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At least 307 records · Page 17

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DOE OSTI2026

Pseudo–Jahn–Teller Distortion in a One-Dimensional π-Conjugated Polymer

Structural distortions in low-dimensional π-conjugated systems profoundly influence their electronic properties, but the control of such behavior in laterally extended systems remains challenging. Here, in this study, we demonstrate that a one-dimensional conjugated polymer─ poly -(difluorenoheptalene-ethynylene) (PDFHE)─undergoes a pronounced out-of-plane backbone distortion, equivalent to a spontaneous symmetry breaking (SSB) of its mirror symmetry. We synthesized PDFHE on noble metal surfaces and characterized its structure and electronic states using low-temperature scanning tunneling microscopy (STM). Rather than adopting a planar, high-symmetry conformation, PDFHE relaxes into nonplanar isomers stabilized by a pseudo–Jahn–Teller (PJT) distortion having mirror-odd out-of-plane character. The distortion lowers the total energy and increases the band gap, providing a concise rationale for the observed symmetry breaking. Density functional theory calculations corroborate these findings, providing a microscopic explanation for the SSB. Our results show that even in mechanically robust extended π-systems, subtle electron–lattice coupling can spontaneously drive significant structural rearrangements, even in mechanically robust extended π-systems.

conformation↗

NASA NTRS1985

Extended atmospheres of outer planet satellites and comets

Collisions between neutral hydrogen atoms in the interstellar medium and those in the so-called Titan hydrogen torus may provide an additional lifetime sink for atoms in the Saturn environment. Progress toward re-sorting the Voyager UVS scans of neutral hydrogen in the Saturn system to enable both a factor of two increase in the amount of data to be analyzed as well as to help identify near-Titan hydrogen is discussed. Progress toward development of the cometary carbon and oxygen models is also discussed and a preliminary model run for the H2O source of cometary oxygen is presented.

Smyth, W. H.↗

NASA NTRS1975

Ecology and Thermal Inactivation of Microbes in and on Interplanetary Space Vehicle Components

Spores of Bacillus subtilis var. niger were heat treated in aqueous suspension at 90 C, and observed for morphological changes and loss of viability. The 5 logs reduction that occurred in broth at 90 min required 210 min in buffered water. Five characteristic changes observed after spores were exposed 120 min at 90 C in buffered water were: (1) 90% loss of spore viability, (2) 5% stainability, (3) 76% increase in spore size (as observed by scanning electron microscopy), (4) 21% of spore areas remaining refractile, and (5) an increase of 77% in packed cell volume (PCV). Stainability and PCV changes were recognized only after secondary exposure in broth. Extended heat exposure (3 h at 90 C) resulted in 99% loss of spore viability and 99% loss of stainability. After 4 hours of heat exposure, 90% of the cells disintegrated. These results suggest that early germinal changes occurr concurrently with the early changes in the heat susceptibility of dormant spores.

Reyes, A. L.↗

NASA NTRS2012

High Resolution Observations of Drop Size Distribution for GPM Ground Validation

During the Mid-latitude Continental Convective Cloud Experiment (MC3E), NASA's GPM GV Disdrometer and Radar Observations of Precipitation (DROP) Facility deployed an array of disdrometers and rain gauges in northern Oklahoma to sample, with high resolution, the drop size distribution for use in development of precipitation retrieval algorithms for the GPM core satellites. The DROP Facility instruments deployed during MC3E consisted of 16 autonomous Parsivel units, 5 two-dimensional video disdrometers (2dvds), a vertically pointing K band radar, and 32 tipping bucket rain gauges. There were several rainfall events during MC3E in which rain drops exceeding 6 mm in diameter were recorded. The disdrometer array revealed large rain drops with diameters exceeding 6 mm and 8 mm during two separate stratiform and convective rainfall events, respectively. The NPOL radar, which was scanning in high resolution RHI mode (every 40 sec) over the disdrometer array during the stratiform event, indicated a 1 km thick bright band with a differential reflectivity column of 2-3 dB extending below the melting layer to the surface where the large drops were recorded by the 2dvds. These large drops are important for GPM since they can have a great impact upon satellite precipitation retrieval, especially near the ground and below heavy convective rainfall cores where satellites have had problems depicting the rainfall.

