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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Reconstructing the metric of the local Universe from number counts observations

Number counts observations available with new surveys such as the Euclid mission will be an important source of information about the metric of the Universe. We compute the low red-shift expansion for the energy density and the density contrast using an exact spherically symmetric solution in presence of a cosmological constant. At low red-shift the expansion is more precise than linear perturbation theory prediction. We then use the local expansion to reconstruct the metric from the monopole of the density contrast. We test the inversion method using numerical calculations and find a good agreement within the regime of validity of the red-shift expansion. The method could be applied to observational data to reconstruct the metric of the local Universe with a level of precision higher than the one achievable using perturbation theory.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Characterizing Photon Reabsorption in Quantum Dot-Polymer Composites for Use as Displacement Sensors

The reabsorption of photoluminescence within a medium, an effect known as the inner filter effect (IFE), has been well studied in solutions, but has garnered less attention in regards to solid-state nanocomposites. Photoluminescence from a quantum dot (QD) can selectively excite larger QDs around it resulting in a net red-shift in the reemitted photon. In CdSe/CdS core/shell QD-polymer nanocomposites, we observe a large spectral red-shift of over a third of the line width of the photoluminescence of the nanocomposites over a distance of 100 μm resulting from the IFE. Unlike fluorescent dyes, which do not show a large IFE red-shift, QDs have a component of inhomogeneous broadening that originates from their size distribution and quantum confinement. By controlling the photoluminescence broadening as well as the sample dispersion and concentration, we show that the magnitude of the IFE within the nanocomposite can be tuned. We further demonstrate that this shift can be exploited in order to spectroscopically monitor the vertical displacement of a nanocomposite in a fluorescence microscope. Large energetic shifts in the measured emission with displacement can be maximized, resulting in a displacement sensor with submicrometer resolution. We further show that the composite can be easily attached to biological samples and is able to measure deformations with high temporal and spatial precision.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS1973

Distortion of the microwave blackbody background radiation implied by the baryon-symmetric cosmology of omnes and the galaxy formation theory of Stecker and Puget

Theories on the distortion of microwave black body spectrum are presented. Data suggest that continuous annihilation of matter-antimatter, during all stages of universe evolution cause distortion by thermal energy distribution at red shifts less than 10,000. Data also show distortions in the Rayleigh-Jeans spectrum are caused by energy depositions at red shifts between 10,000 and 1,000 while those in the Wien spectrum are due to energy deposition at lower red shifts after the cosmic gas cools to its atomic state and thermalization does not take place properly.

Stecker, F. W.↗
NASA NTRS2023

A Technique to Measure Coronal Electron Density, Temperature, and Velocity Above 2.5 R⨀ from Sun Center using Polarized Brightness Spectrum

The current model for the polarized brightness (pB) spectrum has a decades-long history of progressively incorporating its dependence on electron density Ne, temperature Te, and flow velocity in the radial direction V e . The pB N e spectrum follows the exact shape of the photosphere spectrum, which is not smooth, which is expected from the thermal Doppler broadening of the photosphere spectrum due to the high coronal T e ; the pB N e T e spectrum is smooth, but the free coronal electrons remain static and unaffected by solar wind, and the pB N e T e V e spectrum is red-shifted by electrons seeing a red-shifted photosphere spectrum as they flow away from the Sun as solar wind, which takes a radial direction above 2.5 R ⨀ from Sun center. In this article, we review the progress of the above three model pB spectra in describing the observations and highlight the differences, first by comparing the three model pB spectra against wavelength using a model for Ne and constant values for T e and V e , and second by generating three model 2D pB maps by integrating over a selected wavelengthregion in the three model pB spectra along lines of sight passing through the 14 July 2000 (“Bastille Day”) coronal mass ejection (CME) model, which contains 3D information on N e , T e , and V e . In this regard, the COronal Diagnostic EXperiment (CODEX) on the International Space Station (ISS) in 2024 will measure N e , T e , and V e by matching the measured pB with modeled pB N e T e V e in selected wavelength regions using multiple filters.

