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All sources NASA NTRS DOE OSTI

DOE OSTI2017

Lattice Mismatch in Crystalline Nanoparticle Thin Films

For atomic thin films, lattice mismatch during heteroepitaxy leads to an accumulation of strain energy, generally causing the films to irreversibly deform and generate defects. In contrast, more elastically malleable building blocks should be better able to accommodate this mismatch and the resulting strain. In our work, that hypothesis is tested by utilizing DNA-modified nanoparticles as “soft,” programmable atom equivalents to grow a heteroepitaxial colloidal thin film. Calculations of interaction potentials, small-angle X-ray scattering data, and electron microscopy images show that the oligomer corona surrounding a particle core can deform and rearrange to store elastic strain up to ±7.7% lattice mismatch, substantially exceeding the ±1% mismatch tolerated by atomic thin films. Importantly, these DNA-coated particles dissipate strain both elastically through a gradual and coherent relaxation/ broadening of the mismatched lattice parameter and plastically (irreversibly) through the formation of dislocations or vacancies. These data also suggest that the DNA cannot be extended as readily as compressed, and thus the thin films exhibit distinctly different relaxation behavior in the positive and negative lattice mismatch regimes. These observations provide a more general understanding of how utilizing rigid building blocks coated with soft compressible polymeric materials can be used to control nano- and microstructure.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Consequences of Lattice Mismatch for Phase Equilibrium in Heterostructured Solids

Lattice mismatch - the difference in natural bond length between two species comprising a solid is a common occurrence in modern materials. Spatial patterns in certain nanocrystal heterostructures, for instance, are thought to be a result of elastic forces arising from lattice mismatch. However, the role of lattice mismatch in mediating the arrangement of atoms in such materials is incompletely understood. Here we consider a simple microscopic model for lattice mismatch, in which the difference in natural lengths between bonded atoms produces interactions mediated by elastic strain. Computer simulations reveal that the model exhibits rich phase behavior, including structures with periodic order and unusual coexistence scenarios. To explain this phase behavior, we derive an effective pairwise interaction potential between atoms, revealing preferred spatial arrangements of atoms driven by spatial variations in the interaction potential. We then develop a mean field theory based on this effective interaction which qualitatively captures observed transition to phases with modulated order. Finally, we explain the observed scenarios of coexistence between using a graphical construction, based on the realization that the free energy cost of phase separation in elastic systems grows with system size. Here, these results clarify the equilibrium effects of lattice mismatch in macroscopic solids and suggest a role for lattice mismatch in creating spatially heterogeneous compositions in nanoscale materials.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Effect of Coherent Lattice Mismatch on the Morphology and Kinetics of Ordered Precipitates

The morphological evolution and precipitation kinetics of ordered precipitates under the influence of lattice mismatch were studied by using the phase field model. The variation of the average aspect ratio of the precipitates and their distributions was investigated quantitatively, and the relationship of particles shape and particles fraction with the variation of the aspect ratio was determined. As the lattice mismatch increases, the coarsening rate constants and the particles number density decrease, the particles size distribution (PSD) becomes narrower, and the peak value of the PSD becomes lower than the value obtained by the Lifshitz–Slyozov–Wagner theory, while it is close to the value obtained by the Brailsford–Wynblatt theory. The change rate of the particles number density shows four-stage characteristics and decreases as the lattice mismatch and time increase, indicating that the precipitation and coarsening are retarded for a large lattice mismatch and that a large lattice mismatch results in fewer particles being dispersed in the matrix phase. The morphology and the particles number density show that a suitable lattice mismatch can enhance the mechanical properties of the alloys.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Ribosome Structure Reveals Preservation of Active Sites in the Presence of a P-Site Wobble Mismatch

Translation initiation in the P site occasionally occurs at atypical (non-AUG) start codons, including those forming a mismatch in the third (wobble) position. During elongation, however, a pyrimidine-pyrimidine wobble mismatch may trigger a translation quality-control mechanism, whereby the P-site mismatch is thought to perturb the downstream A-site codon or the decoding center, thereby reducing translation fidelity and inducing termination of aberrant translation. We report a crystal structure of the 70S initiation complex containing an AUC codon in the ribosomal P site. Remarkably, the ribosome stabilizes the mismatched codon-anticodon helix, arranging a normally disruptive cytosine-cytosine pair into a Watson-Crick-like conformation. Here, the translation-competent conformations of the tRNA, mRNA, and decoding center suggest that a P-site wobble-position mismatch in the 70S initiation complex does not pre-arrange the mRNA or decoding center to favor subsequent miscoding events.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Security proof of practical quantum key distribution with detection-efficiency mismatch