Gatlin, Patrick N.↗

DOE OSTI2023

Pulsed Laser Annealed Ga Hyperdoped Poly‐Si / SiO x Passivating Contacts for High‐Efficiency Monocrystalline Si Solar Cells

Polycrystalline Si ( poly ‐Si)‐based passivating contacts are promising candidates for high‐efficiency crystalline Si solar cells. We show that nanosecond‐scale pulsed laser melting (PLM) is an industrially viable technique to fabricate such contacts with precisely controlled dopant concentration profiles that exceed the solid solubility limit. We demonstrate that conventionally doped, hole‐selective poly ‐Si/SiO x contacts that provide poor surface passivation of c ‐Si can be replaced with Ga‐ or B‐doped contacts based on non‐equilibrium doping. We overcome the solid solubility limit for both dopants in poly ‐Si by rapid cooling and recrystallization over a timescale of ∼25 ns. We show an active Ga dopant concentration of ∼3 × 10 20 cm −3 in poly ‐Si which is six times higher than its solubility limit in c ‐Si, and a B dopant concentration as high as ∼10 21 cm −3 . We measure an implied open‐circuit voltage of 735 mV for Ga‐doped poly ‐Si/SiO x contacts on Czochralski Si with a low contact resistivity of 35.5 ± 2.4 mΩ cm 2 . Scanning spreading resistance microscopy and Kelvin probe force microscopy show large diffusion and drift current in the p ‐ n junction that contributes to the low contact resistivity. Our results suggest that PLM can be extended for hyperdoping of other semiconductors with low solubility atoms to enable high‐efficiency devices.

14 SOLAR ENERGY↗

DOE OSTI2025

Morphological Characterization of Uranyl Fluoride Particles via Atomic Force Microscopy

Uranium hexafluoride (UF 6 ) undergoes a rapid hydrolysis reaction when exposed to atmospheric water. In addition to producing hazardous HF gas, the hydrolysis reaction produces uranyl fluoride (UO 2 F 2 ), a radioactive solid phase particulate material. Because of the technological utility of UF 6 in the nuclear fuel cycle, understanding the transport properties of UO 2 F 2 aerosol produced via UF 6 hydrolysis is important for accident scenarios. Moreover, the fundamental chemical and physical properties of the UF 6 hydrolysis reaction are not completely understood. Recently, several experiments on the aerosol phase properties of UO 2 F 2 produced in this way have shown that under most relevant conditions, the particle size distribution (PSD) of UO 2 F 2 can be extremely small, approximately 3 to 5 nm, which is well below the threshold that can be routinely observed via scanning electron microscopy (SEM). Although readily observable in the aerosol phase, observation of nanometer-sized particles in the condensed phase (i.e. deposited on surfaces) remains a challenge. Here, in this study, we have used atomic force microscopy (AFM) to study the PSD and morphological characteristics of UO 2 F 2 deposited at low and high concentrations under different humidity conditions, a primary variable in the hydrolysis reaction. Here, we find strong agreement between PSD measured in the aerosol phase via scanning mobility particle sizing and PSD measured via AFM, with particle sizes peaked below 4 nm for low-humidity conditions. At higher humidity, the distribution is centered around 5 to 10 nm but extends up to 20 nm. These results are in stark contrast to previous measurements using SEM that show PSD on the order of 300- to 1000-nm particle sizes; moreover, these are the first direct measurements of individual particles of UO 2 F 2 having been produced via UF 6 hydrolysis deposited on surfaces. These measurements, therefore, open a new avenue for collecting and detecting UO 2 F 2 in the condensed phase and further refine the PSD, which is critical for environmental transport determinations.

Uranium hexafluoride↗

DOE OSTI2021

Stabilizing the heavily-doped and metallic phase of MoS 2 monolayers with surface functionalization

