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NASA NTRS1981

Theoretical quasar emission line ratios. IV - General asymptotic escape probabilities and the effects of linear Stark broadening

Established techniques permitting the evaluation of exact asymptotic forms of photon escape probabilities for a wide range of absorption coefficient profile types are used for QSO radiative transfer effect studies, and it is shown that the exact formulae are easily evaluated. It is found that some of the commonly used expressions overestimate the true value by a factor of about two, and a computationally expedient approximate expression is derived for the asymptotic form of the photon escape probability when linear Stark broadening contributes to the line absorption coefficient profile in hydrogenic lines. Attention is given to Lyman-alpha, for the case in which partial redistribution, over the linear Stark component of the line absorption coefficient profile, dominates single-flight photon escape.

Puetter, R. C.↗

DOE OSTI2020

Fine structure of the isovector giant dipole resonance in Nd 142 – 150 and Sm 152

Inelastic proton scattering at energies of a few hundred MeV and very-forward scattering angles including 0° has been established as a tool for the study of electric-dipole strength distributions in nuclei. The present work reports a systematic investigation of the chain of stable even-mass Nd isotopes representing a transition from spherical to quadrupole-deformed nuclei. Extraction of the equivalent photo-absorption cross sections and analysis of their fine structure in the energy region of the isovector giant dipole resonance (IVGDR). Method: Proton inelastic scattering reactions of 200 MeV protons were measured at the iThemba Laboratory for Accelerator Based Sciences in Cape Town, South Africa. The scattering products were momentum-analyzed by the K600 magnetic spectrometer positioned at θ Lab = 0°. Using dispersion-matching techniques, energy resolutions of ΔE ≈ 40–50 keV (full width at half maximum) were obtained. After subtraction of background and contributions from other multipoles, the spectra were converted to photoabsorption cross sections using the equivalent virtual-photon method. Wavelet-analysis techniques are used to extract characteristic energy scales of the fine structure of the IVGDR from the experimental data. Fine structure of the IVGDR is observed even for the most deformed nuclei studied. Comparisons between the extracted experimental energy scales and those energy scales obtained from the quasiparticle-phonon model (QPM) and Skyrme separable random phase approximation (SSRPA) predictions provide insight into the role of different giant-resonance damping mechanisms. It can be seen that the scales in the spherical and most likely also in the deformed nuclei mainly result from the fragmentation of the one-particle-one-hole (1p1h) strength into several dominant transitions serving as doorway states. In cases where calculations beyond the 1p1h level are available, some impact of the spreading due to coupling of the two-particle-two-hole (2p2h) states to the 1p1h doorway states is observed. New virtual-photon absorption data for the chain of stable Nd isotopes and 152 Sm are presented, with a focus on the phenomenon of nonstatistical cross-section fluctuations, referred to as fine structure, in the energy region of the IVGDR. The wavelet-analysis techniques used allowed for the features of the fine structure to be quantified in the form of characteristic scales. Finally, comparisons between experimental results and model predictions indicate that Landau damping seems to be the main source of the fine structure in both the spherical and deformed nuclei, but calculations including 2p2h degrees of freedom would be beneficial to confirm this for the deformed cases.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRS2003

X-ray single Photon Spectrometers

The research at Yale on superconducting tunnel junctions (STJs) focussed on x-ray detectors, using a 5.9 keV x-ray source. All the Yale tests were carried out at 0.21 K, in a two-stage helium 3 dewar. Careful attention was given to grounding and shielding. All current waveforms were digitially recorded and analyzed subsequently on computer. The imaging device geometry was studied. This allows imaging along the length of the tantalum (Ta) absorber, which is 600 nm thick to provide good x-ray absorption. The quasiparticles produced by single photon absorption rapidly cool to the Ta gap, E(sub g_Ta) = 1.4 meV, and then diffuse. They are trapped in the A1 traps at the two ends (E(sub g_A1) = 0.4 meV), to give two charges that tunnel out of the A1 traps, Q(sub 1) and Q(sub 2). The total charge is Q = Q(sub 1) + Q(sub 2). This lateral trapping is what allows imaging.

