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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 163 records · Page 9

Autioionizing states in the photionization of the 3s(2)3p(4) (3)Pe ground state of sulfur

The partial and total photoionization cross sections for the S(3s/2/3p/4/ /3/Pe) ground state are calculated in both the dipole length and velocity forms. The prominent features in the cross sections are the autoionization Rydberg series converging to S+(3s/2/p/3/ /2/D/0/, /2/P/0/) excited-state thresholds. The results are pertinent to the study of sulfur in the plasma of Jupiter's satellite Io.

Tayal, S. S.↗

A heat-driven monochromatic light source

The efficiency with which heat may be converted into resonance radiation in a cesium thermionic diode is investigated theoretically. An analytical model of a thermionic converter is used which combines the coupled effects of line radiation transport, excited-state kinetics, and plasma diffusion. Operating regimes are established for various degrees of optical density in the plasma. The results indicate that monochromatic radiation can be produced with efficiencies on the order of 30 percent, provided that there is an adequate voltage drop across the plasma. A drop of 1 V was used since it can be maintained without any electrical power input to the device. It is found that high efficiencies are ude to the higher interelectrode distances which the solutions accommodate, and that radiation can be generated efficiently, even with optically dense gases.

Stefani, Francis↗

Frequency and intensity analysis of the nu3, nu4, and nu6 bands of formaldehyde

The infrared spectra of the nu3, nu4, and nu6 bands of formaldehyde in the region from 890/cm to 1580/cm have been obtained at high resolution using tunable diode laser and Fourier transform-infrared spectroscopy. The transition frequencies have been analyzed using a Hamiltonian including terms through sextic in centrifugal distortion and including five interstate vibration-rotation coupling terms. Excited-state pure rotational transitions are also included in the data, and their frequencies are reproduced well. Individual measured line intensities are used to determine dipole derivatives and band strengths using the fully coupled, asymmetric top eigenvectors.

Reuter, D. C.↗

Excited state absorption of pump radiation as a loss mechanism in solid-state lasers

The characteristics of optical pumping dynamics in laser-pumped, rare-earth-doped, solid-state laser materials are investigated by using a tunable alexandrite laser to pump Y3Al5O12:Nd(3+) in an optical cavity. It is found that the slope efficiency of the Nd laser operation depends strongly on the wavelength of the pump laser. For pump wavelengths resulting in low slope efficiencies, intense fluorescence emission is observed from the sample in the blue-green spectral region. This is attributed to the excited-state absorption of pump photons which occurs during radiationless relaxation from the pump band to the metastable state. This type of process is an important loss mechanism for monochromatic pumping of laser systems at specific pump wavelengths.

Kliewer, Michael L.↗

Determination of molecular spectroscopic parameters and energy-transfer rates by double-resonance spectroscopy

The spectroscopy of small to medium-size polyatomic molecules can be extremely complex, especially in higher-lying overtone and combination vibrational levels. The high density of levels also complicates the understanding of inelastic collision processes, which is required to model energy transfer and collision broadening of spectral lines. Both of these problems can be addressed by double-resonance spectroscopy, i.e., time-resolved pump-probe measurements using microwave, infrared, near-infrared, and visible-wavelength sources. Information on excited-state spectroscopy, transition moments, inelastic energy transfer rates and propensity rules, and pressure-broadening parameters may be obtained from such experiments. Examples are given for several species of importance in planetary atmospheres, including ozone, silane, ethane, and ammonia.

Steinfeld, J. I.↗

Photophysics of poly(2,3,4,5,6-pentafluoro styrene) film

The temperature-dependent steady-state emission, emission polarization anisotropy, and fluorescence-kinetics of poly(2,3,4,5,6-pentafluoro styrene) film are reported. Two interconverting excited-state conformations of the chromophore have been identified. The fluorescence of the higher energy conformation results from excitation on the red edge of the polymer absorption band at temperatures below 180 K. The energy barrier for conversion of the high energy conformer to the lower energy conformer is estimated to be E/hc = 27 + or - 7/cm. Electronic energy migration is not evident in this polymer.

O'Connor, Donald B.↗

Effective gain measurements in chromium-doped forsterite

Effective gain cross section in tetravalent chromium-doped forsterite laser crystal was measured over the 1180-1330 nm spectral range. The experiment was performed using two collinear laser beams in a pump-and-probe arrangement. The peak-gain cross section from this measurement is estimated to be 1.9 x 10 to the -19th sq cm at 1215 nm, which is comparable to the value of about 2 x 10 to the -19th sq cm predicted by fluorescence linewidth and lifetime measurements. These results indicate that excited-state absorption is not a major loss mechanism in tetravalent chromium-doped forsterite.

