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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Engineering Directionality in Quantum Dot Shell Lasing Using Plasmonic Lattices

In this paper, we report how the direction of quantum dot (QD) lasing can be engineered by exploiting high-symmetry points in plasmonic nanoparticle (NP) lattices. The nanolaser architecture consists of CdSe-CdS core-shell QD layers conformally coated on two-dimensional square arrays of Ag NPs. Using waveguide-surface lattice resonances (W-SLRs) near the Δ point in the Brillouin zone as optical feedback, we achieved lasing from the gain in CdS shells at off-normal emission angles. Changing the periodicity of the plasmonic lattices enables other high-symmetry points (Γ or M) of the lattice to overlap with the QD shell emission, which facilitates tuning of the lasing direction. We also increased the thickness of the QD layer to introduce higher order W-SLR modes with additional avoided crossings in the band structure, which expands the selection of cavity modes for any desired lasing emission angle.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Hot Electron-Driven Photocatalysis Using Sub-5 nm Gap Plasmonic Nanofinger Arrays

Semiconductor photocatalysis has received increasing attention because of its potential to address problems related to the energy crisis and environmental issues. However, conventional semiconductor photocatalysts, such as TiO2 and ZnO, can only be activated by ultraviolet light due to their wide band gap. To extend the light absorption into the visible range, the localized surface plasmon resonance (LSPR) effect of noble metal nanoparticles (NPs) has been widely used. Noble metal NPs can couple incident visible light energy to strong LSPR, and the nonradiative decay of LSPR generates nonthermal hot carriers that can be injected into adjacent semiconductor material to enhance its photocatalytic activity. Here we demonstrate that nanoimprint-defined gap plasmonic nanofinger arrays can function as visible light-driven plasmonic photocatalysts. The sub-5 nm gaps between pairs of collapsed nanofingers can support ultra-strong plasmon resonance and thus boost the population of hot carriers. The semiconductor material is exactly placed at the hot spots, providing an efficient pathway for hot carrier injection from plasmonic metal to catalytic materials. This nanostructure thus exhibits high plasmon-enhanced photocatalytic activity under visible light. The hot carrier injection mechanism of this platform was systematically investigated. The plasmonic enhancement factor was calculated using the finite-difference time-domain (FDTD) method and was consistent with the measured improvement of the photocatalytic activity. This platform, benefiting from the precise controllable geometry, provides a deeper understanding of the mechanism of plasmonic photocatalysis.

42 ENGINEERING↗
DOE OSTI2023

Optimization and understanding of ZnO nanoarray supported Cu-ZnO-Al 2 O 3 catalyst for enhanced CO 2 -methanol conversion at low temperature and pressure

Cu-ZnO-Al 2 O 3 is the most widely applied catalyst for CO 2 hydrogenation to methanol. However, it is still a challenge to produce methanol using this catalyst under low-temperature (<250 °C) and low-pressure (<10 bar) conditions with desirable yield and selectivity. In this work, by tuning the experimental processing parameters such as solvent, loading amount, and annealing temperature, highly improved ZnO nanoarray supported Cu-ZnO-Al 2 O 3 catalysts have been successfully demonstrated. Here, by using organic solvent (N,N-dimethylformamide (DMF), acetone, or isopropanol) for dip-coating loading process instead of deionized (DI) water, Cu-ZnO-Al 2 O 3 nanocatalysts was comparatively better dispersed on the nanorod array support with populated and abundant active sites, thus enhancing the methanol yield. With the control of the loading amount and annealing temperature, finely distributed Cu nanoparticles were obtained on the ZnO nanorod surfaces to enhance the interactions between Cu and ZnO nanorod surfaces. Further improvement of the catalyst performance is demonstrated by tuning the reaction space velocity. At 200 °C and 10 bar conditions, the optimized catalyst achieved a methanol yield of 6.46 mol h –1 kg –1 with 100 % selectivity. The good stability after prolonged testing of the catalysts demonstrates the potential practical implementation. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements under the 1 bar reveal that the CO 2 hydrogenation to methanol on the ZnO nanoarray supported Cu-ZnO-Al 2 O 3 catalyst follows the CO reaction pathway, due to the surface oxygen vacancies on ZnO nanorods which facilitate CO 2 dissociation.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Characterization of a Pixelated Cadmium Telluride Detector System Using a Polychromatic X-Ray Source and Gold Nanoparticle-Loaded Phantoms for Benchtop X-Ray Fluorescence Imaging

