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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Quantum Emitter Formation Dynamics and Probing of Radiation-Induced Atomic Disorder in Silicon

Near-infrared color centers in silicon are emerging candidates for on-chip integrated quantum emitters, optical-access quantum memories, and sensing. We access ensemble G-color-center formation dynamics and radiation-induced atomic disorder in silicon for a series of megaelectronvolt proton-flux conditions. The photoluminescence results reveal that the G centers are formed more efficiently by pulsed-proton irradiation than by continuous-wave proton irradiation. The enhanced transient excitations and dynamic annealing within nanoseconds allows optimization of the ratio of G-center formation to nonradiative defect accumulation. The G centers preserve narrow line widths of about 0.1 nm when they are generated by moderate pulsed-proton fluences, while the line width broadens significantly as the pulsed-proton fluence increases. This implies vacancy or interstitial clustering by overlapping collision cascades. The tracking of G-center properties for a series of irradiation conditions enables sensitive probing of atomic disorder, serving as a complementary analytical method for sensing damage accumulation. Aided by ab initio electronic structure calculations, we provide insight into the atomic disorder induced inhomogeneous broadening by introducing vacancies, silicon interstitials, and oriented strain fields in the vicinity of a G center. A vacancy leads to a tensile strain and can result in either a red shift or a blue shift of the G-center emission, depending on its position relative to the G center. Meanwhile, Si interstitials lead to compressive strain, which results in a monotonic red shift. In conclusion, high-flux and tunable ion pulses enable the exploration of the fundamental dynamics of radiation-induced defects as well as methods for the optimization of G-center formation and qubit synthesis for quantum information processing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Cation and Anion Channelrhodopsins: Sequence Motifs and Taxonomic Distribution

Cation and anion channelrhodopsins (CCRs and ACRs, respectively) primarily from two algal species, Chlamydomonas reinhardtii and Guillardia theta, have become widely used as optogenetic tools to control cell membrane potential with light. We mined algal and other protist polynucleotide sequencing projects and metagenomic samples to identify 75 channelrhodopsin homologs from four channelrhodopsin families, including one revealed in dinoflagellates in this study. We carried out electrophysiological analysis of 33 natural channelrhodopsin variants from different phylogenetic lineages and 10 metagenomic homologs in search of sequence determinants of ion selectivity, photocurrent desensitization, and spectral tuning in channelrhodopsins. Our results show that association of a reduced number of glutamates near the conductance path with anion selectivity depends on a wider protein context, because prasinophyte homologs with a glutamate pattern identical to that in cryptophyte ACRs are cation selective. Desensitization is also broadly context dependent, as in one branch of stramenopile ACRs and their metagenomic homologs, its extent roughly correlates with phylogenetic relationship of their sequences. Regarding spectral tuning, we identified two prasinophyte CCRs with red-shifted spectra to 585 nm. They exhibit a third residue pattern in their retinal-binding pockets distinctly different from those of the only two types of red-shifted channelrhodopsins known (i.e., the CCR Chrimson and RubyACRs). In cryptophyte ACRs we identified three specific residue positions in the retinal-binding pocket that define the wavelength of their spectral maxima. Lastly, we found that dinoflagellate rhodopsins with a TCP motif in the third transmembrane helix and a metagenomic homolog exhibit channel activity. Channelrhodopsins are widely used in neuroscience and cardiology as research tools and are considered prospective therapeutics, but their natural diversity and mechanisms remain poorly characterized. Genomic and metagenomic sequencing projects are producing an ever-increasing wealth of data, whereas biophysical characterization of the encoded proteins lags behind. In this study, we used manual and automated patch clamp recording of representative members of four channelrhodopsin families, including a family in dinoflagellates that we report in this study. Our results contribute to a better understanding of molecular determinants of ionic selectivity, photocurrent desensitization, and spectral tuning in channelrhodopsins.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Structure of the antenna complex expressed during far-red light photoacclimation in Synechococcus sp. PCC 7335