Petricevic, V.↗

Inelastic collision processes in ozone and their relation to atmospheric pressure broadening

The research task employs infrared double-resonance to determine rotational energy transfer rates and pathways, in both the ground and vibrationally excited states of ozone. The resulting data base will then be employed to test inelastic scattering theories and to assess intermolecular potential models, both of which are necessary for the systematization and prediction of infrared pressure-broadening coefficients, which are in turn required by atmospheric ozone monitoring techniques based on infrared remote sensing. In addition, observation of excited-state absorption transitions will permit us to improve the determination of the 2 nu(sub 3), nu(sub 1) + nu(sub 2), and 2 nu(sub 1) rotational constants and to derive band strengths for hot-band transitions involving these levels.

Steinfeld, J. I.↗

The electronic structure and second-order nonlinear optical properties of donor-acceptor acetylenes - A detailed investigation of structure-property relationships

A series of donor-acceptor acetylene compounds was synthesized in which systematic changes in both the conjugation length and the donor-acceptor strength were made. The effect of these structural changes on the spectroscopic and electronic properties of the molecules and, ultimately, on the measured second-order molecular hyperpolarizabilities (beta) was investigated. It was found that increases in the donor-acceptor strength resulted in increases in the magnitude of beta. For this class of molecules, the increase is dominated by the energy of the intramolecular charge-transfer transition, while factors such as the ground to excited-state dipole moment change and the transition-moment integral are much less important. Increasing the conjugation length from one to two acetylene linkers did not result in an increase in the value of beta; however, beta increased sharply in going from two acetylenes to three. This increase is attributed to the superposition of several nearly isoenergetic excited states.

Stiegman, A. E.↗

Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines

Direct measurements are reported of the excited singlet-state absorption cross section and the associated nonlinear refractive cross section using picosecond pulses at 532 nm in solutions of phthalocyanine and naphthalocyanine dyes. By monitoring the transmittance and far-field spatial beam distortion for different pulsewidths in the picosecond regime, it is shown that both the nonlinear absorption and refraction are fluence (energy-per-unit-area) rather than irradiance dependent. Thus, excited-state absorption is the dominant nonlinear absorption process, and the observed nonlinear refraction is also due to real population excitation.

Wei, T. H.↗

Coherent laser excitation of Ba-137 and Ba-138

Computations are carried out for the 1S(6s2)-1P(6s,6p) coherent laser excitation of Ba-137 and Ba-138 in a magnetic field. Results are presented for both the steady-state and time-dependent excited-state populations of the Zeeman-split magnetic sublevels. The quantum-statistical Liouville-equation approach (for the reduced density matrix) is compared to the rate-equations approach. Significant differences are found between these, due to the interference between strongly overlapping lines (especially for Ba-137). The time-evolution profiles indicate that the Ba-137 transient time is much longer than that of Ba-138.

Lam, Kai-Shue↗

Plume characteristics of an arcjet thruster

An experimental investigation is conducted of the plume of a 1.5 kW hydrogen-fueled arcjet thruster. The velocity and translational temperature are measured by laser induced fluorescence of excited-state atomic hydrogen at a variety of locations and operating conditions. The peak velocity and temperature at the center of the exit plane of 14.7 km/s and 5000 K lead to a Mach number of 1.9. Evidence is presented which demonstrates the extent to which viscous forces dominate the flow, such as the exit plane Reynolds number of 18. Data taken in the plume suggest a transition from supersonic to subsonic flow via viscous dissipation. In addition, the results suggest that high tank pressures (0.4 to 1.5 Torr) limit the ability to simulate space environments for different portions of the plume.

Liebeskind, John G.↗

Investigation of infra-red and nonequilibrium air radiation

This report describes progress on the first year of a research program on the infrared radiation of air plasmas conducted in the High Temperature Gasdynamics Laboratory at Stanford University. This program is intended to investigate the masking of infrared signatures by the air plasma formed behind the bow shock of high velocity missiles. To this date, the radiative emission of air plasmas in the infrared has been the object of few experimental investigations, and although several infrared systems are already modeled in radiation codes such as NEQAIR, measurements are required to validate numerical predictions and indicate whether all transitions of importance are accounted for. The present program is motivated by the fact that 9 excited states (A, B, C, D, B', F, H, and H') of NO radiate in the infrared, especially between 1 and 1.5 microns where at least 9 transitions involving can be observed. Because these IR transitions are relatively well separated from each other, excited NO states concentrations can be easily measured, thus providing essential information on excited-state chemistry for use in optical diagnostics or in electronic excitation model validation. Developing accurate collisional-radiative models for these excited NO states is of importance as the UV-VUV transitions of NO (beta, gamma, epsilon, beta prime, gamma prime) produce a major, if not dominant, fraction of the radiation emitted by air plasmas. During the first year of the program, research has focused on the spectral range 1.0 to 1.5 microns, as detailed in Section 2 of this report. The measurements, conducted in a 50 kW radio-frequency inductively coupled plasma torch operating on air at atmospheric pressure, extend previous shock tube investigations by Wray to a wider spectral range (1.0 to 1.5 microns vs 0.9 to 1.2 microns) and higher temperatures (7600 K in the plasma torch versus 6700 K in the shock-tube). These higher temperatures in the present experiment have made it possible to observe high-lying excited NO states that were previously undetectable. These measurements are currently being extended up to 5 microns, with particular attention paid to the rovibronic bands of ground state NO, molecular continua, CO transitions, and other systems of importance. Publications and presentations resulting from or related to this work are cited in Section 3, and Section 4 lists the personnel who contributed to this report.