In this paper, the imaging dose and scan time have been considered as the two major constraints for routine benchtop x-ray fluorescence computed tomography (XFCT) imaging. One way to address this issue is to acquire x-ray fluorescence (XRF) signals in parallel through a 2D array of single-crystal detectors or a pixelated detector along with the cone-beam x-ray source. To identify a detector system suitable for this purpose, a commercially available, fully spectroscopic cadmium telluride (CdTe) pixelated detector, HEXITEC (High-Energy X-ray Imaging Technology), was tested under the experimental conditions optimized for benchtop XFCT imaging of gold nanoparticles (GNPs). Specifically, two different parallel-hole stainless steel collimators were fabricated and coupled with the detector for seamless integration into our existing benchtop cone-beam XFCT system. After the detector deployment, this benchtop XFCT system was used to detect XRF photons from GNP-loaded phantoms. A pixel-merging algorithm was introduced to enhance the sensitivity of XRF photon detection thereby minimizing the scan time. The effect of pixel-level charge sharing correction algorithms was investigated within the context of benchtop XFCT imaging. The detector energy resolution, in terms of the full width at half maximum (FWHM) values at different gold K-shell XRF energies, was also determined. Of the two charge sharing correction algorithms examined, the charge sharing addition gave better sensitivity than the charge sharing discrimination (csd). On the other hand, under the current experimental conditions, the energy resolution of the HEXITEC detector was the best with the csd and estimated to be 1.56 keV FWHM at 66-69 keV photon energy. Overall, despite some degradation of the detector energy resolution (compared with typical single crystal CdTe detectors), the HEXITEC detector enabled parallel data acquisition under the experimental conditions typical of benchtop XFCT imaging and operated well within our benchtop XFCT setup.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Engineering endosomolytic nanocarriers of diverse morphologies using confined impingement jet mixing

The clinical translation of many biomolecular therapeutics has been hindered by undesirable pharmacokinetic (PK) properties, inadequate membrane permeability, poor endosomal escape and cytosolic delivery, and/or susceptibility to degradation. Overcoming these challenges merits the development of nanoscale drug carriers (nanocarriers) to improve the delivery of therapeutic cargo. Herein, we implement a flash nanoprecipitation (FNP) approach to produce nanocarriers of diverse vesicular morphologies by using various molecular weight PEG-bl-DEAEMA-co-BMA (PEG-DB) polymers. We demonstrated that FNP can produce uniform (PDI < 0.1) particles after 5 impingements, and that by varying the copolymer hydrophilic mass fraction, FNP enables access to a diverse variety of nanoarchitectures including micelles, unilamellar vesicles (polymersomes), and multi-compartment vesicles (MCVs). We synthesized a library of 2 kDa PEG block copolymers, with DEAEMA-co-BMA second block molecular weights of 3, 6, 12, 15, 20, and 30 kDa. All formulations were both pH responsive, endosomolytic, and capable of loading and cytosolically delivering small negatively charged molecules – albeit to different degrees. Using a B16.F10 melanoma model, we showcased the therapeutic potential of a lead FNP formulated PEG-DB nanocarrier, encapsulating the cyclic dinucleotide (CDN) cGAMP to activate the stimulator of interferon genes (STING) pathway in a therapeutically relevant context. Collectively, these data demonstrate that an FNP process can be used to formulate pH-responsive nanocarriers of diverse morphologies using a PEG-DB polymer system. As FNP is an industrially scalable process, these data address the critical translational challenge of producing PEG-DB nanoparticles at scale. Furthermore, the diverse morphologies produced may specialize in the delivery of distinct biomolecular cargos for other therapeutic applications, implicating the therapeutic potential of this platform in an array of disease applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Optics-Free Chip-Scale Intraoperative Imaging Using NIR-Excited Upconverting Nanoparticles