Quantum key distribution (QKD) protocols with threshold detectors are driving high-performance QKD demonstrations. The corresponding security proofs usually assume that all physical detectors have the same detection efficiency. However, the efficiencies of the detectors used in practice might show a mismatch depending on the manufacturing and setup of these detectors. A mismatch can also be induced as the different spatial-temporal modes of an incoming signal might couple differently to a detector. Here we develop a method that allows to provide security proofs without the usual assumption. Our method can take the detection-efficiency mismatch into account without having to restrict the attack strategy of the adversary. Especially, we do not rely on any photon-number cutoff of incoming signals such that our security proof is directly applicable to practical situations. We illustrate our method for a receiver that is designed for polarization encoding and is sensitive to a number of spatial-temporal modes. In our detector model, the absence of quantum interference between any pair of spatial-temporal modes is assumed. For a QKD protocol with this detector model, we can perform a security proof with characterized efficiency mismatch and without photon-number cutoff assumption. Our method also shows that in the absence of efficiency mismatch in our detector model, the key rate increases if the loss due to detection inefficiency is assumed to be outside of the adversary's control, as compared to the view where for a security proof this loss is attributed to the action of the adversary.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2019

Bifacial PV System Mismatch Loss Estimation & Parameterization

Non-uniform irradiance on the rear-side of bifacial PV systems can cause additional mismatch loss which may not be appropriately captured in PV energy production estimates and software. We have evaluated several rooftop mounted systems over high albedo reflective roofs. Mismatch losses of up to 2% annual loss for very close-mounted (0.15 m) rooftop systems were found, but losses for high ground-clearance rooftop systems were lower (<0.5%). A simplified empirical relationship was found that links the spatial variation of irradiance (specifically the mean absolute difference of irradiance) to the resulting mismatch loss factor, with a R2 fit better than 0.985. This approximate relationship has been validated by experiments on mismatched PV modules, and provides a basis for fast estimation of bifacial mismatch loss factors for use in hourly PV performance simulations such as PVSyst or SAM.

14 SOLAR ENERGY↗

DOE OSTI2019

Bifacial PV System Mismatch Loss Estimation and Parameterization: Preprint

Non-uniform irradiance on the rear-side of bifacial PV systems can cause additional mismatch loss which may not be appropriately captured in PV energy production estimates and software. We have evaluated several scenarios including horizontal single-axis tracking (HSAT) and rooftop mounted systems over high albedo reflective roofs. Mismatch losses of up to 2% annual loss for very close-mounted (0.15 m) rooftop systems were found, but losses for HSAT systems and high ground-clearance rooftop systems were lower (<0.5%). A simplified empirical relationship was found that links the spatial variation of irradiance (specifically the mean absolute difference of irradiance) to the resulting mismatch loss factor, with a R2 fit better than 0.985. This approximate relationship has been validated by experiments on mismatched PV modules, and provides a basis for fast estimation of bifacial mismatch loss factors for use in hourly PV performance simulations such as PVSyst or SAM.

14 SOLAR ENERGY↗

DOE OSTI2017

Overcoming the Interfacial Lattice Mismatch: Geometry Control of Gold-Nickel Bimetallic Heteronanostructures

Seed-mediated heteroepitaxial growth provides a versatile synthetic approach to a diverse set of geometrically distinct bimetallic heteronanostructures. In bimetallic nanocrystal systems, interfacial heteroepitaxial growth typically occurs between structurally similar metals with lattice mismatch below 5%, whereas controlled epitaxial growth of bimetallic nanocrystals comprising metals with larger lattice mismatches or even dissimilar crystalline structures has long been challenging. Here in this work, the epitaxial growth of both face-centered cubic (fcc) and hexagonal close-packed (hcp) Ni on fcc Au nanocrystal seeds in polyol solvents is systematically investigated, to shed light on the complex mechanisms underpinning the intriguing geometric evolution of lattice-mismatched bimetallic nanocrystals during seed-mediated heteroepitaxial overgrowth. The success in geometry-controlled syntheses of a series of Au–Ni bimetallic heteronanostructures, such as conformal core–shell nanoparticles, asymmetric heterodimers, and multibranched core–satellite nanocrystals, represents a significant step toward the extension of nanoscale interfacial heteroepitaxy from lattice-matched bimetallic systems to the ones exhibiting large lattice mismatches and even dissimilar crystalline structures. In conclusion, the insights gained from this work serve as a central design principle that guides the development of new synthetic approaches to architecturally sophisticated and compositionally diverse multimetallic heteronanostructures.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Amplified detection of single base mismatches with the competing-strand assay reveals complex kinetic and thermodynamic behavior of strand displacement at the electrode surface

