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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 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
NASA NTRS1996

High Spectral Resolution Lidar Measurements of Multiple Scattering

The University of Wisconsin High Spectral Resolution Lidar (HSRL) provides unambiguous measurements of backscatter cross section, backscatter phase function, depolarization, and optical depth. This is accomplished by dividing the lidar return into separate particulate and molecular contributions. The molecular return is then used as a calibration target. We have modified the HSRL to use an I2 molecular absorption filter to separate aerosol and molecular signals. This allows measurement in dense clouds. Useful profiles extend above the cloud base until the two way optical depth reaches values between 5 and 6; beyond this, photon counting errors become large. In order to observe multiple scattering, the HSRL includes a channel which records the combined aerosol and molecular lidar return simultaneously with the spectrometer channel measurements of optical properties. This paper describes HSRL multiple scattering measurements from both water and ice clouds. These include signal strengths and depolarizations as a function of receiver field of view. All observations include profiles of extinction and backscatter cross sections. Measurements are also compared to predictions of a multiple scattering model based on small angle approximations.

Eloranta, E. W.↗
NASA NTRS2021

Continuum, cyclotron line, and absorption variability in the high-mass X-ray binary Vela X-1

Because of its complex clumpy wind, prominent cyclotron resonant scattering features, intrinsic variability, and convenient physical parameters (close distance, high inclination, and small orbital separation), which facilitate the observation and analysis of the system, Vela X-1 is one of the key systems for understanding accretion processes in high-mass X-ray binaries on all scales. We revisit Vela X-1 with two new observations taken with NuSTAR at orbital phases ∼0.68–0.78 and ∼0.36–0.52, which show a plethora of variability and allow us to study the accretion geometry and stellar wind properties of the system. We follow the evolution of spectral parameters down to the pulse period timescale using a partially covered power law continuum with a Fermi-Dirac cutoff to model the continuum and local absorption. We are able to confirm anti-correlations between the photon index and the luminosity and, for low fluxes, between the folding energy and the luminosity, implying a change of properties in the Comptonising plasma. We were not able to confirm a previously seen correlation between the cyclotron line energy and the luminosity of the source in the overall observation, but we observed a drop in the cyclotron line energy following a strong flare. We see strong variability in absorption between the two observations and within one observation (for the ∼0.36–0.52 orbital phases) that can be explained by the presence of a large-scale structure, such as accretion and photoionisation wakes in the system, and our variable line of sight through this structure.

C. M. Diez↗
DOE OSTI2021

Multilayer Lateral Heterostructures of Van Der Waals Crystals with Sharp, Carrier–Transparent Interfaces

Abstract Research on engineered materials that integrate different 2D crystals has largely focused on two prototypical heterostructures: Vertical van der Waals stacks and lateral heterostructures of covalently stitched monolayers. Extending lateral integration to few layer or even multilayer van der Waals crystals could enable architectures that combine the superior light absorption and photonic properties of thicker crystals with close proximity to interfaces and efficient carrier separation within the layers, potentially benefiting applications such as photovoltaics. Here, the realization of multilayer heterstructures of the van der Waals semiconductors SnS and GeS with lateral interfaces spanning up to several hundred individual layers is demonstrated. Structural and chemical imaging identifies {110} interfaces that are perpendicular to the (001) layer plane and are laterally localized and sharp on a 10 nm scale across the entire thickness. Cathodoluminescence spectroscopy provides evidence for a facile transfer of electron‐hole pairs across the lateral interfaces, indicating covalent stitching with high electronic quality and a low density of recombination centers.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unveiling the Structural Origins of Dynamic Diversity in Pd-Based Metallic Glasses

The β -relaxation is one of the major dynamic behaviors in metallic glasses (MGs) and exhibits diverse features. Despite decades of efforts, the understanding of its structural origin and contribution to the overall dynamics of MG systems is still unclear. Here two palladium-based Pd—Cu—P and Pd—Ni—P MGs are reported with distinct different β -relaxation behaviors and reveal the structural origins for the difference using the advanced X-ray photon correlation spectroscopy and absorption fine structure techniques together with the first-principles calculations. The pronounced β -relaxation and fast atomic dynamics in the Pd—Cu—P MG mainly come from the strong mobility of Cu atoms and their locally favored structures. In contrast, the motion of Ni atoms is constrained by P atoms in the Pd—Ni—P MG, leading to the weakened β -relaxation peak and sluggish dynamics. Finally, the correlation of atomic dynamics with microscopic structures provides a way to understand the structural origins of different dynamic behaviors as well as the nature of aging in disordered materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Resonant double-core excitations with ultrafast, intense X-ray pulses