Here we present an optics-free CMOS image sensor that incorporates a novel time-gated dual-photodiode pixel design to allow filter- and lens-less image acquisition of near-infrared-excited (NIR-excited) upconverting nanoparticles. Recent biomedical advances have highlighted the benefits of NIR excitation, but NIR interaction with silicon has remained a challenge, even with high-performance optical blocking filters. Using a secondary diode and a dual-photodiode design, this sensor is able to remove the 100s of mV of NIR background on pixels and bring it down to single-digit mV level, nearing its noise floor of 2.2 mV rms, not achievable with any optical filter. Non-linear effects of background cancellation using the diode pair has been mitigated using an initial one-time pixel-level curve fitting and calibration in a post-processing setting. This imager comprises a highly linear 11 fF metal-oxide-metal (MOM) capacitor and includes integrated angle-selective gratings to reject oblique light and enhance sharpness. Each pixel also includes two distinct correlated double sampling schemes, to remove low frequency flicker noise and systematic offset in the datapath. We demonstrate the performance of this imager using pulsed NIR-excited upconverting nanoparticles on standard United-States-Air-Force (USAF) resolution targets and achieve an SNR of 15 dB, while keeping NIR background below 6 mV. This 36-by-80-pixel array measures only 2.3 mm by 4.8 mm and can be thinned down to 25 µm, allowing it to become surgically compatible with intraoperative instruments and equipment, while remaining optics-free.

42 ENGINEERING↗
DOE OSTI2023

Improving nanoparticle superlattice stability with deformable polymer gels

The self-assembly of colloidal nanoparticles into ordered superlattices typically uses dynamic interactions to govern particle crystallization, as these non-permanent bonds prevent the formation of kinetically trapped, disordered aggregates. However, while the use of reversible bonding is critical in the formation of highly ordered particle arrangements, dynamic interactions also inherently make the structures more prone to disassembly or disruption when subjected to different environmental stimuli. Thus, there is typically a trade-off between the ability to initially form an ordered colloidal material and the ability of that material to retain its order under different conditions. Here, we present a method for embedding colloidal nanoparticle superlattices into a polymer gel matrix. This encapsulation strategy physically prevents the nanoparticles from dissociating upon heating, drying, or the introduction of chemicals that would normally disrupt the lattice. However, the use of a gel as the embedding medium still permits further modification of the colloidal nanoparticle lattice by introducing stimuli that deform the gel network (as this deformation in turn alters the nanoparticle lattice structure in a predictable manner). Moreover, encapsulation of the lattice within a gel permits further stabilization into fully solid materials by removing the solvent from the gel or by replacing the solvent with a liquid monomer that can be photopolymerized. This embedding method therefore makes it possible to incorporate ordered colloidal arrays into a polymer matrix as either dynamic or static structures, expanding their potential for use in responsive materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Runtime performance of a GAMESS quantum chemistry application offloaded to GPUs

Summary Computational chemistry is at the forefront of solving urgent societal problems, such as polymer upcycling and carbon capture. The complexity of modeling these processes at appropriate length and time scales is mainly manifested in the number and types of chemical species involved in the reactions and may require models of several thousand atoms and large basis sets to accurately capture the chemical complexity and heterogeneity in the physical and chemical processes. The quantum chemistry package General Atomic and Molecular Electronic Structure System (GAMESS) has a wide array of methods that can efficiently and accurately treat complex chemical systems. In this work, we have used the GAMESS Effective Fragment Molecule Orbital (EFMO) method for electronic structure calculation of a challenging mesoporous silica nanoparticle (MSN) model surrounded by about 4700 water molecules to investigate the strong scaling and GPU offloading on hybrid CPU‐GPU nodes. Experiments were performed on the Perlmutter platform at the National Energy Research Scientific Computing Center. Good strong scaling and load balancing have been observed on up to 88 hybrid nodes for different settings of the execution parameters for the calculation considered here. When GPUs are oversubscribed by offloading work from multiple CPU processes, using the NVIDIA multi‐process service (MPS) has consistently reduced time to solution and energy consumed. Additionally, for some configuration parameter settings, oversubscription with MPS improved performance by up to 5.8% over the case without oversubscription.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Thermodynamic approach for enhancing superconducting critical current performance

