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At least 73 records · Page 4

Electronic spectroscopy of diatomic molecules

This article provides an overview of the principal computational approaches and their accuracy for the study of electronic spectroscopy of diatomic molecules. We include a number of examples from our work that illustrate the range of application. We show how full configuration interaction benchmark calculations were instrumental in improving the understanding of the computational requirements for obtaining accurate results for diatomic spectroscopy. With this understanding it is now possible to compute radiative lifetimes accurate to within 10% for systems involving first- and second-row atoms. We consider the determination of the infrared vibrational transition probabilities for the ground states of SiO and NO, based on a globally accurate dipole moment function. We show how we were able to assign the a(sup "5)II state of CO as the upper state in the recently observed emission bands of CO in an Ar matrix. We next discuss the assignment of the photoelectron detachment spectra of NO and the alkali oxide negative ions. We then present several examples illustrating the state-of-the-art in determining radiative lifetimes for valence-valence and valence-Rydberg transitions. We next compare the molecular spectroscopy of the valence isoelectronic B2, Al2, and AlB molecules. The final examples consider systems involving transition metal atoms, which illustrate the difficulty in describing states with different numbers of d electrons.

Partridge, Harry↗

Micro Raman Spectroscopy for Characterizing Molecular Contamination on Space Flight Hardware

In the field of contamination control,many unknowns exist. Often, contamination control engineers have to utilize multiple spectroscopic, macroscopic, and microscopic tools to identify contamination sources when there is a potential contamination exposure to space flight hardware. Understanding the chemical composition of the molecular contamination provides an opportunity for contamination control engineers to determine if this contamination is problematic or benign. In this study, an existing witness plate program for monitoring space flight hardware during the assembly, integration, and testing phases is coupled with micro Raman spectroscopy analysis. The main goal of this study is to determine the limitations, reproducibility, and throughput of micro Raman spectroscopy for characterizing molecular contamination. Micro Raman Spectroscopy will be an additional tool used by contamination control engineers to monitor the cleanliness of space flight hardware.

Microscope↗

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tandem bulk oxygen diffusion and surface reactions in reducible metal oxides control redox cycle dynamics

The interplay between bulk oxygen diffusion and surface reactions in reducible metal oxides is key in heterogeneous catalysts, but direct measurements of oxygen mobility, transient kinetics, and in situ spectroscopies have been lacking. Here, we reveal complex dynamic behavior of ceria-zirconia by H 2 using transient kinetics via mass spectrometry and in situ Raman and near-ambient pressure x-ray photoelectron spectroscopies. Molecular dynamics simulations with a machine learning potential delineate competitive oxygen diffusion mechanisms, with an optimal mobility at intermediate reductions. We expose a compensation between vacancy availability and lattice distortion at intermediate to high reductions and Frenkel defects at low reductions, underscoring a potential deficiency of 16 O/ 18 O exchange experiments in deducing oxygen mobility. Vacancies in proximity require electron localization on Ce atoms further away. The continuous replenishment of surface oxygen results in a varying reduction rate, with H 2 dissociation being the rate-limiting step. Multiscale transient simulations, consistent with experiments, indicate catalysts of potentially spatially varying oxidation states. The approach is broadly applicable to reducible oxide materials.

36 MATERIALS SCIENCE↗

Parity-doublet coherence times in optically trapped polyatomic molecules

Polyatomic molecules provide complex internal structures that are ideal for applications in quantum information science, quantum simulation and precision searches for physics beyond the standard model. A key feature of polyatomic molecules is the presence of parity-doublet states. These structures, which generically arise from the rotational and vibrational degrees of freedom afforded by polyatomic molecules, are a powerful feature to pursue diverse quantum science applications. Linear triatomic molecules contain ℓ-type parity-doublet states in the vibrational bending mode, which are predicted to exhibit robust coherence properties. Here we report optically trapped CaOH molecules prepared in ℓ-type parity-doublet states and realize a bare qubit coherence time of $T$$^{*}_{2}$, which is longer than the 0.36 s lifetime of the bending mode. We suppress differential Stark shifts by cancelling ambient electric fields using molecular spectroscopy and characterize parity-dependent trap shifts, which are found to limit the coherence time. Furthermore, the parity-doublet coherence times achieved in this work are a defining milestone for the use of polyatomic molecules in quantum science.