Electron density↗
NASA NTRS2023

A Technique to Measure Coronal Electron Density, Temperature, and Velocity Above 2.5 R from Sun Center Using Polarized Brightness Spectrum

The current model for the polarized brightness (pB) spectrum has a decades-long history of progressively incorporating its dependence on electron density N(e), temperature T(e), and flow velocity in the radial direction V(e). The pBNe spectrum follows the exact shape of the photosphere spectrum, which is not smooth, which is expected from the thermal Doppler broadening of the photosphere spectrum due to the high coronal T(e). The pBN(e) spectrum is smooth, but the free coronal electrons remain static and unaffected by solar wind, and the pBN(e)T(e)V(e) spectrum is red-shifted by electrons seeing a red-shifted photosphere spectrum as they flow away from the Sun as solar wind, which takes a radial direction above 2.5 R from Sun center. In this article, we review the progress of the above three model pB spectra in describing the observations and highlight the differences, first by comparing the three model pB spectra against wavelength using a model for Ne and constant values for T(e) and V (e), and second by generating three model 2D pB maps by integrating over a selected wavelength region in the three model pB spectra along lines of sight passing through the 14 July 2000 (“Bastille Day”) coronal mass ejection (CME) model, which contains 3D information on N(e), T(e), and V e. In this regard, the COronal Diagnostic EXperiment (CODEX) on the International Space Station (ISS) in 2024 will measure N(e), T(e), and V(e) by matching the measured pB with modeled pBN(e)T(e)V(e) in selected wavelength regions using multiple filters.

Electron density↗
NASA NTRS1990

Strong associated C 4 absorption in low redshift quasars

IUE spectra of quasars were used to determine the frequency of occurrence of strong associated C 4 absorption systems at low red shifts. Four systems are found with rest frame equivalent width (REW) greater than 5 angstroms in the spectra of 38 quasars. This rate of occurrence of 0.12 is not significantly different from the rate of 0.064 determined for high red shift quasars. The detected strong associated systems are all in low red shift quasars which have been imaged from the ground. One of the quasars is unusual, having two nuclei, a close companion and distorted isotopes. Two of the others also have close companion galaxies at projected distances of under 100 kpc. The conclusion was made that a much larger sample is needed.

Tytler, David↗
DOE OSTI2020

Ligand-Dependent Tuning of Interband and Intersubband Transitions of Colloidal CdSe Nanoplatelets

Although surface ligands of colloidal nanocrystals are known to adjust the absolute energy levels of valence and conduction bands of semiconductor nanocrystals, they typically have only minor influence on the band gap or effective masses. This changes in nanoplatelets. Ligand exchange of CdSe colloidal nanoplatelets induces large (up to 300 meV) bathochromic shifts of both interband and intersubband transitions. Here, three families of ligands-halides, thiolates, and phosphonates-are used to tune interband transitions, reflecting electron and hole confinement, across visible wavelengths and intersubband transitions, reflecting electron confinement, across the near-infrared spectral window. Furthermore, careful examination shows that delocalization from expansion of the nanoplatelet short axis, which was reported previously, cannot alone explain observed red shifts. Instead, comparison of intersubband, interband, and hole energy levels shows that ligand head group chemistry confers specific, idiosyncratic adjustments of the contribution of conduction and valence bands to the observed bathochromic shifts. Phosphonate ligands show the largest band gap reductions but the smallest red shift of intersubband transition energies; halide-exchanged samples displayed smaller reductions in band gap but large red shifts of intersubband transitions; thiolates fall in between. A related specificity is observed in hole states, which implicates ligand-responsive valence band curvature as an additional contribution driving optical changes. For nanoplatelets, surface ligand chemistry offers not only a tool to adjust the absolute energy level of conduction and valence bands but also an alternative route to preferential electron or hole band engineering that is normally achieved with inorganic shells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Tuning Optical Properties of Conjugated Molecules by Lewis Acids: Insights from Electronic Structure Modeling

Understanding and controlling the optoelectronic properties of organic semiconductors at the molecular level remains a challenge due to the complexity of chemical structures and intermolecular interactions. A common strategy to address this challenge is to utilize both experimental and computational approaches. In this contribution, we show that density functional theory (DFT) calculation is a useful tool to provide insights into the bonding, electron population distribution, and optical transitions of adducts between conjugated molecules and Lewis acids (CM-LA). Adduct formation leads to relevant modifications of key properties, including a red shift in optical transitions and an increase in charge carrier density and charge mobility, compared to the parent conjugated molecules. We show that electron density transfer from the CM to the LA, which was hypothesized to cause the experimental red shift in absorption spectra upon LA binding, can be quantified and interpreted by population analysis. Experimental red shifts in optical transitions for all molecular families can also be predicted by time dependent DFT calculations with different density functionals. Finally, these detailed insights help to optimize a priori design guidelines for future applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Hydrothermally robust Ti/SiO 2 epoxidation catalysts via surface modification with oligomeric PMHS