Abstract The addition of artificial pinning centers has led to an impressive increase in the critical current density ( J c ) of superconductors, enabling record-breaking all-superconducting magnets and other applications. The J c of superconductors has reached ~0.2–0.3 J d , where J d is the depairing current density, and the numerical factor depends on the pinning optimization. By modifying λ and/or ξ, the penetration depth and coherence length, respectively, we can increase J d . For (Y 0.77 Gd 0.23 )Ba 2 Cu 3 O y ((Y,Gd)123), we can achieve this by controlling the carrier density, which is related to λ and ξ. We can also tune λ and ξ by controlling the chemical pressure in Fe-based superconductors, i.e., BaFe 2 (As 1− x P x ) 2 films. The variation in λ and ξ leads to an intrinsic improvement in J c via J d , allowing extremely high values of J c of 130 MA/cm 2 and 8.0 MA/cm 2 at 4.2 K, consistent with an enhancement in J d of a factor of 2 for both incoherent nanoparticle-doped (Y,Gd)123 coated conductors (CCs) and BaFe 2 (As 1− x P x ) 2 films, showing that this new material design is useful for achieving high critical current densities in a wide array of superconductors. The remarkably high vortex-pinning force in combination with this thermodynamic and pinning optimization route for the (Y,Gd)123 CCs reached ~3.17 TN/m 3 at 4.2 K and 18 T ( H || c ), the highest values ever reported for any superconductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Dark and bright modes, and their coherent control in dipolar metasurface bilayers

Several plasmonic nanoparticles supporting dipolar resonances can couple to form normal modes. Here, we develop an analytical model to explain the formation of nonradiative “dark” and radiative “bright” modes through radiative coupling in bilayers consisting of dipolar nanoantenna arrays that are separated by a subwavelength distance. We also include near-field contributions in our model and show that the absorption and reflectance spectra obtained from our model agree reasonably well with the respective finite-difference time-domain simulation results for both perfectly aligned and misaligned bilayers. Here, the ability to vary the reflection and absorption spectra of these bilayers by changing the material and geometrical parameters has potential applications in the design of efficient spectral filters. We also show that we can selectively excite these modes by adjusting the phase between two counterpropagating normally incident fields, which has applications in all-optical modulators and switches based on purely linear interferometric effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Probing T Cell 3D Mechanosensing With Magnetically-Actuated Structures

The ability of cells to recognize and respond to the mechanical properties of their environment is of increasing importance in T cell physiology. However, initial studies in this direction focused on planar hydrogel and elastomer surfaces, presenting several challenges in interpretation including difficulties in separating mechanical stiffness from changes in chemistry needed to modulate this property. We introduce here the use of magnetic fields to change the structural rigidity of microscale elastomer pillars loaded with superparamagnetic nanoparticles, independent of substrate chemistry. This magnetic modulation of rigidity, embodied as the pillar spring constant, changed the interaction of mouse naïve CD4 + T cells from a contractile morphology to one involving deep embedding into the array. Furthermore, increasing spring constant was associated with higher IL-2 secretion, showing a functional impact on mechanosensing. The system introduced here thus separates local substrate stiffness and long-range structural rigidity, revealing new facets of T cell interaction with their environment.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2023

Flexible Vanadium Dioxide Photodetectors for Visible to Longwave Infrared Detection at Room Temperature

Abstract Flexible optoelectronics is a rapidly growing field, with a wide range of potential applications. From wearable sensors to bendable solar cells, curved displays, and curved focal plane arrays, the possibilities are endless. The criticality of flexible photodetectors for many of these applications is acknowledged, however, devices that are demonstrated thus far are limited in their spectral range. In this study, flexible photodetectors are demonstrated using a VO x nanoparticle ink, with an extremely broad operating wavelength range of 0.4 to 20 µm. This ink is synthesized using a simple and scalable wet‐chemical process. These photodetectors operate at room temperature and exhibit minimal variance in performance even when bent at angles of up to 100 ° at a bend radius of 6.4 mm. In addition, rigorous strain testing of 100 bend and release cycles revealed a photoresponse with a standard deviation of only 0.55%. This combination of mechanical flexibility, wide spectral response, and ease of fabrication makes these devices highly desirable for a wide range of applications, including low‐cost wearable sensors and hyperspectral imaging systems.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Nanoporous Titanium (Oxy)nitride Films as Broadband Solar Absorbers