Detection of single-base mismatches with respect to a probe strand has been a predominant pursuit in electrochemical biosensor efforts, due to links found between single nucleotide polymorphisms (SNPs) and the predisposition to various diseases. We report an osmium tetroxide bipyridine-based, thermally-controlled, competitive-strand electrochemical assay to allow amplified detection of single-base mismatches. Optimally designed competitive-strand displacement and hybridization temperature allows us to distinguish the single-mismatched-target from the fully complementary sequence with unambiguous, highly reproducible, robust signal differences of over 90%. Furthermore, we find a complex interplay between the position of the redox label, variations in strand displacement kinetics due to mismatches incorporated into the competitive strand, and alterations in the melting temperature of DNA duplexes tethered on the gold surface, when probed by square-wave voltammetry. Furthermore, these insights will apply to any surface-tethered DNA-based electrochemical biosensor, and can help with understanding complex phenomena involved in these types of assays.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

A Coordinated Compensation Strategy for Module-Mismatch of CHB-PV Systems Based on Improved LS-PWM and Reactive Power Injection

Here, the cascaded H-bridge (CHB) converter has become a promising candidate topology for utility-scale photovoltaic systems thanks to merits like modular structure, distributed maximum power point tracking (MPPT), and direct distribution grid access without medium-voltage transformers, etc. However, module-mismatches arising from non-ideal elements like partial shading and parameter variations pose a technical challenge for such systems. If not dealt with properly, module-mismatches can lead to adverse effects like unbalanced dc-link voltages of the modules, distortion of grid current, reduced power generation, etc. Conventional methods, such as reactive power compensation and level-shifted pulse-width modulation (LS-PWM) based compensation, can alleviate this issue, but their performances are still limited by the allowable modulation range of power converters. In this paper, a compensation strategy combining reactive power compensation with a novel modulation method is proposed to extend the operating range in terms of module mismatch. Experimental results on a 2.4kW/208V single-phase setup are presented and have demonstrated that the proposed method can not only ride through a larger range of module-mismatches but also improve solar power utilization and system efficiency owing to reduced switching events, non-compromised MPPT, and less required reactive power.

42 ENGINEERING↗

DOE OSTI2022

Locating fast-varying line disturbances with the frequency mismatch

In an attempt to provide an efficient method for line disturbance identification in complex networks of diffusively coupled agents, we recently proposed to leverage the frequency mismatch. The frequency mismatch filters out the intricate combination of interactions induced by the network structure and quantifies to what extent the trajectory of each agent is affected by the disturbance. In this previous work, we provided some analytical evidence of its efficiency when the perturbation is assumed to be slow. Here we claim that the frequency mismatch performs actually well for most disturbance regimes. This is shown through a series of simulations and is backed up by an analytical argument. Therefore, we argue that the frequency mismatch is an efficient and elegant tool for line disturbance location in complex networks of diffusively coupled agents.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2014

The spontaneous replication error and the mismatch discrimination mechanisms of human DNA polymerase β

To provide molecular-level insights into the spontaneous replication error and the mismatch discrimination mechanisms of human DNA polymerase β (polβ), we report four crystal structures of polβ complexed with dG•dTTP and dA•dCTP mismatches in the presence of Mg 2+ or Mn 2+ . The Mg 2+ -bound ground-state structures show that the dA•dCTP-Mg 2+ complex adopts an ‘intermediate’ protein conformation while the dG•dTTP-Mg 2+ complex adopts an open protein conformation. The Mn 2+ -bound ‘pre-chemistry-state’ structures show that the dA•dCTP-Mn2+ complex is structurally very similar to the dA•dCTP-Mg 2+ complex, whereas the dG•dTTP-Mn 2+ complex undergoes a large-scale conformational change to adopt a Watson–Crick-like dG•dTTP base pair and a closed protein conformation. These structural differences, together with our molecular dynamics simulation studies, suggest that polβ increases replication fidelity via a two-stage mismatch discrimination mechanism, where one is in the ground state and the other in the closed conformation state. In the closed conformation state, polβ appears to allow only a Watson–Crick-like conformation for purine•pyrimidine base pairs, thereby discriminating the mismatched base pairs based on their ability to form the Watson–Crick-like conformation. Overall, the present studies provide new insights into the spontaneous replication error and the replication fidelity mechanisms of polβ.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Enhanced spontaneous DNA twisting/bending fluctuations unveiled by fluorescence lifetime distributions promote mismatch recognition by the Rad4 nucleotide excision repair complex