Quantum information↗

Supercontinuum generation in oxide and semiconductor materials (InP, Si, GaN, GaAs, PbMoO 4 , YVO 4 , ZGP, TiO 2 , diamond) pumped by radiation of the Cr:ZnS fs-MOPA system

Ultrashort light sources in the middle-infrared range are highly beneficial for applications such as gas molecular spectroscopy, remote sensing, atmospheric science, medical treatments, and light–matter interaction studies. Ultrafast lasers utilizing chromium-doped ZnS/Se (Cr:ZnS/Se) have proven to be robust and stable solutions within this spectral region. Nonlinear spectral broadening is fundamentally important, as it pushes the pulse duration limits imposed by the bandwidth of laser media. In this study, we demonstrate the spectral broadening and supercontinuum generation in several bulk materials, including InP, Si, GaN, GaAs, PbMoO 4 , YVO 4 , diamond, and TiO 2 , using pump radiation with up to 4 W average power centered at 2.35 µm from a Cr:ZnS femtosecond MOPA system. Some of the investigated materials have excellent potential as effective media for middle-infrared supercontinuum generation, demonstrating the feasibility of developing a single-cycle pulse middle-infrared laser system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Chemistry between the stars

A unit is presented for the secondary school teacher of physics, chemistry, astronomy, or earth sciences. Included are a list of reference materials, teaching aids, and projects. Discussion questions and a glossary are also provided. Concepts developed are: the nature of interstellar space, spectroscopy, molecular signals from space and interstellar molecules and other areas of astronomy.

Gammon, R. H.↗

Investigation of infrared spectra of atmospheric gases to support stratospheric spectroscopic investigations

Four papers are presented which discuss the following: information measures in nonlinear experimental design; information in spectra of collision broadened absorption lines; band analysis by spectral curve fitting; and least squares analysis of Voight shaped lines. Abstracts of five research papers on which the author collaborated and which were delivered at the 34th Symposium of Molecular Spectroscopy (Ohio State University, June 1979) are included along with a subroutine for use with BMDP3R to retrieve the parameters of 10 Voight shaped lines.

Shaw, J. H.↗

Laboratory Research

To properly interpret the rapidly growing body of data from comet observations, many types of laboratory measurements are needed. These include: (1) molecular spectroscopy in the visible, ultraviolet, infrared and microwave region of the spectra; (2) laser fluorescent spectroscopy of photofragments; (3) laboratory cross-section or reaction rate measurements using flow tube techniques, fluorescent spectroscopy detection for neutrals and ion-molecule reaction techniques; (4) experiments to simulate solar-wind interactions with comets; (5) studies of the properties and behavior of ice mixtures; (6) experiments on the sublimation rate of ice, and the phase transition from amorphous to crystalline ice; (7) investigations of the irradiation of ice; and (8) the electron impact dissociation and excitation of molecules of cometary interest. A nearly completed experiment on the proton irradiation of ice is described.

Donn, B.↗

Optically pumped submillimeter-waves and applications

Rapid development of optically pumped lasers has shown the potential to be used as a source for a high resolution spectrometer. In this connection, a compact, stable FIR laser was designed, fabricated, and assembled, integrating both the pump laser and the FIR cavity in the same mechanical structure for its improved (both thermal and mechanical) stability and mobility. Performance of the mixer structure which was designed and constructed for the evaluation of the Schottky diodes was found to be satisfactory. The feasibility of generating tunable sideband for molecular spectroscopy studies was demonstrated.

Dutta, J. M.↗

A high-resolution atlas of the infrared spectrum of the Sun and the Earth atmosphere from space: A compilation of ATMOS spectra of the region from 650 to 4800 cm (2.3 to 16 micron). Volume 1: The Sun

During the period April 29 through May 2, 1985, the Atmospheric Trace Molecular Spectroscopy experiment was operated as part of the Spacelab-3 payload of the shuttle Challenger. The instrument, a modified Michelson Interferometer covering the frequency range from 600 to 5000/cm, at a spectral resolution of 0.01/cm, recorded infrared spectra of the Sun and of the Earth's atmosphere at times close to entry into and exit from occultation by the Earth's limb as seen from the shuttle orbit of 360 km. Spectra were obtained that are free from absorptions due to constituents of the atmosphere (i.e., solar pure spectra), as well as spectra of the atmosphere itself, covering line-of-sight tangent altitudes that span the range from the lower thermosphere to the bottom of the troposphere. This atlas, believed to be the first record of observations of the continuous high resolution infrared spectrum of the Sun and the Earth's atmosphere from space, provides a compilation of these spectra arranged in a hardcopy format suitable for quick-look reference purposes; the data are also available in digital form.

Farmer, Crofton B.↗

Analysis of pressure-broadened ozone spectra in the 3 micron region

The Molecular Spectroscopy Lab at NASA-Langley has been involved in a long term effort to carefully characterize the infrared spectra of small molecules of atmospheric interest, including methane, water vapor, ozone, and their isotopic counterparts. High resolution gas phase infrared spectra are obtained using both a tunable diode laser system, and the McMath Fourier transform spectrometer at the Kitt Peak Solar Observatory. Spectra are obtained at various pressures and temperatures for pure gas samples, and for samples containing mixtures of the species of interest in nitrogen, oxygen, or air. From these spectra, using a nonlinear least squares fitting technique, spectral parameters of position, intensity, and half-width were determined for varying laboratory conditions that approximate atmospheric conditions experienced in remote sensing situations. These parameters are of interest in theoretical studies of these species, as well as in allowing more accurate interpretation of remote sensing data. The current work involves the analysis of a series of McMath FTIR spectra of ozone broadened by mixing with air, nitrogen, or oxygen. Each spectrum covers the region from 2396 to 4057/cm. Each vibrational band is analyzed by first diving its region into small intervals containing a few well isolated absorption lines of reasonable intensity. Each of these small intervals is fit by multiple iterations of the nonlinear least square program until residuals are minimized to a reasonable value which corresponds to the noise level of the measured spectrum. Intervals for the 3 nu(sub 3) ozone band in the region from 3000 to 3060 wavenumbers are being examined.