Prober, Daniel↗

NASA NTRS1984

Fluorescence from photofragments as an aid in identifying new molecular states - The N2 case

Synchrotron radiation has been used to measure the excitation function for producing fluorescence in the 1050-1800 A region through photodissociative excitation of N2 in the 400-620 A region and the photoabsorption cross section of N2 in the 600-670 A region. From the fluorescence excitation function there is found (1) a molecular state(s) in the 21-22.5 eV region which has not been observed in absorption and photoionization spectra, (2) structures which correlate with known two-electron excited Rydberg states, and (3) a decrease in fluorescence cross section at photon energies greater than 23.8 eV, which indicates the existence of new competing processes. The observed molecular state(s) as well as the weak absorption structure in the 19-21 eV region are tentatively assigned as a Rydberg series leading to the D2Pi(g) of N2(+). The newly observed Rydberg states in the 21-22.5 eV region may account for the unusual behavior recently reported in photoelectron spectroscopy results.

Wu, C. Y. R.↗

NASA NTRS1994

The Hubble Space Telescope quasar absorption line key project. 6: Properties of the metal-rich systems

We present an analysis of the properties of a sample of 18 metal-rich, low-redshift z(sub abs) much less than z(sub em) absorbers seen in low- and medium-resolution spectra obtained for the Quasar Absorption Line Key Project with the Hubble Space Telescope Faint Object Spectrograph (HST/FOS). For most of the C IV and Lyman-limit systems, observations in the optical wavelength range of the expected associated Mg II absorption are available. As at high redshift (z approximately 2), there are two subclasses of absorbers which are characterized by the presence or absence of MG II absorption. However, some low-redshift Mg II and Fe absorptions originate from regions optically thin to UV ionizing photons and thus, at low redshift, the low-ionization systems do not always trace high opacities, as is the case at high redshift. This implies that the mean ionization state of metal-rich, optically thin absorbing clouds falls with decreasing redshift, which is consistent with the hypothesis that the gas is photoionized by the metagalactic UV background radiation field. Two main constraints are derived from the analysis of the Lyman-limit sample, assuming photoionization models are valid. First, a low opacity to ionizing photons (tau(sub LL) approximately less than 1), as observed for several Mg II-Fe II systems at z approximately 0.5, sets limits on the ionization level of hydrogen, thus on the total hydrogen column density and the heavy element abundances, (Z/H) approximately -0.5 to -0.3. Second, the dimensions of individual Mg II clouds are smaller than at high redshift by a factor 3-10. At z approximately greater than 0.6, the O VI absorption doublet is detected in four of the five z(sub abs) much less than z(sub em) systems for which the O VI wavelength range has been observed, whereas the associated N V doublet is detected in only two cases. This suggests that the presence of a high-ionization O VI phase is a general property of z approximately 0.6-1 absorption systems, as is also probably the case at high redshift. These O VI absorbers can be ionized by the UV metagalactic field if their density is low, nH approximately less than 3 x 10(exp -4)/cc. The O VI phase would then be a homogeneous region of large extent, r approximately greater than 50 kpc. A detailed photoionization model of the z(sub abs) = 0.791 absorber toward PKS 2145+06 confirms the properties derived from the Mg II, C IV, O VI, and Lyman-limit samples. The galaxy causing this extensive metal-line absorption system has been identified, and its possible contribution to the UV ionizing flux does not substantially modify the value of the derived parameters. The heavy element abundances are about half the solar values. The O VI region has a density about 20 times lower than the Mg II clouds and a size of approximately 70 kpc. Alternatively, the high-ionization phase could be collisionally ionized and trace gas associated with a possible group of galaxies at the absorber redshift.

Bergeron, Jacqueline↗

DOE OSTI2022

Room-Temperature Optical Detection of 14 CO 2 below the Natural Abundance with Two-Color Cavity Ring-Down Spectroscopy

Radiocarbon’s natural production, radiative decay, and isotopic rarity make it a unique tool to probe carbonaceous systems in the life and earth sciences. However, the difficulty of current radiocarbon ( 14 C) detection methods limits scientific adoption. Here, two-color cavity ring-down spectroscopy detects 14 CO 2 in room-temperature samples with an accuracy of one-tenth the natural abundance in 3 min. The intracavity pump–probe measurement uses two cavity-enhanced lasers to cancel out cavity ring-down rate fluctuations and strong one-photon absorption interference (>10 000 1/s) from hot-band transitions of CO 2 isotopologues. Selective, room-temperature detection of small 14 CO 2 absorption signals (<1 1/s) reduces the technical and operational burdens for cavity-enhanced measurements of radiocarbon, which can benefit a wide range of applications like biomedical research and field-detection of combusted fossil fuels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1989