We investigate grafting of poly(methylhydrosiloxane) (PMHS) onto Ti/SiO 2 catalysts for improving their robustness to water, using olefin epoxidation catalysis with organic hydroperoxide as oxidant as a relevant probe reaction. Our approach involves triggering catalyst deactivation with added water in the reactants as a means to simulate catalyst deactivation, thereby causing grafted Ti-site aggregation. When using harsh aqueous Soxhlet extraction conditions as a trigger for this aggregation, significant differences are observed via diffuse-reflectance UV-Vis spectrscopy on samples before and after treatment, for Ti/SiO 2 catalysts containing grafted PMHS. Not only was there a lack of appearance of red-shifted bands in the UV-Vis spectrum following Soxhlet extraction, the batch catalytic activity for catalysts before and after PMHS grafting remained virtually unchanged. This was in stark contrast to an unmodified Ti/SiO 2 catalyst, which showed a more than 60% decrease in catalytic activity following Soxhlet extraction as a result of aggregation, as ascertained by red shifts in its UV-Vis spectrum after Soxhlet extraction. Similar red shifts were also observed for a hydrophobically modified TMS Ti/SiO 2 catalyst. However, when comparing these catalysts under more gentle olefin epoxidation catalysis conditions with added water in a flow reactor, it was more difficult to differentiate the TMS Ti/SiO2 and grafted PMHS catalysts. Both catalysts exhibited similar activity and selectivity after a prolonged time on stream, though the rate of initial deactivation in the latter was less pronounced. Altogether, our data demonstrate that grafted PMHS catalysts are positively differentiated from conventional catalysts based on either TMS surface modification or no surface modification, under conditions involving aggregation induced via extreme hydrothermal environmentst. Thus, we expect that PMHS grafting of Lewis acid catalysts can offer an alternative approach for endowing hydrolytic stability to such catalysts, as demonstrated here for Ti/SiO 2 epoxidation catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Electro-absorption of silicene and bilayer graphene quantum dots

We study numerically the optical properties of low-buckled silicene and AB-stacked bilayer graphene quantum dots subjected to an external electric field, which is normal to their surface. Within the tight-binding model, the optical absorption is calculated for quantum dots, of triangular and hexagonal shapes, with zigzag and armchair edge terminations. We show that in triangular silicene clusters with zigzag edges a rich and widely tunable infrared absorption peak structure originates from transitions involving zero energy states. The edge of absorption in silicene quantum dots undergoes red shift in the external electric field for triangular clusters, whereas blue shift takes place for hexagonal ones. In small clusters of bilayer graphene with zigzag edges the edge of absorption undergoes blue/red shift for triangular/hexagonal geometry. In armchair clusters of silicene blue shift of the absorption edge takes place for both cluster shapes, while red shift is inherent for both shapes of the bilayer graphene quantum dots.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Structure-Based Exciton Hamiltonian and Dynamics for the Reconstituted Wild-type CP29 Protein Antenna Complex of the Photosystem II