Rad4/XPC recognizes diverse DNA lesions including ultraviolet-photolesions and carcinogen-DNA adducts, initiating nucleotide excision repair. Studies have suggested that Rad4/XPC senses lesion-induced helix-destabilization to flip out nucleotides from damaged DNA sites. However, characterizing how DNA deformability and/or distortions impact recognition has been challenging. Here, using fluorescence lifetime measurements empowered by a maximum entropy algorithm, we mapped the conformational heterogeneities of artificially destabilized mismatched DNA substrates of varying Rad4-binding specificities. The conformational distributions, as probed by FRET between a cytosine-analog pair exquisitely sensitive to DNA twisting/bending, reveal a direct connection between intrinsic DNA deformability and Rad4 recognition. High-specificity CCC/CCC mismatch, free in solution, sampled a strikingly broad range of conformations from B-DNA-like to highly distorted conformations that resembled those observed with Rad4 bound; the extent of these distortions increased with bound Rad4 and with temperature. Conversely, the non-specific TAT/TAT mismatch had a homogeneous, B-DNA-like conformation. Molecular dynamics simulations also revealed a wide distribution of conformations for CCC/CCC, complementing experimental findings. We propose that intrinsic deformability promotes Rad4 damage recognition, perhaps by stalling a diffusing protein and/or facilitating ‘conformational capture’ of pre-distorted damaged sites. Surprisingly, even mismatched DNA specifically bound to Rad4 remains highly dynamic, a feature that may reflect the versatility of Rad4/XPC to recognize many structurally dissimilar lesions

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2016

Optical CT imaging of solid radiochromic dosimeters in mismatched refractive index solutions using a scanning laser and large area detector

Purpose: The practical use of the PRESAGE® solid plastic dosimeter is limited by the inconvenience of immersing it in high-viscosity oils to achieve refractive index matching for optical computed tomography (CT) scanning. The oils are slow to mix and difficult to clean from surfaces, and the dosimeter rotation can generate dynamic Schlieren inhomogeneity patterns in the reference liquid, limiting the rotational and overall scan speed. Therefore, it would be beneficial if lower-viscosity, water-based solutions with slightly unmatched refractive index could be used instead. The purpose of this work is to demonstrate the feasibility of allowing mismatched conditions when using a scanning laser system with a large acceptance angle detector. A fiducial-based ray path measurement technique is combined with an iterative CT reconstruction algorithm to reconstruct images. Methods: A water based surrounding liquid with a low viscosity was selected for imaging PRESAGE® solid dosimeters. Liquid selection was optimized to achieve as high a refractive index as possible while avoiding rotation-induced Schlieren effects. This led to a refractive index mismatch of 6% between liquid and dosimeters. Optical CT scans were performed with a fan-beam scanning-laser optical CT system with a large area detector to capture most of the refracted rays. A fiducial marker placed on the wall of a cylindrical sample occludes a given light ray twice. With knowledge of the rotation angle and the radius of the cylindrical object, the actual internal path of each ray through the dosimeter can be calculated. Scans were performed with 1024 projections of 512 data samples each, and rays were rebinned to form 512 parallel-beam projections. Reconstructions were performed on a 512 × 512 grid using 100 iterations of the SIRT iterative CT algorithm. Proof of concept was demonstrated with a uniformly attenuating solution phantom. PRESAGE® dosimeters (11 cm diameter) were irradiated with Cobalt-60 irradiator to achieve either a uniform dose or a 2-level “step-dose” pattern. Results: With 6% refractive index mismatching, a circular field of view of 85% of the diameter of a cylindrical sample can be reconstructed accurately. Reconstructed images of the test solution phantom were uniform (within 3%) inside this radius. However, the dose responses of the PRESAGE® samples were not spatially uniform, with variations of at least 5% in sensitivity. The variation appears as a “cupping” artifact with less sensitivity in the middle than at the periphery of the PRESAGE® cylinder. Polarization effects were also detected for these samples. Conclusions: The fiducial-based ray path measurement scheme, coupled with an iterative reconstruction algorithm, enabled optical CT scanning of PRESAGE® dosimeters immersed in mismatched refractive index solutions. However, improvements to PRESAGE® dose response uniformity are required.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

Measures of illuminant-induced metameric mismatch: theory, comparative analysis, and implications for application