Intense few-to-sub-femtosecond soft X-ray pulses can produce neutral, two-site excited double-core-hole states by promoting two core electrons to the same unoccupied molecular orbital. We theoretically investigate double nitrogen K-edge excitations of nitrous oxide (N$_2$O) with multiconfigurational electronic structure calculations. We show that the second core-excitation energy is reduced with respect to its ground state value. A site-selective double core-excitation mechanism using intense few-femtosecond x-rays is investigated using time-dependent Schrodinger equation (TDSE) simulations. The subsequent two-step Auger-Meitner and two-electrons-one-electron decay spectra of the double core-excited states are analysed using a Mulliken population analysis of the multiconfirational wavefunctions. The change in the electron emission lineshape between the absorption of 1 or 2 photons in the resonant core-excitation is predicted by combining this approach with the TDSE simulations. Furthermore, we examine the possibility of resolving the double core-excited states with X-ray pump-probe techniques by calculating the chemical shifts of the core-electron binding energy of the core-excited states and decay products.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Anthracene Diphosphate Ligands for CdSe Quantum Dots; Molecular Design for Efficient Upconversion

Quantum dot (QD)-sensitized photon upconversion follows a multi-step energy transfer process from the QD to transmitter ligand to a soluble annihilator. Using a novel 10-R-anthracene-1,8-diphosphoric acid (R = octyl, 2- hexyldecyl, phenyl) ligand with high binding affinity for CdSe QD surfaces, we demonstrate a photon upconversion process that is limited by the transmitter to annihilator transfer efficiency. Using 1 H NMR spectroscopy, we demonstrate that these bidentate diphosphate ligands rapidly and irreversibly displace two carboxylate ligands. These ligands mediate energy transfer from the photoexcited QDs to a triplet annihilator (1,10-diphenylanthracene), producing overall photon upconversion quantum efficiencies as high as 17%, the highest for QDs with no shells. In conclusion, transient absorption spectroscopy shows that the anthracene dihydrogen phosphate (ADP) ligand supports a 3.4 fold longer triplet state lifetime compared to 9-anthracene carboxylic acid (299.9 ± 9.5 vs 88.2 ± 2.1 μs), increasing the probability of energy transfer.

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

Transparent conducting oxides: from all-dielectric plasmonics to a new paradigm in integrated photonics

During the past few years, the optics and photonics communities have renewed their attention toward transparent conducting oxides (TCOs), which for over two decades have been broadly employed for the fabrication of transparent electrodes in photovoltaic and communication technologies. This reinvigorated research curiosity is twofold: on the one hand, TCOs, with their metal-like properties, low optical absorption, and fabrication flexibility, represent an appealing alternative to noble metals for designing ultra-compact plasmonic devices. On the other hand, this class of hybrid compounds has been proved to possess exceptionally high optical nonlinearities when operating on a frequency window centered around their crossover point, the wavelength point at which the real part of the dielectric permittivity switches sign. Because TCOs are wide-bandgap materials with the Fermi level located in the conduction band, they are hybrid in nature, thus presenting both interband and intraband nonlinearities. This is the cause of a very rich nonlinear physics that is yet to be fully understood and explored. In addition to this, TCOs are epsilon-near-zero (ENZ) materials within a broad near-infrared spectral range, including the entire telecom bandwidth. In this operational window a myriad of novel electromagnetic phenomena have been demonstrated experimentally such as supercoupling, wavefront freezing, and photon doping. Furthermore, TCOs stand out among all other ENZ systems due to one fundamental characteristic, which is hardly attainable even by using structured materials. In fact, around their ENZ wavelength and for a quite generous operational range, these materials can be engineered to have an extremely small real index. This peculiarity leads to a slow-light effect that is ultimately responsible for a significant enhancement of the material nonlinear properties and is the cornerstone of the emerging field of near-zero-index photonics. In this regard, the recent history of nonlinear optics in conductive oxides is growing extremely fast due to a great number of experiments reporting unprecedentedly remarkable effects, including unitary index change, bandwidth-large frequency shift, efficient ultra-low-power frequency conversion, and many others. This review is meant to guide the reader through the exciting journey of TCOs, starting as an industrial material for transparent electrodes, then becoming a new alternative for low-loss plasmonics, and recently opening up new frontiers in integrated nonlinear optics. The present review is mainly focused on experimental observations.