Here we provide an analysis of the pigment composition of reconstituted wild type CP29 complexes. The obtained stoichiometry of 9 ± 0.6 Chls a and 3 ± 0.6 Chls b per complex, with some possible heterogeneity in the carotenoid binding, is in agreement with 9 Chls a and 3.5 Chls b revealed by the modeling of low-temperature optical spectra. We find that ~50% of Chl b614 is lost during the reconstitution/purification procedure, while Chls a are almost fully retained. The excitonic structure and the nature of the low-energy (low-E) state(s) are addressed via simulations (using Redfield theory) of 5 K absorption and fluorescence/nonresonant hole-burned (NRHB) spectra obtained at different excitation/burning conditions. We show that, depending on laser excitation frequency, reconstituted complexes display two (independent) low-E states (i.e., the A and B traps) with different NRHB and emission spectra. The red-shifted state A near 682.4 nm is assigned to a minor (~10%) subpopulation (Sub. II) that most likely originates from an imperfect local folding occurring during protein reconstitution. Its lowest energy state A (localized on Chl a604) is easily burned with λ B = 488.0 nm and has a red-shifted florescence origin band near 683.7 nm that is not observed in native (isolated) complexes. Prolonged burning by 488.0 nm light reveals a second low-E trap at 680.2 nm (state B) with a fluorescence origin-band ~681 nm which is also observed when using a direct lowfluence excitation near 650 nm. The latter state is mostly delocalized over the a611, a612, a615 Chl trimer, and corresponds to the lowest energy state of the major (~90%) subpopulation (Sub. I) which exhibits a lower hole-burning quantum yield. Thus, we suggest that major Sub. I correspond to the native folding of CP29, whereas the red-shift of the Chl a604 site energy observed in the minor Sub. II occurs only in reconstituted complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Diamagnetic susceptibility and optical properties of a spherical quantum dot: effects of the parabolic and the shifted parabolic potentials

Centred charge donor related diamagnetic susceptibility and optical properties of a spherical GaAs quantum dot are presented. In particular, effects of intrinsic parabolic and shifted parabolic potentials on these quantities are investigated. This is theoretically achieved by solving the Schrödinger equation within the effective mass approximation. It is observed that the parabolic potential reduces the magnitude of the diamagnetic susceptibility while the shifted parabolic potential increases it. Other findings are that the parabolic potential blue-shifts both the absorption coefficient and the change in refractive index of quantum dots, while the shifted parabolic potential red-shifts these quantities. These features are discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Growth of Au nanoparticle films and the effect of nanoparticle shape on plasmon peak wavelength

Metal nanoparticles (NPs) exhibit localized surface plasmon resonance (LSPR) and thus have potential for use in a wide range of applications. A facile technique for the preparation of NP films using an electron-cyclotron-resonance plasma sputtering method without a dewetting process is described. Field emission scanning electron microscopy (FE-SEM) observations revealed that the Au NPs grew independently as island-like particles during the first stage of sputtering and then coalesced with one another as sputtering time increased to ultimately form a continuous film. A plasmon absorption peak was observed via optical measurement of absorption efficiency. The LSPR peak shifted toward longer wavelengths (red shift) with an increase in sputtering time. The cause of this plasmon peak shift was theoretically investigated using the finite-difference time-domain calculation method. A realistic statistical distribution of the particle shapes based on FE-SEM observations was applied for the analysis, which has not been previously reported. It was determined that the change in the shape of the NPs from spheroidal to oval or slender due to coalescence with neighbouring NPs caused the LSPR peak shift. These results may enable the design of LSPR devices by controlling the characteristics of the nanoparticles, such as their size, shape, number density, and coverage.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Gain and tuning characteristics of mid-infrared InSb quantum dot diode lasers

There have been relatively few reports of lasing from InSb quantum dots (QDs). In this work, type II InSb/InAs QD laser diodes emitting in the mid-infrared at 3.1 μm have been demonstrated and characterized. The gain was determined to be 2.9 cm{sup −1} per QD layer, and the waveguide loss was ∼15 cm{sup −1} at 4 K. Spontaneous emission measurements below threshold revealed a blue shift of the peak wavelength with increasing current, indicating filling of ground state heavy hole levels in the QDs. The characteristic temperature, T{sub 0} = 101 K below 50 K, but decreased to 48 K at higher temperatures. The emission wavelength of these lasers showed first a blue shift followed by a red shift with increasing temperature. A hybrid structure was used to fabricate the laser by combining a liquid phase epitaxy grown p-InAs{sub 0.61}Sb{sub 0.13}P{sub 0.26} lower cladding layer and an upper n{sup +} InAs plasmon cladding layer which resulted in a maximum operating temperature (T{sub max}) of 120 K in pulsed mode, which is the highest reported to date.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Shifting the MLCT of d 6 metal complexes to the red and NIR