Monolayer molybdenum disulfide (MoS 2 ) is one of the most studied two-dimensional (2D) transition metal dichalcogenides that is being investigated for various optoelectronic properties, such as catalysis, sensors, photovoltaics, and batteries. One such property that makes this material attractive is the ease in which 2D MoS 2 can be converted between the semiconducting (2H) and metallic/semi-metallic (1T/1T') phases or heavily n-type doped 2H phase with ion intercalation, strain, or excess negative charge. Using n-butyl lithium (BuLi) immersion treatments, we achieve 2H MoS 2 monolayers that are heavily n-type doped with shorter immersion times (10–120 mins) or conversion to the 1T/1T' phase with longer immersion times (6–24 h); however, these doped/converted monolayers are not stable and promptly revert back to the initial 2H phase upon exposure to air. To overcome this issue and maintain the modification of the monolayer MoS 2 upon air exposure, we use BuLi treatments plus surface functionalization p-(CH 3 CH 2 ) 2 NPh-MoS 2 (Et 2 N-MoS 2 )—to maintain heavily n-type doped 2H phase or the 1T/1T' phase, which is preserved for over two weeks when on indium tin oxide or sapphire substrates. We also determine that the low sheet resistance and metallic-like properties correlate with the BuLi immersion times. These modified MoS 2 materials are characterized with confocal Raman/photoluminescence, absorption, x-ray photoelectron spectroscopy as well as scanning Kelvin probe microscopy, scanning electrochemical microscopy, and four-point probe sheet resistance measurements to quantify the differences in the monolayer optoelectronic properties. We will demonstrate chemical methodologies to control the modified monolayer MoS 2 that likely extend to other 2D transition metal dichalcogenides, which will greatly expand the uses for these nanomaterials.

2D TMDC↗

DOE OSTI2023

Hard x-ray – optical four-wave mixing using a split-and-delay line

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray, x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

A robust clustering algorithm for analysis of composition-dependent organic aerosol thermal desorption measurements

Abstract. One of the challenges of understanding atmospheric organic aerosol (OA) particles stems from its complex composition. Mass spectrometry is commonly used to characterize the compositional variability of OA. Clustering of a mass spectral dataset helps identify components that exhibit similar behavior or have similar properties, facilitating understanding of sources and processes that govern compositional variability. Here, we developed an algorithm for clustering mass spectra, the noise-sorted scanning clustering (NSSC), appropriate for application to thermal desorption measurements of collected OA particles from the Filter Inlet for Gases and AEROsols coupled to a chemical ionization mass spectrometer (FIGAERO-CIMS). NSSC, which extends the common density-based special clustering of applications with noise (DBSCAN) algorithm, provides a robust, reproducible analysis of the FIGAERO temperature-dependent mass spectral data. The NSSC allows for the determination of thermal profiles for compositionally distinct clusters of mass spectra, increasing the accessibility and enhancing the interpretation of FIGAERO data. Applications of NSSC to several laboratory biogenic secondary organic aerosol (BSOA) systems demonstrate the ability of NSSC to distinguish different types of thermal behaviors for the components comprising the particles along with the relative mass contributions and chemical properties (e.g., average molecular formula) of each mass spectral cluster. For each of the systems examined, more than 80 % of the total mass is clustered into 9–13 mass spectral clusters. Comparison of the average thermograms of the mass spectral clusters between systems indicates some commonality in terms of the thermal properties of different BSOA, although with some system-specific behavior. Application of NSSC to sets of experiments in which one experimental parameter, such as the concentration of NO, is varied demonstrates the potential for mass spectral clustering to elucidate the chemical factors that drive changes in the thermal properties of OA particles. Further quantitative interpretation of the thermograms of the mass spectral clusters will allow for a more comprehensive understanding of the thermochemical properties of OA particles.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1975

Scanning electron microscopy of a pink inclusion from the Allende meteorite

A scanning electron microscope study of a fine-grained, pin, Ca-rich inclusion from the Allende meteorite has revealed strong evidence for direct condensation of its constituent minerals from a vapor. This observation extends to the alkali-bearing phases in addition to the Ca-, Al-silicates and suggests that the feldspathoids as well as the refractory silicates are solar nebular condensates.

Grossman, L.↗

NASA NTRS1976

Spectroscopic photoelectric imaging Fabry-Perot interferometer - Its development and preliminary observational results

In order to observe extended astronomical objects at high spatial and spectral resolution, we have constructed a spectroscopic photoelectric imaging Fabry-Perot interferometer (SPIFI). Among the properties chosen for the instrument are an air-spaced, piezoelectrically scanned design allowing an accurately settable free spectral range and employing a single etalon of high finesse. Careful design of the etalon mountings and optical train preserves high light throughput. We either obtain spectra of single spatial elements with a photomultiplier or use an SEC vidicon detector to record a series of images through the interferometer while scanning the wavelength in discrete steps. The latter procedure yields sufficient information to reconstruct spectral features over the entire object. For the conditions assumed, either series of observations requires only a small fraction of a rotational period for Jupiter or Saturn, for example.