42 ENGINEERING↗
DOE OSTI2023

On-demand directional microwave photon emission using waveguide quantum electrodynamics

Routing quantum information between non-local computational nodes is a foundation for extensible networks of quantum processors. Quantum information transfer between arbitrary nodes is generally mediated either by photons that propagate between them or by resonantly coupling nearby nodes. The utility is determined by the type of emitter, propagation channel and receiver. Conventional approaches involving propagating microwave photons have limited fidelity due to photon loss and are often unidirectional, whereas architectures that use direct resonant coupling are bidirectional in principle but can generally accommodate only a few local nodes. Here we demonstrate high-fidelity, on-demand, directional, microwave photon emission. We do this using an artificial molecule comprising two superconducting qubits strongly coupled to a bidirectional waveguide, effectively creating a chiral microwave waveguide. Quantum interference between the photon emission pathways from the molecule generates single photons that selectively propagate in a chosen direction. This circuit will also be capable of photon absorption, making it suitable for building interconnects within extensible quantum networks.

42 ENGINEERING↗
NASA NTRS1994

The chemistry of hydrocarbon ions in the Jovian ionosphere

We have modeled the chemistry of hydrocarbon ions in the jovian ionosphere. We find that a layer of hydrocarbon ions is formed in the altitude range 300-400 km above the ammonia cloud tops, due largely to direct ionization of hydrocarbons by photons in the wings of the H2 absorption lines in the 912- to 1100-A region that penetrate to below the methane homopause. We have explicitly included in the model 156 ion-neutral reactions involving hydrocaron ions with up to two carbon atoms. Larger hydrocarbon ions are included as two pseudoions, C3Hn(+) and C4Hn(+). The model shows that 15 reactions of H(+), CH3(+), CH5(+), C2H3(+), C2H5(+), and C2H6(+) with hydrocarbon neutrals are the major processes that are responsible for the production and growth of C1-, C2- and C3- or C4-ions in the hydrocarbon ion layer. The model also shows that ions initially produced in the hydrocarbon ion layer are converted into hydrocarbon ions with more than two carbon atoms with very little loss by recombination. It is likely that successive hydrocarbon ion-neutral reactions continue to produce even larger hydrocarbon ions, so the terminal ions probably have more than three or four carbon atoms. In the auroral regions, the chemistry of hydrocarbon ions may modify the densities of neutral hydrocarbons, especially C2H2 in the upper mesosphere, and may play a major role in the production of polar haze particles.

Kim, Y. H.↗
NASA NTRS2004

Coherence Phenomena in Coupled Optical Resonators

We predict a variety of photonic coherence phenomena in passive and active coupled ring resonators. Specifically, the effective dispersive and absorptive steady-state response of coupled resonators is derived, and used to determine the conditions for coupled-resonator-induced transparency and absorption, lasing without gain, and cooperative cavity emission. These effects rely on coherent photon trapping, in direct analogy with coherent population trapping phenomena in atomic systems. We also demonstrate that the coupled-mode equations are formally identical to the two-level atom Schrodinger equation in the rotating-wave approximation, and use this result for the analysis of coupled-resonator photon dynamics. Notably, because these effects are predicted directly from coupled-mode theory, they are not unique to atoms, but rather are fundamental to systems of coherently coupled resonators.

Smith, D. D.↗
NASA NTRS2010

Derivation of a Relation for the Steepening of TeV Selected Blazar Gamma-Ray Spectra with Energy and Redshift

We derive a relation for the steepening of blazar gamma-ray spectra between the multi-GeV Fermi energy range and the TeV energy range observed by atmospheric Cerenkov telescopes. The change in spectral index is produced by two effects: (1) an intrinsic steepening, independent of redshift, owing to the properties of emission and absorption in the source, and (2) a redshift-dependent steepening produced by intergalactic pair production interactions of blazar gamma-rays with low energy photons of the "intergalactic background light" (IBL). Given this relation, with good enough data on the mean gamma-ray SED of TeV Selected BL Lacs, the redshift evolution of the IBL can, in principle, be determined independently of stellar evolution models. We apply our relation to the results of new Fermi observations of TeV selected blazars.