Far-red light photoacclimation, or FaRLiP, is a facultative response exhibited by some cyanobacteria that allows them to absorb and utilize lower energy light (700–800 nm) than the wavelengths typically used for oxygenic photosynthesis (400–700 nm). During this process, three essential components of the photosynthetic apparatus are altered: photosystem I, photosystem II, and the phycobilisome. In all three cases, at least some of the chromophores found in these pigment–protein complexes are replaced by chromophores that have red-shifted absorbance relative to the analogous complexes produced in visible light. Recent structural and spectroscopic studies have elucidated important features of the two photosystems when altered to absorb and utilize far-red light, but much less is understood about the modified phycobiliproteins made during FaRLiP. We used single-particle, cryo-EM to determine the molecular structure of a phycobiliprotein core complex comprising allophycocyanin variants that absorb far-red light during FaRLiP in the marine cyanobacterium Synechococcus sp. PCC 7335. The structure reveals the arrangement of the numerous red-shifted allophycocyanin variants and the probable locations of the chromophores that serve as the terminal emitters in this complex. It also suggests how energy is transferred to the photosystem II complexes produced during FaRLiP. The structure additionally allows comparisons with other previously studied allophycocyanins to gain insights into how phycocyanobilin chromophores can be tuned to absorb far-red light. These studies provide new insights into how far-red light is harvested and utilized during FaRLiP, a widespread cyanobacterial photoacclimation mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1978

Interpretation of observed cosmic microwave background radiation

The Alfven and Mendis (1977) conclusion that dust grains in galaxies render the universe opaque to cosmic microwave background at a red shift ratio equal to 40 is challenged by a calculation of the opacity of galactic dust grains to the microwave background radiation from the time of decoupling at emission red shift ratio equal to 1500 to the present in the standard big bang model. In the present calculation, evolutionary effects on grain opacity and abundance are estimated. At wavelengths used in studying the microwave background, the optical depth of the grains is found to be 0.18 when the deceleration parameter equals 0.03, and 0.05 when the deceleration parameter equals 0.5. The results indicate that microwave background can provide information on an early dense phase of the universe.

Pollaine, S.↗
NASA NTRS1984

Quasars as probes of the intergalactic medium

Spectral energy distributions for 10 high red shift quasars in the wavelength range 1250 to 10,000 A were obtained by IUE. A pronounced steepening is detected shortward of 1200 A, which correlates well with quasar red shift, but poorly with luminosity. The observed slope change is explained by Lyman continuum absorption from the strongest 5% of the Lyman alpha forest lines, identified with the low column density metal containing systems. Reddening may also contribute to the steepening, but a much lower neutral gas to dust ratio than that found in the Galaxy is required. Optically thick Lyman limit discontinuities are seen with zabs zem. These systems are metal containing, constant in comoving density with epoch, and require in L* galaxy to have a cross section of 5 to 10 Holmberg radii.

Green, R. F.↗
DOE OSTI2018

Supramolecular self-assembly of bacteriochlorophyll c molecules in aerosolized droplets to synthesize biomimetic chlorosomes

The unique properties of chlorosomes, arising out of the self-assembled bateriochlorophyll (BChl) c structure, have made them attractive for use in solar cells. In this work, we have demonstrated the self-assembly of BChl c in aerosolized droplets to mimic naturally occurring chlorosomes. We compare two different methods for self-assembly of BChl c , one using a single-solvent and the other using two-solvents, and demonstrate the superiority of the two-solvent method. Results show that the self-assembled BChl c sprayed at different concentrations resulted in a varying red shift of 69-75 nm in absorption spectrum compared to the solution, which has peak at 668 nm corresponding to the monomeric BChl c . The sample fluoresces at 780 nm indicating a quality of self-assembly comparable to that observed in naturally occurring chlorosomes. In order to mimic chlorosomes, solution containing BChl c , BChl a, lipids and carotenes in same proportion as in chlorosomes is sprayed. The resulting self-assembly has an absorption peak at 750 nm, shifted by 82 nm compared to that of monomers and the fluorescence peak at 790 nm. Thus in presence of lipids and carotenes, both the absorption and fluorescence peaks are red shifted. Further, using grazing incidence small angle X-ray scattering (GISAXS), we characterized the deposited films, and the 2D X-ray scattering patterns of sample clearly indicate the distinct lamellar structure as present in chlorosomes. Here, the results of this work provide new insights into self-assembly in aerosolized droplets, which can be used for assembling a wide range of molecules.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Amorphous Ag 2-x Cu x S quantum dots: “all-in-one” theranostic nanomedicines for near-infrared fluorescence/photoacoustics dual-modal-imaging-guided photothermal therapy