Illuminant-induced metameric mismatch is an important consideration in the specification of light sources for some architectural environments, yet there is currently no standardized performance measure. The goal of this work was to evaluate two recent research proposals: the metameric uncertainty index ( R t ) and the metamer mismatching color rendering index (MMCRI). To compare the relative performance of these two measures, 100,000 spectral power distributions were generated with 3, 4, 5, 6, and 7 Gaussian spectral components and spectral widths varying from 1 nm (monochromatic) to 100 nm. Both measures generally agree with the theory that broadband radiation should cause less metameric mismatch than narrowband radiation. The two measures have relatively better agreement for broadband SPDs and relatively worse agreement for narrower spectra. Despite some similarities, non-parametric statistical tests suggest that R t and MMCRI are significantly different quantifications of illuminant-induced metameric mismatch ( p < 0.0001 for all comparisons). Characteristics of the MMCRI computation that are potentially problematic for applied lighting were observed.

42 ENGINEERING↗

NASA NTRS1993

Radio metric errors due to mismatch and offset between a DSN antenna beam and the beam of a troposphere calibration instrument

Two components of the error of a troposphere calibration measurement were quantified by theoretical calculations. The first component is a beam mismatch error, which occurs when the calibration instrument senses a conical volume different from the cylindrical volume sampled by a Deep Space Network (DSN) antenna. The second component is a beam offset error, which occurs if the calibration instrument is not mounted on the axis of the DSN antenna. These two error sources were calculated for both delay (e.g., VLBI) and delay rate (e.g., Doppler) measurements. The beam mismatch error for both delay and delay rate drops rapidly as the beamwidth of the troposphere calibration instrument (e.g., a water vapor radiometer or an infrared Fourier transform spectrometer) is reduced. At a 10-deg elevation angle, the instantaneous beam mismatch error is 1.0 mm for a 6-deg beamwidth and 0.09 mm for a 0.5-deg beam (these are the full angular widths of a circular beam with uniform gain out to a sharp cutoff). Time averaging for 60-100 sec will reduce these errors by factors of 1.2-2.2. At a 20-deg elevation angle, the lower limit for current Doppler observations, the beam-mismatch delay rate error is an Allan standard deviation over 100 sec of 1.1 x 10(exp -14) with a 4-deg beam and 1.3 x 10(exp -l5) for a 0.5-deg beam. A 50-m beam offset would result in a fairly modest (compared to other expected error sources) delay error (less than or equal to 0.3 mm for 60-sec integrations at any elevation angle is greater than or equal to 6 deg). However, the same offset would cause a large error in delay rate measurements (e.g., an Allan standard deviation of 1.2 x 10(exp -14) over 100 sec at a 20-deg elevation angle), which would dominate over other known error sources if the beamwidth is 2 deg or smaller. An on-axis location is essential for accurate troposphere calibration of delay rate measurements. A half-power beamwidth (for a beam with a tapered gain profile) of 1.2 deg or smaller is desired for calibration of all types of radio metrics. A water-vapor radiometer calibration beam of this size with very low sidelobes would require a clear aperture antenna with a diameter of at least 1.5 m if the primary water vapor sensing channel were in the 20-22 GHz range.

R P Linfield↗

NASA NTRS2009

A Direct Adaptive Control Approach in the Presence of Model Mismatch

This paper considers the problem of direct model reference adaptive control when the plant-model matching conditions are violated due to abnormal changes in the plant or incorrect knowledge of the plant's mathematical structure. The approach consists of direct adaptation of state feedback gains for state tracking, and simultaneous estimation of the plant-model mismatch. Because of the mismatch, the plant can no longer track the state of the original reference model, but may be able to track a new reference model that still provides satisfactory performance. The reference model is updated if the estimated plant-model mismatch exceeds a bound that is determined via robust stability and/or performance criteria. The resulting controller is a hybrid direct-indirect adaptive controller that offers asymptotic state tracking in the presence of plant-model mismatch as well as parameter deviations.

Joshi, Suresh M.↗

NASA NTRS2011

Decentralized Adaptive Control of Systems with Uncertain Interconnections, Plant-Model Mismatch and Actuator Failures

Decentralized adaptive control is considered for systems consisting of multiple interconnected subsystems. It is assumed that each subsystem s parameters are uncertain and the interconnection parameters are not known. In addition, mismatch can exist between each subsystem and its reference model. A strictly decentralized adaptive control scheme is developed, wherein each subsystem has access only to its own state but has the knowledge of all reference model states. The mismatch is estimated online for each subsystem and the mismatch estimates are used to adaptively modify the corresponding reference models. The adaptive control scheme is extended to the case with actuator failures in addition to mismatch.

Patre, Parag↗