Stecker, F.↗
NASA NTRS2008

Molecules for Fluorescence Detection of Specific Chemicals

A family of fluorescent dye molecules has been developed for use in on-off fluorescence detection of specific chemicals. By themselves, these molecules do not fluoresce. However, when exposed to certain chemical analytes in liquid or vapor forms, they do fluoresce (see figure). These compounds are amenable to fixation on or in a variety of substrates for use in fluorescence-based detection devices: they can be chemically modified to anchor them to porous or non-porous solid supports or can be incorporated into polymer films. Potential applications for these compounds include detection of chemical warfare agents, sensing of acidity or alkalinity, and fluorescent tagging of proteins in pharmaceutical research and development. These molecules could also be exploited for use as two-photon materials for photodynamic therapy in the treatment of certain cancers and other diseases. A molecule in this family consists of a fluorescent core (such as an anthracene or pyrene) attached to two end groups that, when the dye is excited by absorption of light, transfer an electron to the core, thereby quenching the fluorescence. The end groups can be engineered so that they react chemically with certain analytes. Upon reaction, electrons on the end groups are no longer available for transfer to the core and, consequently, the fluorescence from the core is no longer quenched. The chemoselectivity of these molecules can be changed by changing the end groups. For example, aniline end groups afford a capability for sensing acids or acid halides (including those contained in chemical warfare agents). Pyridine or bipyridyl end groups would enable sensing of metal ions. Other chemicals that can be selectively detected through suitable choice of end groups include glucose and proteins. Moreover, the fluorescent cores can be changed to alter light-absorption and -emission characteristics: anthracene cores fluoresce at wavelengths around 500 nm, whereas perylene cores absorb and emit at wavelengths of about 600 nm.

Fedor, Steve↗
DOE OSTI2024

Deciphering between enhanced light emission and absorption in multi-mode porphyrin cavity polariton samples

Abstract It remains unclear how the collective strong coupling of cavity-confined photons to the electronic transitions of molecular chromophore leverages the distinct properties of the polaritonic constituents for future technologies. In this study, we design, fabricate, and characterize multiple types of Fabry-Pérot (FP) mirco-resonators containing copper(II) tetraphenyl porphyrin (CuTPP) to show how cavity polariton formation affects radiative relaxation processes in the presence of substantial non-Condon vibronic coupling between two of this molecule’s excited electronic states. Unlike the prototypical enhancement of Q state radiative relaxation of CuTPP in a FP resonator incapable of forming polaritons, we find the light emission processes in multimode cavity polariton samples become enhanced for cavity-exciton energy differences near those of vibrations known to mediate non-Condon vibronic coupling. We propose the value of this detuning is consistent with radiative relaxation of Herzberg-Teller polaritons into collective molecular states coupled to the cavity photon coherently. We contrast the feature stemming from light emission from the HT polariton state with those that occur due to polariton-enhanced light absorption. Our results demonstrate the landscape of molecular and photonic interactions enabled by cavity polariton formation using complex chromophores and how researchers can design resonators to leverage these interactions to characterize and control polaritonic properties.

Odewale, Elizabeth O.↗
DOE OSTI2021

Probing the polar-nonpolar oxide interfaces using resonant x-ray standing wave techniques

Transition metal (TM) oxide heterostructure superlattices have attracted great attention in research communities because of their emergent interfacial phenomena that do not exist in the bulk form. In order to understand the mechanisms that cause these phenomena, it is important to use depth-resolved spectroscopies to study the electronic structure across the buried oxide interfaces. In this review, we focus on the recent applications of standing wave (SW) photoemission (SW-XPS) and resonant inelastic x-ray scattering (SW-RIXS) spectroscopy to study the depth profiles of electronic structure or carriers around the polar-nonpolar oxide interfaces. Here, using the incident photon energies near the TM x-ray absorption resonance, the created SW excitation can enhance the spectral response and certain electronic transitions, providing important insight into the interfacial electronic structure in the energy and real space regimes. Following the background introductions, we describe two SW experiments and demonstrate that the combination of SW-XPS and SW-RIXS has the potential to obtain the depth distribution of electronic/orbital states around the buried interfaces with Angstrom precision.