Prochaska, Eleanor S.↗

Tunable Electro-optic modulators for lidar systems and atmospheric applications

In global sensing applications using different types of lidars, the spectral range and fine frequency coverages are often limited because of the finite tunabilities of molecular lasers and the number of molecular species that are available. To overcome the above obstacle, we have proposed new broadband frequency tunable electro-optic (EO) modulators that can cover a wide range from the mid-infrared to the visible as lidar sources in atmospheric sensing applications such as high resolution atmospheric molecular spectroscopy, Differential Absorption Lidar (DIAL), and laser radar imaging. The configuration of the proposed new tunable EO modulators includes an electro-optic active crystal element surrounded by a ferrite tuning element which is placed inside a microwave waveguide. The tuning is provided by an external magnetic field, which is either longitudinal or transverse, and the modulator can be either single sideband type or a double sideband type depending on the application required for the spectral purity of the modulator output.

Eng, R. S.↗

The solar spectrum

The UV-IR solar spectrum is presented and discussed with a view to the comparative value of the data and their application in atomic or molecular spectroscopy and in solar, atmospheric, planetary, cometary, or stellar physics. Attention is given to intensity spectra, terrestrial atmospheric spectra, the 296-1300 nm Solar Flux Atlas of Kurucz et al. (1984), and line identifications.

Kurucz, Robert L.↗

Middle and upper atmosphere pressure-temperature profiles and the abundances of CO2 and CO in the upper atmosphere from ATMOS/Spacelab 3 observations

An improved method for retrieving pressure-temperature profiles is described and is used to retrieve profiles of the kinetic-temperature and atmospheric-pressure profiles between 20 and 116 km altitudes and the CO2 and CO volume-mixing ratios between 70 and 116 km, using the IR occultation spectra recorded by the Spacelab 3 atmospheric trace molecular spectroscopy (ATMOS) Fourier transform spectrometer between April 29 and May 6, 1985. Profiles are derived for six ATMOS occultations. The CO2 and CO volume-mixing profiles are compared with previous observations and model predictions. Evidence is found for vibrational non-LTE by analyzing the lines of the (nu-2 + nu-3 - nu-2) (C-12)(O-16) band. Results are used for deriving (C-12)(O-16) (010) vibrational temperatures, which are compared with the retrieved kinetic temperatures and the predictions of non-LTE effects by recent models.

Rinsland, C. P.↗

Exploration of the solar system by infrared remote sensing

The remote sensing of objects in the solar system using infrared radiation is discussed. Theories of radiative transfer, molecular spectroscopy, and atmospheric physics are used to show how infrared spectra of model planetary atmospheres are calculated. Instrumental techniques are described and the effect of instruments on the measurement of the emerging radiation field is addressed. Techniques that allow the retrieval of atmospheric and surface parameters from observations are examined. All the planets except Pluto are studied, and many of the planetary satellites.

Hanel, R. A.↗

Space physics educational outreach

The goal of this Space Physics Educational Outreach project was to develop a laboratory experiment and classroom lecture on Earth's aurora for use in lower division college physics courses, with the particular aim of implementing the experiment and lecture at Saint Mary's College of California. The strategy is to teach physics in the context of an interesting natural phenomenon by investigating the physical principles that are important in Earth's aurora, including motion of charged particles in electric and magnetic fields, particle collisions and chemical reactions, and atomic and molecular spectroscopy. As a by-product, the undergraduate students would develop an appreciation for naturally occurring space physics phenomena.

Copeland, Richard A.↗

Atmospheric Sulfur Cycle Effects of Carbonyl Sulfide (OCS)

Carbonyl Sulfide(OCS) is considered to be one of the major sources of sulfur appearing in the stratosphere due to its relative inertness, about I to 10 yearsl. However, the roles of OCS as well as other reduced sulfur compounds such as carbon disulfide (CS2), hydrogen sulfide (H2S), and dimethyl disulfide(CH3)2S2, are not completely understood in the atmosphenc sulfur cycle. Consequently vely little information is available about the effect of sulfur compounds in the stratosphere. The ability of OCS to penetrate into the stratosphere makes it an excellent tracer for study of the role of the sulfi r cycle in stratospheric chemistry. Previously techniques such as gas chromatography and whole air sampling have been used to measure OCS analytically. Each technique had its drawbacks however, with both being quite slow, and whole air sampling being somewhat unreliable. With molecular spectroscopy, however, it has been found in recent years that the tunable diode laser absorption spectrometer (TDL) provides a very rapid and accurate method of measuring OCS and other trace gases

McBee, Joshua↗