Broadband absorption of solar light is a key aspect in many applications that involve an efficient conversion of solar energy to heat. Titanium nitride (TiN)-based materials, in the form of periodic arrays of nanostructures or multilayers, can promote significant heat generation upon illumination thanks to their efficient light absorption and refractory character. In this work, pulsed laser deposition was chosen as a synthesis technique to shift metallic bulk-like TiN to nanoparticle-assembled hierarchical oxynitride (TiO x N y ) films by increasing the background gas deposition pressure. The nanoporous hierarchical films exhibit a tree-like morphology, a strong broadband solar absorption (~90% from the UV to the near-infrared range), and could generate temperatures of ~475 °C under moderate light concentration (17 Suns). The high heat generation achieved by treelike films is ascribed to their porous morphology, nanocrystalline structure, and oxynitride composition, which overall contribute to a superior light trapping and dissipation to heat. These properties pave the way for the implementation of such films as solar absorber structures.

14 SOLAR ENERGY↗
NASA NTRS2007

Ultra-Lightweight Hybrid Thin-Film Solar Cells: A Survey of Enabling Technologies for Space Power Applications

The development of hybrid inorganic/organic thin-film solar cells on flexible, lightweight, space-qualified, durable substrates provides an attractive solution for fabricating solar arrays with high mass specific power (W/kg). Next generation thin-film technologies may well involve a revolutionary change in materials to organic-based devices. The high-volume, low-cost fabrication potential of organic cells will allow for square miles of solar cell production at one-tenth the cost of conventional inorganic materials. Plastic solar cells take a minimum of storage space and can be inflated or unrolled for deployment. We will explore a cross-section of in-house and sponsored research efforts that aim to provide new hybrid technologies that include both inorganic and polymer materials as active and substrate materials. Research at University of Texas at Arlington focuses on the fabrication and use of poly(isothianaphthene-3,6-diyl) in solar cells. We describe efforts at Norfolk State University to design, synthesize and characterize block copolymers. A collaborative team between EIC Laboratories, Inc. and the University of Florida is investigating multijunction polymer solar cells to more effectively utilize solar radiation. The National Aeronautics and Space Administration (NASA)/Ohio Aerospace Institute (OAI) group has undertaken a thermal analysis of potential metallized substrates as well as production of nanoparticles of CuInS2 and CuInSe2 in good yield at moderate temperatures via decomposition of single-source precursors. Finally, preliminary work at the Rochester Institute of Technology (R.I.T.) to assess the impact on performance of solar cells of temperature and carbon nanotubes is reported. Technologies that must be developed to enable ultra-lightweight solar arrays include: monolithic interconnects, lightweight array structures, and new ultra-light support and deployment mechanisms. For NASA applications, any solar cell or array technology must not only meet weight and AMO efficiency goals, but also must be durable enough to survive launch conditions and space environments.

Hepp, Aloysius F.↗
NASA NTRS2004

Electrochemical Reconstitution of Biomolecules for Applications as Electrocatalysts for the Bionanofuel Cell

Platinum-cored ferritins were synthesized as electrocatalysts by electrochemical biomineralization of immobilized apoferritin with platinum. The platinum cored ferritin was fabricated by exposing the immobilized apoferritin to platinum ions at a reduction potential. On the platinum-cored ferritin, oxygen is reduced to water with four protons and four electrons generated from the anode. The ferritin acts as a nano-scale template, a biocompatible cage, and a separator between the nanoparticles. This results in a smaller catalyst loading of the electrodes for fuel cells or other electrochemical devices. In addition, the catalytic activity of the ferritin-stabilized platinum nanoparticles is enhanced by the large surface area and particle size phenomena. The work presented herein details the immobilization of ferritin with various surface modifications, the electrochemical biomineralization of ferritin with different inorganic cores, and the fabrication of self-assembled 2-D arrays with thiolated ferritin.

Kim, Jae-Woo↗
DOE OSTI2023

Electrochemical polymer pen lithography

Disclosed herein is a massively parallel patterning tool for the deposition of single metals or metal alloys with size and composition control. Methods of the disclosure use a hydrogel array of pyramidal pen tips as a medium for localized electrodeposition, in conjunction with a scanning probe lithography platform and a three-electrode cell. This versatile technique can be used for high-throughput 3D printing, biomolecule patterning, or screening of catalyst nanoparticles or thin films.

Mirkin, Chad A.↗