Fast molecular shocks. I - Reformation of molecules behind a dissociative shock

The physical and chemical processes that operate in the cooling gas behind a fast, dissociative, single-fluid shock propagating in a dense interstellar cloud are discussed. The treatment extends previous theoretical work on fast molecular shocks by including the effects of the conversion of Ly-alpha photons into radiation of the two-photon continuum and into H2 Lyman band emission lines, the effects of CO photodissociation following line absorption, and the formation and destruction of molecules containing the elements nitrogen, silicon, and sulphur, and of the complex hydrocarbons. Abundance profiles for the molecular species of interest are presented. After molecular hydrogen begins to reform, by means of gas phase and grain surface processes, the neutral species OH, H2O, O2, CO, CN, HCN, N2, NO, SO, and SiO reach substantial abundances. The molecular ions HeH(+), OH(+), SO(+), CH(+), H2(+), and H3(+), are produced while the gas is still hot and partially ionized. Emissions from them provide a possible diagnostic probe of fast molecular shocks.

Neufeld, David A.↗

DOE OSTI2024

Argon metastable density and temperature of a 94 GHz microplasma

Laser diode absorption spectroscopy is used to experimentally measure Ar(1s 5 ) metastable density and translational gas temperature within a 94 GHz microplasma. A square two-dimensional photonic crystal (PhC) at this resonance frequency serves to ignite and sustain the plasma from 20 to 200 Torr (2.7 × 10 3 –2.7 × 10 4 Pa) by using millimeter wave power from 300 to 1000 mW. Metastable density within the plasma is estimated from the absorption line shape of the laser traversing the PhC. The metastable density reaches an order of 10 19 m –3 at lower pressure and decreases as pressure increases. From the Lorentzian line shape of the absorption profile at 811.53 nm, the gas temperature is extracted and found to increase from 500 K at 20 Torr to 1300 K at 200 Torr. Furthermore, these data are analyzed and compared with a zero-dimensional plasma model and with previous experimental plasma results at 43 GHz.

42 ENGINEERING↗

DOE OSTI2020

Table-Top X-ray Spectroscopy of Benzene Radical Cation

Herein, ultrafast table-top X-ray spectroscopy at the carbon K-edge is used to measure the X-ray spectral features of benzene radical cations (Bz + ). The ground state of the cation is prepared selectively by two-photon ionization of neutral benzene, and the X-ray spectra are probed at early times after the ionization by transient absorption using X-rays produced by high harmonic generation (HHG). Bz + is well-known to undergo Jahn-Teller distortion, leading to a lower symmetry and splitting of the π orbitals. Comparison of the X-ray absorption spectra of the neutral and the cation reveals a splitting of the two degenerate π* orbitals as well as an appearance of a new peak due to excitation to the partially occupied π-subshell. The π* orbital splitting of the cation, elucidated on the basis of high-level calculations in a companion theoretical paper, is discovered to be due to both the symmetry distortion and even more dominant spin coupling of the unpaired electron in the partially vacant π orbital (from ionization) with the unpaired electrons resulting from the transition from the 1s C core orbital to the fully vacant π* orbitals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2009

nBn Infrared Detector Containing Graded Absorption Layer

It has been proposed to modify the basic structure of an nBn infrared photodetector so that a plain electron-donor- type (n-type) semiconductor contact layer would be replaced by a graded n-type III V alloy semiconductor layer (i.e., ternary or quarternary) with appropriate doping gradient. The abbreviation nBn refers to one aspect of the unmodified basic device structure: There is an electron-barrier ("B" ) layer between two n-type ("n" ) layers, as shown in the upper part of the figure. One of the n-type layers is the aforementioned photon-absorption layer; the other n-type layer, denoted the contact layer, collects the photocurrent. The basic unmodified device structure utilizes minority-charge-carrier conduction, such that, for reasons too complex to explain within the space available for this article, the dark current at a given temperature can be orders of magnitude lower (and, consequently, signal-to-noise ratios can be greater) than in infrared detectors of other types. Thus, to obtain a given level of performance, less cooling (and, consequently, less cooling equipment and less cooling power) is needed. [In principle, one could obtain the same advantages by means of a structure that would be called pBp because it would include a barrier layer between two electron-acceptor- type (p-type) layers.] The proposed modifications could make it practical to utilize nBn photodetectors in conjunction with readily available, compact thermoelectric coolers in diverse infrared- imaging applications that could include planetary exploration, industrial quality control, monitoring pollution, firefighting, law enforcement, and medical diagnosis.