36 MATERIALS SCIENCE↗
NASA NTRS2012

Airborne Lidar Measurements of Atmospheric Pressure Made Using the Oxygen A-Band

Accurate measurements of greenhouse gas mixing ratios on a global scale are currently needed to gain a better understanding of climate change and its possible impact on our planet. In order to remotely measure greenhouse gas concentrations in the atmosphere with regard to dry air, the air number density in the atmosphere is also needed in deriving the greenhouse gas concentrations. Since oxygen is stable and uniformly mixed in the atmosphere at 20.95%, the measurement of an oxygen absorption in the atmosphere can be used to infer the dry air density and used to calculate the dry air mixing ratio of a greenhouse gas, such as carbon dioxide or methane. OUT technique of measuring Oxygen uses integrated path differential absorption (IPDA) with an Erbium Doped Fiber Amplifier (EDF A) laser system and single photon counting module (SPCM). It measures the absorbance of several on- and off-line wavelengths tuned to an O2 absorption line in the A-band at 764.7 nm. The choice of wavelengths allows us to maximize the pressure sensitivity using the trough between two absorptions in the Oxygen A-band. Our retrieval algorithm uses ancillary meteorological and aircraft altitude information to fit the experimentally obtained lidar O2 line shapes to a model atmosphere and derives the pressure from the profiles of the two lines. We have demonstrated O2 measurements from the ground and from an airborne platform. In this paper we will report on our airborne measurements during our 2011 campaign for the ASCENDS program.

Riris, Haris↗
DOE OSTI2021

Monte Carlo Modeling and Design of Photon Energy Attenuation Layers for >10× Quantum Yield Enhancement in Si-Based Hard X-ray Detectors

High-energy (>20 keV) X-ray photon detection at high quantum yield, high spatial resolution, and short response time has long been an important area of study in physics. Scintillation is a prevalent method but limited in various ways. Directly detecting high-energy X-ray photons has been a challenge to this day, mainly due to low photon-to-photoelectron conversion efficiencies. Commercially available state-of-the-art Si direct detection products such as the Si charge-coupled device (CCD) are inefficient for >10 keV photons. Here, we present Monte Carlo simulation results and analyses to introduce a highly effective yet simple high-energy X-ray detection concept with significantly enhanced photon-to-electron conversion efficiencies composed of two layers: a top high-Z photon energy attenuation layer (PAL) and a bottom Si detector. We use the principle of photon energy down conversion, where high-energy X-ray photon energies are attenuated down to ≤10 keV via inelastic scattering suitable for efficient photoelectric absorption by Si. Our Monte Carlo simulation results demonstrate that a 10–30× increase in quantum yield can be achieved using PbTe PAL on Si, potentially advancing high-resolution, high-efficiency X-ray detection using PAL-enhanced Si CMOS image sensors.

47 OTHER INSTRUMENTATION↗
NASA NTRS1990

An intercomparison of airborne nitrogen dioxide instruments

Results on NO2 instruments are reported from the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 (CITE 2) program in summer 1986. The instruments tested were (1) a two-photon LIF system using a laser for NO2-NO photolysis, (2) a chemiluminescence (CL) detector using FeSO4 for NO2-NO conversion, (3) a CL detector using an arc lamp for NO2-NO photolysis, and (4) a tunable-laser-diode multipath-absorption system. The procedures for the CITE 2 ground-based and flight tests are described in detail, and the results are presented in extensive graphs. Instrument (2) was eliminated because the FeSO4 converted atmospheric PAN to NO, resulting in spuriously high NO2 values. The remaining instruments gave readings in 30-40-percent agreement at NO2 mixing ratios of 100-200 parts per trillion by volume (pptv). At ratios below 50 pptv, the correlation among the measurements was very poor, with a tendency for system (4) to give higher values than (1) or (3).

Gregory, G. L.↗
DOE OSTI2023

Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH 3 I probed by coincident ion momentum imaging

The UV-induced photodissociation dynamics of iodomethane (CH 3 I) in its A-band are investigated by time-resolved coincident ion momentum imaging using strong-field ionization as a probe. The delay-dependent kinetic energy distribution of the photofragments resulting from double ionization of the molecule maps the cleavage of the carbon–iodine bond and shows how the existence of a potential well in the di-cationic potential energy surfaces shapes the observed distribution at small pump–probe delays. Furthermore, the competition between single- and multi-photon excitation and ionization of the molecule is studied as a function of the intensity of the UV-pump laser pulse. Two-photon excitation to Rydberg states is identified by tracking the transformation of the delay-dependent singly-charged iodomethane yield from a pure Gaussian distribution at low intensity to a Gaussian with an exponentially decaying tail at higher intensities. In conclusion, dissociative ionization induced by absorption of three UV photons is resolved as an additional delay-dependent feature in the kinetic energy of the fragment ions detected in coincidence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