical Probe for Single-Molecule Imaging and Time-Resolved Optical Spectroscopy. While chemistry science and technology greatly benefit from Atomic Force Microscopy in surface characterization, time-resolved chemical imaging on the single-molecule level lags far behind. Current scanning probe microscopy only obtains information about mechanical but not optical/chemical properties. To address this problem, the Actoprobe LLC research team has proposed a novel class of Atomic Force Microscopy probes, Ultra-Fast Pulsed Active Atomic Force Microscopy Optical Probes (UFP AAOPs), that will allow ultrafast time-resolved optical and chemical imaging at the nanoscale. As envisioned, these unique optical probes will perform the functions of conventional Atomic Force Microscopy probes and, in addition, will simultaneously provide chemical information about molecular scale interactions. This innovation is accomplished by integrating an ultrafast pulsed Quantum Dot laser source into an Atomic Force Microscopy probe. This report describes our progress with the fabrication of an ultrafast micrometer-size semiconductor laser, based on “artificial atoms” - Quantum Dots, integrated with an Atomic Force Microscopy probe. In this Phase II/IIA project, we have demonstrated the feasibility of the UFP AAOP concept by fabricating a first prototype of the UFP AAOP. The excellent performance of the probe has been proven in terms of AFM and optical spatial resolution through rigorous tests. The UFP AAOP provides pulses with less than 4 ps duration and higher than 11 GHz repetition rate, and spatial resolution better than 300 nm at 1240 nm wavelength. Technically, it is possible to reduce the pulse width to less than 1 ps and to improve lateral resolution to ~ 0.5 nm, which implies the potential capability for the probe to characterize chemical compounds with single-molecule resolution. The UFP AAOP fabrication procedure has been developed for wafer-scale production of multiple devices, with the yield of the process estimated to be lower than 1% with the limited fabrication capabilities and equipment available for use in the research project. However, using high-volume production tools and special GaAs processing equipment, the yield can be significantly improved, theoretically to ~ 50%. Finally, economic feasibility and scale-up manufacturing potential were analyzed for UFP AAOP and found to be very promising. In summary, the Actoprobe team has successfully demonstrated the feasibility of the UFP AAOP concept.

36 MATERIALS SCIENCE↗

Probe the Localized Electrochemical Environment Effects and Electrode Reaction Dynamics for Metal Batteries using In Situ 3D Microscopy

Uncontrollable dendrite growth is closely related to non-uniform reaction environments. However, there is a lack of understanding and analysis methods to probe the localized electrochemical environment (LEE). Here the effects of the LEE are investigated, including localized ion concentrations, current density, and electric potential, on metal plating/stripping dynamics and dendrite minimization. A novel in situ 3D microscopy technique is developed to image the morphology dynamics and deposition rate of Zn plating/stripping processes on 3D Zn–Mn anodes. Using the in situ 3D microscope, the electrode morphology changes during the reactions are directly imaged and Zn deposition rate maps at different time points are obtained. It is found that reaction kinetics are highly correlated to LEE and electrode morphology. To further quantify the LEE effects, the digital twin technique is employed that allows the accurate calculation of the electrochemical environments, such as localized ion concentrations, current density, and electric potential, which cannot be directly measured from experiments. We found that the curvature of the 3D electrode surface determines the LEE and significantly influences reaction kinetics. This provides a new strategy to minimize the dendrite formation by designing and optimizing the 3D geometry of the electrode to control the LEE.

36 MATERIALS SCIENCE↗

Foundations of machine learning for low-temperature plasmas: methods and case studies