Integrating dual-modal imaging and photothermal effect within a single nanosystem is an enormous challenge for current nanomedicine application. In this study, non-toxic amorphous Ag 2-x Cu x S quantum dots (QDs) possessing near-infrared fluorescence (NIRF), enhanced photothermal and photoacoustic (PA) performance, as “one-in-all” nanomedicines, are designed and obtained. Cu doping in amorphous Ag 2 S QDs causes red-shift of NIRF to the lowest tissue absorption wavelength in so called “first biowindow” (~820 nm) and improves photothermal conversion efficiency to 44.0% simultaneously. Density functional theory simulation results suggest the fluorescence red-shift and enhanced photothermal/photoacoustics properties can be attributed to the generation of intragap states introduced by Cu doping. The amorphous Ag 2-x Cu x S QDs exhibit high long-term biocompatibility. Under a single laser irradiation with relatively low power density, an effective tumor ablation induced by high photothermal effect of amorphous Ag 2-x Cu x S QDs is achieved in vivo. Simultaneously, the PTT process can be guided by high quality NIRF/PA dual-modal-imaging.

36 MATERIALS SCIENCE↗
NASA NTRS1972

Position annihilation radiation from neutron stars

Matter accreted on the surfaces of neutron stars consists of energetic particles of a few tens to a couple hundred MeV/nucleon, depending on the neutron star mass. In addition to heat, such particles produce nuclear reactions with the surface material. It is proposed that the recently observed 473 + or - 30 keV spectral feature from the galactic center is gravitationally red-shifted positron annihilation radiation produced at the surfaces of old neutron stars. The principal observational tests of the model would be the detection of nuclear gamma ray lines from the galactic center and red-shifted positron annihilation radiation from the galactic disk.

Ramaty, R.↗
NASA NTRS1986

X-ray studies of Seyfert galaxies and quasars

Einstein X-ray observations of optically selected radio-quiet quasars are presented (summarizing the report of Kriss and Canizares, 1985) and analyzed along with published data. The data set comprises 77 quasars (including nine new high-red-shift quasars) and Seyferts and 101 upper limits. The ratio of X-ray to optical luminosity in the quasars is found to decrease as optical luminosity increases and to depend only weakly on red shift, and statistical discrepancies between the optically selected sample and the X-ray-selected Medium Sensitivity Survey (Gioia et al., 1984) are discussed. Also included are analyses of X-ray spectra and short-timescale variability for 64 Seyfert galaxies: variability is detected in IIIZw2, Mkn 766, and Mkn 78.

Canizares, Claude R.↗
DOE OSTI2025

Spectroscopic Identification of Carbamate Formation and Synergistic Binding in Amide–CO$^{–}_{2}$ Complexes

Carbamate formation is an elementary step that governs nitrogencentered nucleophilic CO 2 capture across diverse environments, yet a direct, structure-specific understanding has been lacking. Here, we report the first gas-phase characterization of closed-shell carbamate formation by deprotonated amides, using cryogenic ion trap vibrational spectroscopy combined with quantum chemical calculations. Reactions of deprotonated benzamide and isophthalamide anions with CO 2 form carbamate species, with the amide nitrogen serving as the nucleophilic site. Diagnostic, strongly red-shifted antisymmetric CO 2 stretching vibrational bands, supported by a bonding analysis, establish chemisorption with substantial charge transfer. In the multiamide system, an intramolecular N−H···O hydrogen bond provides synergistic stabilization, correlating with larger red shifts and more exothermic binding. These structure-assigned benchmarks provide molecular-level insights into the binding motif, charge redistribution, and hydrogen bond-mediated stabilization of amide carbamates, which aid the characterization of carbamate formation in condensed phase.

Amides↗
DOE OSTI2023

Size-Dependent Thermal Shifts to MOF Nanocrystal Optical Gaps Induced by Dynamic Bonding

Conventional semiconductor nanocrystals exhibit wide-ranging optical behavior, whereas the size-dependent photophysical properties of metal–organic framework (MOF) nanocrystals remain an open research frontier. Furthermore, we present size- and temperature-dependent optical absorption spectra of common MOFs with particle sizes ranging from tens of nanometers to several micrometers. All materials exhibit optical gaps that decrease at elevated temperatures, which we attribute to the dynamic nature of MOF metal–linker bonds. Accordingly, whereas the labile titanium–carboxylate bonds of MIL-125 give rise to bandgaps that red-shift by ~600 meV over 300 K, the more rigid zinc–imidazolate bonds of ZIF-8 produce a red-shift of only ~10 meV. Furthermore, smaller particles induce far larger decreases to optical gaps. Taken together, these results suggest MOF bonding becomes more flexible with smaller nanocrystal sizes, offering a powerful tool for manipulating optical behavior through composition, temperature, and dimensionality.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRSDate not supplied