Smith, W. H.↗

NASA NTRS1979

An efficient technique for the computation of vector secondary patterns of offset paraboloid reflectors

A series approach for the rapid computation of the vector secondary pattern of offset paraboloid reflectors wherein the feed is displaced is presented. We show that the Jacobi polynomial series method, which has been demonstrated to provide an efficient means for evaluating the radiation integral of symmetric paraboloid reflectors, can be extended to the case of an offset paraboloid without compromising the ease or speed of computation. The analysis leading to the series formula is also useful for deriving an analytic expression for the optimum scan plane for the displacement of the feed. Representative numerical results illustrating the application of the method and the properties of the offset paraboloid are presented.

Mittra, R.↗

NASA NTRS1983

Infrared properties of extragalactic H II complexes

Infrared observations of relatively isolated giant H II complexes in the LMC and the spiral arms of M33 and M101 are discussed, and complexes which extend over several kiloparsecs near the galactic centers are examined. The 30 Doradus nebula is emphasized, showing the variation of the 50-100 micron color temperature with position in that object. Ten-micron scans through the nucleus of NGC 1097 are compared to a visual photograph, showing the enhanced infrared emission which occurs at the nucleus and at the ring of H II regions about 1 kpc from the nucleus.

Telesco, C. M.↗

NASA NTRS1986

IRAS surface brightness maps of visible reflection nebulae: Evidence for non-equilibrium infrared emission

Surface brightness maps at 12, 25, 60, and 100 microns of 16 visible reflection nebulae were extracted from the Infrared Astronomy Satellite (IRAS) database. The maps were produced by coadding IRAS survey scans over areas centered on the illuminating stars, and have spatial resolutions of 0.9' x 4' at 12 and 25 microns, 1.8' x 4.5' at 60 microns, and 3.6' x 5' at 100 microns. Extended emission in the four IRAS bandpasses was detected in fourteen of the reflection nebulae. The IRAS data were used to measure the flux of the infrared emission associated with each source. The energy distributions show that the 12 micron flux is greater than the 25 micron flux in 11 of the nebulae, and the peak flux occurs in the 60 or 100 micron bandpass in all 16 nebular. The 60 and 100 micron flux can be approximated by blackbodies with temperatures between 30 and 50 K, consistent with temperatures expected from extrapolation of greybody fits to the 60 and 100 micron data. The excess 12 and 25 micron emission is attributed to a nonequilibrium process such as emission from thermal fluctuations of very small grains excited by single ultraviolet photons, or emission from polycyclic aromatic hydrocarbons (PAHs) excited by ultraviolet radiation. The common features of the energy distributions of the 16 reflection nebulae, also seen in the reflection nebulae associated with the Pleiades, suggest that PAHs or very small grains may be found in most reflection nebulae.

Castelaz, M. W.↗

DOE OSTI2023

Hollow Ptychography: Toward Simultaneous 4D Scanning Transmission Electron Microscopy and Electron Energy Loss Spectroscopy

With the recent development of high-acquisition-speed pixelated detectors, 4D scanning transmission electron microscopy (4D-STEM) is becoming routinely available in high-resolution electron microscopy. 4D-STEM acts as a “universal” method that provides local information on materials that is challenging to extract from bulk techniques. It extends conventional STEM imaging to include super-resolution techniques and to provide quantitative phase-based information, such as differential phase contrast, ptychography, or Bloch wave phase retrieval. However, an important missing factor is the chemical and bonding information provided by electron energy loss spectroscopy (EELS). 4D-STEM and EELS cannot currently be acquired simultaneously due to the overlapping geometry of the detectors. Here, the feasibility of modifying the detector geometry to overcome this challenge for bulk specimens is demonstrated, and the use of a partial or defective detector for ptycholgaphic structural imaging is explored. Here, results show that structural information beyond the diffraction-limit and chemical information from the material can be extracted together, resulting in simultaneous multi-modal measurements, adding the additional dimensions of spectral information to 4D datasets.