Light-active d 6 -coordination compounds hold great promise for light energy conversion, sensors and therapeutic applications. However, the activity in the red-to-NIR spectral region is highly desirable to convert solar light more efficiently, use low-cost red-light sources and activate these chromophores in biological tissue environment. Due to their versatility, tunability and broad intense absorption, d 6 -coordination compounds with metalto-ligand charge transfer (MLCT) transitions are especially interesting. This review article offers a comprehensive collection of strategies to tune MLCT excited states in d 6 metal complexes and gives insights on group 6 to group 9 transition metals and their respective state-of-the-art MLCT engineering towards red-shifted absorption and emission properties with long-lived excited states. Strategies comprise lowering the π* level of the ligands, destabilizing and mixing of the metal-based HOMO, switching within a group of transition metals, matrix effects and insights into dealing with excited state deactivation in the context of the energy gap law.

Metal to ligand charge transfer (MLCT)↗
NASA NTRS1988

The Einstein Observatory extended medium sensitivity survey sample of BL Lacertae objects

We present new results on BL Lacertae Objects discovered in an extensive X-ray survey of the high galactic latitude sky performed by the Einstein satellite. While BL Lacs have been found primarily in high frequency radio surveys, we show that X-ray emission is an efficient new method for finding such objects and will offer an outstanding opportunity to find many of these objects in the near future using the ROSAT all-sky survey. It is also shown that X-ray selected BL Lac objects have somewhat different optical and radio properties than their radio selected counterparts. Using a complete, flux limited sample of 16 X-ray selected BL Lacs, we show that their number counts differ decisively from those of X-ray selected QSOs. Moreover, using the few red shifts available for these objects and limits on red shift determined from resolving the optical images of most of the remainder of the sample, a preliminary V/Vmax = 0.37 +/- 0.06. This value suggests an evolution in luminosity and/or density opposite in sense to that of QSOs.

Stocke, John T.↗
DOE OSTI2015

Self-assembly and photoluminescence evolution of hydrophilic and hydrophobic quantum dots in sol–gel processes

Graphical abstract: Highly luminescent quantum dots (QDs) with tunable photoluminescence (PL) wavelength were assembled into various morphologies including chain, hollow spheres, fibers, and ring structures through sol–gel processes. The PL properties during assembly as investigated. - Highlights: • Highly luminescent quantum dots (QDs) were synthesized from several ligands. • The evolution of PL in self-assembly via sol–gel processes was investigated. • CdTe QDs were assembled into a chain by controlling hydrolysis and condensation reactions. • Hollow spheres, fibers, and ring structures were created via CdSe/ZnS QDs in sol–gel processes. - Abstract: Highly luminescent quantum dots (QDs) with tunable photoluminescence (PL) wavelength were synthesized from several ligands to investigate the PL evolution in QD self-assembly via sol–gel processes. After ligand exchange, CdTe QDs were assembled into a chain by controlling the hydrolysis and condensation reaction of 3-mercaptopropyl-trimethoxysilane. The chain was then coated with a SiO{sub 2} shell from tetraethyl orthosilicate (TEOS). Hollow spheres, fibers, and ring structures were created from CdSe/ZnS QDs via various sol–gel processes. CdTe QDs revealed red-shifted and narrowed PL spectrum after assembly compared with their initial one. In contrast, the red-shift of PL spectra of CdSe/ZnS QDs is small. By optimizing experimental conditions, SiO{sub 2} spheres with multiple CdSe/ZnS QDs were fabricated using TEOS and MPS. The QDs in these SiO{sub 2} spheres retained their initial PL properties. This result is useful for application because of their high stability and high PL efficiency of 33%.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1980

Impulsive EUV bursts observed in C IV with OSO-8

Time sequences of profiles of the 1548 A line of C IV containing 51 EUV bursts observed in or near active regions are analyzed to determine the brightness, Doppler shift and line broadening characteristics of the bursts. The bursts have mean lifetimes of approximately 150 s, and mean increases in brightness at burst maximum of four-fold as observed with a field of view of 2 x 20 arc sec. Mean burst diameters are estimated to be 3 arc sec, or smaller. All but three of the bursts show Doppler shifts with velocities sometimes exceeding 75 km/s; 31 are dominated by red shifts and 17 are dominated by blue shifts. Approximately half of the latter group have red-shifted precursors. The bursts are interpreted as prominence material, such as surges and coronal rain, moving through the field of view of the spectrometer.

Athay, R. G.↗