Gunapala, Sarath D.↗

DOE OSTI2023

Multimessenger signals of heavy axionlike particles in core-collapse supernovae: Two-dimensional simulations

Core-collapse supernovae are a useful laboratory to probe the nature of exotic particles. If axionlike particles (ALPs) are produced in supernovae, they can affect the transfer of energy and leave traces in observational signatures. In this work, we present results from two-dimensional supernova models including the effects of the production and the absorption of ALPs that couple with photons. It is found that the additional heating induced by ALPs can enhance the diagnostic energy of explosion, E diag . For example, for moderate ALP-photon coupling, we find explosion energies ~0.6×10 51 erg compared to our reference model without ALPs of ~0.4×10 51 erg in the first ~0.5 s postbounce explored in this work. Further, our findings indicate that when the coupling constant is sufficiently high, the neutrino luminosities and mean energies are decreased because of the additional cooling of the proto-neutron star via ALPs. The gravitational wave amplitude is also reduced because the mass accretion on the proto-neutron star is suppressed. Although the ALP-photon coupling can foster explodability, including enhancing the explosion energy closer to recent observations, more long-term simulations in three spatial dimensions are needed to draw robust conclusions.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS2000

Nebular Hydrogen Absorption in the Ejecta of Eta Carinae

Space Telescope Imaging Spectrograph (STIS) observations of Eta Carinae and immediate ejecta reveal narrow Balmer absorption lines in addition to the nebular-scattered broad P-Cygni absorptions. The narrow absorption correlates with apparent disk structure that separates the two Homunculus lobes. We trace these features about half way up the Northern lobe until the scattered stellar Balmer line doppler-shifts redward beyond the nebular absorption feature. Three-dimensional data cubes, made by mapping the Homunculus at Balmer alpha and Balmer beta with the 52 x 0.1 arcsecond aperture and about 5000 spectral resolving power, demonstrate that the absorption feature changes slowly in velocity with nebular position. We have monitored the stellar Balmer alpha line profile of the central source over the past four years. The equivalent width of the nebular absorption feature changes considerably between observations. The changes do not correlate with measured brightness of Eta Carinae. Likely clumps of neutral hydrogen with a scale size comparable to the stellar disk diameter are passing through the intervening light path on the timescales less than several months. The excitation mechanism involves Lyman alpha radiation (possibly the Lyman series plus Lyman continuum) and collisions leading to populating the 2S metastable state. Before the electron can jump to the ground state by two photon emission (lifetime about 1/8 second), a stellar Balmer photon is absorbed and the electron shifts to an NP level. We see the absorption feature in higher Balmer lines, and but not in Paschen lines. Indeed we see narrow nebular Paschen emission lines. At present, we do not completely understand the details of the absorption. Better understanding should lead to improved insight of the unique conditions around Eta Carinae that leads to these absorptions.

Gull, Theodore R.↗

NASA NTRS1990

H2/O2 three-body rates at high temperatures

The extraction of thrust from air breathing hypersonic propulsion systems is critically dependent on the degree to which chemical equilibrium is reached in the combustion process. In the combustion of H2/Air mixtures, slow three-body chemical reactions involving H-atoms, O-atoms, and the OH radical play an important role in energy extraction. A first-generation high temperature and pressure flash-photolysis/laser-induced fluorescence reactor was designed and constructed to measure these important three-body rates. The system employs a high power excimer laser to produce these radicals via the photolysis of stable precursors. A novel two-photon laser-induced fluorescence technique is employed to detect H-atoms without optical thickness or O2 absorption problems. To demonstrate the feasibility of the technique the apparatus in the program is designed to perform preliminary measurements on the H + O2 + M reaction at temperatures from 300 to 835 K.