Kruger, Charles H.↗

Photodissociation of cyanoacetylene: Application to the atmospheric chemistry of Titan

The quantum yield and reaction threshold for the photochemical dissociation of cyanoacetylene into a hydrogen atom and the cyanoethynyl radical have been determined. The quantum yield at 185 nm is approximately 0.09. The threshold is approximately 240 nm. Combination of this data with literature values shows that production of excited-state cyanoacetylene is the major primary process resulting from irradiation between 185 and 254 nm. Also determined are the relative rate constants for the abstraction of a hydrogen atom from hydrogen, methane, and ethane by the cyanoethynyl radical (k(H2):k(CH4):k(C2H6) = 1:9.3:63). Implications of these results for the proposal that hydrogen abstraction plays an important role in the conversion of methane to ethane and in the protection of unsaturated compounds from photoconsumption in the atmosphere of Titan are discussed.

Clarke, David W.↗

Investigation of Infra-red and Nonequilibrium Air Radiation

This report summarizes the results obtained during a research program on the infrared radiation of air plasmas conducted in the High Temperature Gasdynamics Laboratory at Stanford University. This program was intended to investigate the masking of infrared signatures by the air plasma formed behind the bow shock of high velocity missiles. Prior to this work, the radiative emission of air plasmas in the infrared had been the object of few experimental investigations, and although several infrared systems were already modeled in radiation codes such as NEQAIR, measurements were required to validate numerical predictions and indicate whether all transitions of importance were accounted for in the model. The program was further motivated by the fact that 9 excited states (A, B, C, D, B', F, H, and H') of NO radiate in the infrared, especially between 1 and 1.5 microns where at least 9 transitions involving can be observed. Because these IR transitions are relatively well separated from each other, excited NO states concentrations can be easily measured, thus providing essential information on excited-state chemistry for use in optical diagnostics or in electronic excitation model validation. Detailed comparisons between measured and simulated spectra are presented.

Kruger, Charles H.↗

Correlations in alpha-alpha scattering and semi-classical optical models

We show the equivalence of semi-classical solutions to optical model coupled-channel equations derived from Watson's form of the nucleus-nucleus multiple-scattering series to the Glauber multiple-scattering series. A second-order solution to the semi-classical coupled-channel elastic amplitude is shown to be nearly equivalent to a second-order optical-phase-shift approximation to the Glauber amplitude if the densities of all nuclear excited states are approximated by the ground-state density. Using the Jastrow method to model the two-body density we find an average excited-state density to be of negligible importance in the double-scattering region of alpha-alpha scattering.

NASA Discipline Number 04-10↗

Enhanced Reverse Saturable Absorption and Optical Limiting in Heavy-Atom Substituted Phthalocyanines

The reverse saturable absorption and optical limiting response of metal phthalocyaninies can be enhanced by using the heavy-atom effect. Phthalocyanines containing heavy metal atoms, such as In, Sn, and Pb show nearly a factor of two enhancement in the ratio of effective excited-state to ground-state absorption cross sections compared to those containing lighter atoms, such as Al and Si. In an f/8 optical geometry, homogeneous solutions of heavy metal phthalocyanines, at 30% linear transmission, limit 8-ns, 532-nm laser pulses to less than or equal to 3 (micro)J (the energy for 50% probability of eye damage) for incident pulses up to 800 (micro)J.

metal phthalocyanines↗

Dissipation Enables Strongly Detuning-Dependent Interference in Pulsed Dynamical Decoupling

One of the defining features of pulsed dynamical decoupling is its suppression of a driven qubit's sensitivity to static detuning errors between the drive field and qubit resonance. In this paper, we show that dissipation, in the form of excited-state decay, can change this behavior entirely, producing an interference signal with a strong detuning dependence. This signal arises from decay during driven evolution and relies on coherence retained by the qubit after such a decay event. We develop analytical and numerical models that capture the underlying mechanism and observe this same dissipation-induced detuning dependence experimentally in both a free-space strontium atom interferometer and a superconducting transmon qubit system. We also use this dissipation-induced detuning dependence as the basis for a new spectroscopic technique called Dissipative Carr-Purcell Spectroscopy (DCPS) and compare it with a traditional Ramsey sequence. Our results establish a regime of pulsed dynamical decoupling in which dissipation reshapes, rather than merely degrades, coherent control, and we expect these dynamics to be relevant to a wide range of quantum systems.

DeRose, Kenneth [Northwestern U.; Fermilab] (ORCID↗