4D-scanning transmitting electron microscopy (STEM↗

NASA NTRS2020

Terra MODIS: 20 years of on-orbit calibration and performance

Since its launch in December 1999, Terra Moderate Resolution Imaging Spectroradiometer (MODIS) has successfully operated for more than 20 years, with its observations generating a broad range of science data products that have greatly enabled the remote sensing community and users worldwide in their studies of many key geophysical parameters of the Earth’s systems. MODIS collects data in 36 spectral bands, covering wavelengths from 0.41 to 14.4 μm, which are calibrated by a set of onboard calibrators (OBCs). Also contributing to the sensor’s mission-long on-orbit calibration and characterization are near-monthly scheduled lunar observations and multiple time series of the sensor’s responses over select ground targets at a variety of scan angles. To a large extent, the quality of MODIS data products relies strongly on the dedicated efforts to operate and calibrate the instrument, to derive and update calibration parameters, and to develop and implement new calibration strategies and algorithms in response to on-orbit changes of the sensor’s characteristics and its OBC functions. We provide an overview of the Terra MODIS on-orbit operation and calibration activities over the last 20 years, including changes made to extend and preserve the instrument and OBC functions and their operation strategies. It also illustrates the sensor’s on-orbit performance with results derived from its OBC, lunar observations, and select ground targets and discusses major changes in sensor characteristics and corrections applied to the L1B algorithms as well as calibration lookup table updates. To date, the Terra MODIS instrument and its OBCs continue to operate and function normally. Except for those identified prelaunch, most spectral bands and detectors continue to meet their specified calibration requirements. Also discussed in our paper are lessons learned from Terra MODIS operation and calibration, as well as future efforts to further extend and maintain the quality of its long-term data records.

Terra↗

DOE OSTI2025

Energetic and structural control of polyspecificity in a multidrug transporter

Multidrug efflux pumps are dynamic molecular machines that drive antibiotic resistance by harnessing ion gradients to export chemically diverse substrates. Despite their clinical importance, the molecular principles underlying multidrug promiscuity and energy efficiency remain poorly understood. Using multiparametric deep mutational scanning across eight substrates and two energy conditions, we deconvolute the contributions of substrate recognition, energetic coupling, and protein stability, providing an integrated, high-resolution view of multidrug transport. We find that substrate specificity arises from a distributed network of residues extending beyond the binding site, with mutations that reshape binding, coupling, conformational flexibility, and membrane interactions. Further, we apply a pH-based selection scheme to measure the effect of mutation on pH-dependent transport efficiency. By integrating these data, we reveal a fundamental relationship between efficiency and promiscuity: Highly efficient variants exhibit broad substrate profiles, while inefficient variants are narrower. In conclusion, these findings establish a direct link between energy coupling and polyspecificity, uncovering the biochemical logic underlying multidrug transport.

Biological Sciences↗

DOE OSTI2022

Towards automating structural discovery in scanning transmission electron microscopy *

Abstract Scanning transmission electron microscopy is now the primary tool for exploring functional materials on the atomic level. Often, features of interest are highly localized in specific regions in the material, such as ferroelectric domain walls, extended defects, or second phase inclusions. Selecting regions to image for structural and chemical discovery via atomically resolved imaging has traditionally proceeded via human operators making semi-informed judgements on sampling locations and parameters. Recent efforts at automation for structural and physical discovery have pointed towards the use of ‘active learning’ methods that utilize Bayesian optimization with surrogate models to quickly find relevant regions of interest. Yet despite the potential importance of this direction, there is a general lack of certainty in selecting relevant control algorithms and how to balance a priori knowledge of the material system with knowledge derived during experimentation. Here we address this gap by developing the automated experiment workflows with several combinations to both illustrate the effects of these choices and demonstrate the tradeoffs associated with each in terms of accuracy, robustness, and susceptibility to hyperparameters for structural discovery. We discuss possible methods to build descriptors using the raw image data and deep learning based semantic segmentation, as well as the implementation of variational autoencoder based representation. Furthermore, each workflow is applied to a range of feature sizes including NiO pillars within a La:SrMnO 3 matrix, ferroelectric domains in BiFeO 3 , and topological defects in graphene. The code developed in this manuscript is open sourced and will be released at github.com/nccreang/AE_Workflows .

47 OTHER INSTRUMENTATION↗