Marinelli, William J.↗

DOE OSTI2020

Extrinsic Absorption Pathways in Vanadium-Doped SiC Measured Using a Total Internal Reflection Geometry

Vanadium-doped SiC is under study for high-power photoconductive switches and is receiving increased attention as a potential material system for quantum computing, as the V can act as a quantum emitter at telecom wavelengths. Knowledge of the defect-mediated electronic transition pathways from sub-bandgap illumination in this material with low absorption and multi-photon and multi-path transition probability is important in optimizing quantum efficiency. Herein, the optical transitions of vanadium-doped SiC for two polytypes as a function of dopant concentration using a total internal reflection (TIR) geometry are examined. Furthermore, normalized quantum efficiency is reported and correlated with both dopant concentrations (V, N, B, and Al) measured by secondary ion mass spectroscopy (SIMS) and absorption measurements. Although both polytypes respond well to 532 nm light, efficiency at longer wavelengths does not correlate 1:1 with absorption coefficient and strongly depends on the polytype and net background co-dopant concentration. This has important implications for efficient excitation of both carriers for optoelectronics and for the use of V as a quantum emitter.

36 MATERIALS SCIENCE↗

NASA NTRS1991

H2/O2 three-body rates at high temperatures

Hydrogen atoms are produced in the presence of excess O2, and the first-order decay are studied as a function of temperature and pressure in order to obtain the rate coefficient for the three-body reaction between H-atoms and O2. Attention is focused on the kinetic scheme employed as well as the reaction cell and photolysis and probe laser system. A two-photon laser-induced fluorescence technique is employed to detect H-atoms without optical-thickness or O2-absorption problems. Results confirm measurements reported previously for the H + O2 + N2 reaction at 300 K and extend these measurements to higher temperatures. Preliminary data indicate non-Arrehenius-type behavior of this reaction rate coefficient as a function of temperature. Measurements of the rate coefficient for H + O2 + Ar reaction at 300 K give a rate coefficient of 2.1 +/- 0.1 x 10 to the -32nd cm exp 6/molecule sec.

Marinelli, William J.↗

DOE OSTI2021

Regio‐Regular Polymer Acceptors Enabled by Determined Fluorination on End Groups for All‐Polymer Solar Cells with 15.2 % Efficiency

Abstract Polymerization sites of small molecule acceptors (SMAs) play vital roles in determining device performance of all‐polymer solar cells (all‐PSCs). Different from our recent work about fluoro‐ and bromo‐ co‐modified end group of IC‐FBr (a mixture of IC‐FBr1 and IC‐FBr2), in this paper, we synthesized and purified two regiospecific fluoro‐ and bromo‐ substituted end groups (IC‐FBr‐ o & IC‐FBr‐ m ), which were then employed to construct two regio‐regular polymer acceptors named PYF‐T‐ o and PYF‐T‐ m , respectively . In comparison with its isomeric counterparts named PYF‐T‐ m with different conjugated coupling sites, PYF‐T‐ o exhibits stronger and bathochromic absorption to achieve better photon harvesting. Meanwhile, PYF‐T‐ o adopts more ordered inter‐chain packing and suitable phase separation after blending with the donor polymer PM6, which resulted in suppressed charge recombination and efficient charge transport. Strikingly, we observed a dramatic performance difference between the two isomeric polymer acceptors PYF‐T‐ o and PYF‐T‐ m . While devices based on PM6:PYF‐T‐ o can yield power conversion efficiency (PCE) of 15.2 %, devices based on PM6:PYF‐T‐ m only show poor efficiencies of 1.4 %. This work demonstrates the success of configuration‐unique fluorinated end groups in designing high‐performance regular polymer acceptors, which provides guidelines towards developing all‐PSCs with better efficiencies.

Yu, Han↗

DOE OSTI2021

Regio‐Regular Polymer Acceptors Enabled by Determined Fluorination on End Groups for All‐Polymer Solar Cells with 15.2 % Efficiency

Yu, Han↗

DOE OSTI2022

Multipolariton control in attosecond transient absorption of autoionizing states

Tunable attosecond transient absorption spectroscopy is an ideal tool for studying and manipulating autoionization dynamics in the continuum. We investigate near-resonant two-photon couplings between the bright 3s –1 4p and dark 3s –1 4f autoionizing states of argon that lead to Autler-Townes-like interactions, forming entangled light-matter states or polaritons. We observe that one-photon couplings with intermediate dark states play an important role in this interaction, leading to the formation of multiple polaritonic branches whose energies exhibit avoided crossings as a function of the dressing-laser frequency. Our experimental measurements and theoretical essential-state simulations show good agreement and reveal how the delay, frequency, and intensity of the dressing pulse govern the properties of autoionizing polariton multiplets. Furthermore, these results demonstrate new pathways for quantum control of autoionizing states with optical fields.

74 ATOMIC AND MOLECULAR PHYSICS↗