Abstract Machine learning (ML) and artificial intelligence have proven to be an invaluable tool in tackling a vast array of scientific, engineering, and societal problems. The main drivers behind the recent proliferation of ML in practically all aspects of science and technology can be attributed to: (a) improved data acquisition and inexpensive data storage; (b) exponential growth in computing power; and (c) availability of open-source software and resources that have made the use of state-of-the-art ML algorithms widely accessible. The impact of ML on the field of low-temperature plasmas (LTPs) could be particularly significant in the emerging applications that involve plasma treatment of complex interfaces in areas ranging from the manufacture of microelectronics and processing of quantum materials, to the LTP-driven electrification of the chemical industry, and to medicine and biotechnology. This is primarily due to the complex and poorly-understood nature of the plasma-surface interactions in these applications that pose unique challenges to the modeling, diagnostics, and predictive control of LTPs. As the use of ML is becoming more prevalent, it is increasingly paramount for the LTP community to be able to critically analyze and assess the concepts and techniques behind data-driven approaches. To this end, the goal of this paper is to provide a tutorial overview of some of the widely-used ML methods that can be useful, amongst others, for discovering and correlating patterns in the data that may be otherwise impractical to decipher by human intuition alone, for learning multivariable nonlinear data-driven prediction models that are capable of describing the complex behavior of plasma interacting with interfaces, and for guiding the design of experiments to explore the parameter space of plasma-assisted processes in a systematic and resource-efficient manner. We illustrate the utility of various supervised, unsupervised and active learning methods using LTP datasets consisting of commonly-available, information-rich measurements (e.g. optical emission spectra, current–voltage characteristics, scanning electron microscope images, infrared surface temperature measurements, Fourier transform infrared spectra). All the ML demonstrations presented in this paper are carried out using open-source software; the datasets and codes are made publicly available. The FAIR guiding principles for scientific data management and stewardship can accelerate the adoption and development of ML in the LTP community.

Physics↗

On the solid phase crystallization of In{sub 2}O{sub 3}:H transparent conductive oxide films prepared by atomic layer deposition

Hydrogen-doped indium oxide (In{sub 2}O{sub 3}:H) has emerged as a highly transparent and conductive oxide, finding its application in a multitude of optoelectronic devices. Recently, we have reported on an atomic layer deposition (ALD) process to prepare high quality In{sub 2}O{sub 3}:H. This process consists of ALD of In{sub 2}O{sub 3}:H films at 100 °C, followed by a solid phase crystallization step at 150–200 °C. In this work, we report on a detailed electron microscopy study of this crystallization process which reveals new insights into the crucial aspects for achieving the large grain size and associated excellent properties of the material. The key finding is that the best optoelectronic properties are obtained by preparing the films at the lowest possible temperature prior to post-deposition annealing. Electron microscopy imaging shows that such films are mostly amorphous, but feature a very low density of embedded crystallites. Upon post-deposition annealing, crystallization proceeds merely from isotropic crystal grain growth of these embedded crystallites rather than by the formation of additional crystallites. The relatively high hydrogen content of 4.2 at. % in these films is thought to cause the absence of additional nucleation, thereby rendering the final grain size and optoelectronic properties solely dependent on the density of embedded crystallites. The temperature-dependent grain growth rate has been determined, from which an activation energy of (1.39 ± 0.04) eV has been extracted. Finally, on the basis of the observed crystallization mechanism, a simple model to fully describe the crystallization process has been developed. This model has been validated with a numerical implementation thereof, which accurately predicts the observed temperature-dependent crystallization behaviour.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The nature of catastrophic OLED lighting panel failure

Catastrophic failure due to electrical shorting is currently one of the key reliability challenges for commercial organic light emitting diode (OLED) solid-state lighting panels. Here, we explore the origin of panel-killing shorts through the use of a temperature-selective electroluminescence imaging technique that allows us to locate them early in their life cycle and study their growth over time. We identify two general classes of panel defect, termed bright spots and hot spots, which respectively originate from indium-tin-oxide agglomerations and microscale organic semiconductor dust particles on the substrate. The former are largely benign, whereas the latter can lead to local shunts that grow over time and cause catastrophic failure. We understand the growth process as a self-reinforcing cycle, where shunt-induced heating volatilizes the surrounding organic semiconductor, which in turn expands the shunt and leads to even more heating. Finally based on these results, we identify several practical strategies to arrest the growth of early-stage shorts or prevent them entirely, which could reduce the cost and improve the reliability of OLED lighting.

36 MATERIALS SCIENCE↗