A Low-Cost Innovative Observatory for the Reionization Explorer Mission (REX)

The early universe, from 400 to 800 million years after the Big Bang, or “Cosmic Dawn,” is characterized by large scale distributions of neutral and ionized intergalactic gas undergoing reionization on a cosmic scale at redshifts effectively unobservable through Earth’s atmosphere. Characterizing this active period of cosmological history requires wide-field, narrow passband surveys of galactic Lyman-alpha light red-shifted to the near infrared. REX combines low noise Near Infrared detectors and wide field optics to rapidly map large areas of space during the crucial Cosmic Dawn epoch of 400-800 million years after the Big Bang (Red Shift z=7 to z=10+).

T Casey↗
DOE OSTI2015

Self-catalyzed growth of dilute nitride GaAs/GaAsSbN/GaAs core-shell nanowires by molecular beam epitaxy

Bandgap tuning up to 1.3 μm in GaAsSb based nanowires by incorporation of dilute amount of N is reported. Highly vertical GaAs/GaAsSbN/GaAs core-shell configured nanowires were grown for different N contents on Si (111) substrates using plasma assisted molecular beam epitaxy. X-ray diffraction analysis revealed close lattice matching of GaAsSbN with GaAs. Micro-photoluminescence (μ-PL) revealed red shift as well as broadening of the spectra attesting to N incorporation in the nanowires. Replication of the 4K PL spectra for several different single nanowires compared to the corresponding nanowire array suggests good compositional homogeneity amongst the nanowires. A large red shift of the Raman spectrum and associated symmetric line shape in these nanowires have been attributed to phonon localization at point defects. Transmission electron microscopy reveals the dominance of stacking faults and twins in these nanowires. The lower strain present in these dilute nitride nanowires, as opposed to GaAsSb nanowires having the same PL emission wavelength, and the observation of room temperature PL demonstrate the advantage of the dilute nitride system offers in the nanowire configuration, providing a pathway for realizing nanoscale optoelectronic devices in the telecommunication wavelength region.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Laser entrance window transmission and reflection measurements for preheating in magnetized liner inertial fusion

Laser-driven magnetized liner inertial fusion (MagLIF) is being developed on the OMEGA Laser System to study scaling. MagLIF targets require a preheat laser entrance window that can hold the gas in the target yet allow sufficient laser energy to enter the gas. For OMEGA MagLIF targets, 1.8-μm-thick polyimide foils were found to be sufficient to hold a fuel pressure of up to 14 atm. Transmission and reflection of an OMEGA beam incident on such foils were measured with a calorimeter and time-resolved spectrometers for 2.5-ns square-shaped pulses, with energies from 60 to 200 J, focused to intensities from 0.65 to 2.2 × 10 14 W/cm 2 . The laser energy transmitted in every case exceeded that required to achieve the goal of preheating the gas to 100 eV. The time-resolved measurements showed an initial period with very low, decreasing transmission, the duration of which decreased with increasing intensity, followed by a rapid transition to full transmission, accompanied by brief sidescattering of the transmitted light with a significant red shift. Reflection was always negligible. Two-dimensional radiation–hydrodynamic simulations, using 3-D ray tracing with inverse bremsstrahlung energy deposition, did not capture the rapid transition to full transmission, showing instead a slow increase in transmission, without significant sidescatter or red shift. Finally, we propose that full transmission is achieved by relativistic self-focusing, enhanced by focusing related to the electron density profile that forms, followed by a ponderomotive blowout of the plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Time-refraction optics with single cycle modulation

Abstract We present an experimental study of optical time-refraction caused by time-interfaces as short as a single optical cycle. Specifically, we study the propagation of a probe pulse through a sample undergoing a large refractive index change induced by an intense modulator pulse. In these systems, increasing the refractive index abruptly leads to time-refraction where the spectrum of all the waves propagating in the medium is red-shifted, and subsequently blue-shifted when the refractive index relaxes back to its original value. We observe these phenomena in the single-cycle regime. Moreover, by shortening the temporal width of the modulator to ∼5–6 fs, we observe that the rise time of the red-shift associated with time-refraction is proportionally shorter. The experiments are carried out in transparent conducting oxides acting as epsilon-near-zero materials. These observations raise multiple questions on the fundamental physics occurring within such ultrashort time frames, and open the way for experimenting with photonic time-crystals, generated by periodic ultrafast changes to the refractive index, in the near future.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2003

Precision Clocks in Space and alpha-Variations

Important developments of both in theoretical and observational cosmology have fueled considerable interest in searches for variations of the fine structure constant. Experimentally, Webb et. al. have found evidence for a cosmological variation of the fine structure constant through an analysis of the absorption lines in galactic halos from quasar-emitted light. Recently developed small ion atomic clocks enable Solar System tests for equivalence principle (EP) violating (alpha)-variations by way of rate-comparisons of three ultra-stable atomic clocks near-to and far-from the sun where gravitational red-shift changes are more than 10(exp 4) larger than in low Earth orbit. No space tests of the EP have been made in nearly 30 years, since the GP-A hydrogen maser reached a 10,000 km apogee confirming EP red-shift predictions ~1 part in 10(exp 4). Today's small ion clocks, nearly 100x more stable and 100x smaller then the GP-A H-maser, could probe for EP violating scalar fields near the sun for mission costs comparable to low Earth orbiters and improve the GP-A sensitivity by 5 to 6 orders of magnitude.

(alpha)-variation↗
DOE OSTI2024

Intramolecular Polarization Contributions to the pKa’s of Carboxylic Acids Through the Chain Length Dependence of Vibrational Tag-Shifts in Cryogenically Cooled Pyridinium-(CH2)n-COOH (n = 1-7) Cations

The pKa’s of acids are known to depend on the ionic strength of an electrolyte solution, an effect that qualitatively results from electrostatic interactions of the acid and conjugate base with proximal ions. Here we explore an intramolecular variation on this theme in which a carboxylic acid group is tethered to a pyridinium cationic charge center with increasingly long alkyl linkages in the series Py+-(CH2)n-COOH, with n = 1-7. The effective acidities of the carboxylic acid group in the isolated cations are determined by recording the red-shifts in the frequencies of the acid OH stretches upon attachment to D2 and N2 molecules, measured by using cryogenic ion spectroscopy. The short chains indeed lead to substantial increases in acidity, with the effect falling off in the range of n = 4-5. The response of the CO stretch on the acid head group is surprisingly strong and, in contrast to the expected red shift of the OH, displays a blue shift as the chain length is reduced. Electronic structure calculations recover these trends and indicate that the proximal cationic charge center acts to draw electron density away from the acid C=O bond. This acts to blue shift the CO stretch while weakening the C-C bond that attaches the head group to the chain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

A comparative study of optical absorption and photocatalytic properties of nanocrystalline single-phase anatase and rutile TiO{sub 2} doped with transition metal cations

The effect of nanocrystalline TiO{sub 2} doping with transition metal cations (Cu{sup 2+}, Fe{sup 3+}, Co{sup 2+}, Cr{sup 3+}) on their optical absorption and photocatalytic properties was investigated. The obtained metal-doped TiO{sub 2} samples were characterized by X-ray diffraction, scanning electron microscopy, and UV-vis absorption spectroscopy. It is shown that doping effect on anatase (A) and rutile (R) properties is quite different, being much stronger and complicated on A than on R. Contrary to doped R, doped A revealed a significant red shift of the absorption edge along with the band gap narrowing. Photocatalytic activity of anatase increases upon doping in the order: A R/Co>R/Cu>R/Fe>R/Cr, indicating the inhibitory effect of impurity cations. This fact correlates with the decrease in the UV absorption of the doped rutile in the region of the Hg-lamp irradiation at 4.88 eV. - Graphical abstract: A red shift of the absorption edge of nanocrystalline single-phase anatase after doping with transition metal cations. Highlights: Black-Right-Pointing-Pointer Single-phase anatase and rutile powders surface-doped with transition metal cations. Black-Right-Pointing-Pointer Absorption edge and band gap of rutile do not change with surface doping. Black-Right-Pointing-Pointer Band gap of surface-doped anatase reduces being the lowest for A/Fe. Black-Right-Pointing-Pointer The surface-doping improves photocatalytic activity of anatase. Black-Right-Pointing-Pointer The surface-doping inhibits photocatalytic activity of rutile.

36 MATERIALS SCIENCE↗