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Vacuum-ultraviolet absorption cross-sections of functionalized four-carbon species
Absorption cross-sections were measured in the vacuum ultraviolet from 5.17 – 9.92 eV using differential absorption spectroscopy for 33 four-carbon species: n-butane, trans-2-butene, cis-2-butene, butanal, butyric acid, ethyloxirane, trans-2,3-dimethyloxirane, cis-2,3-dimethyloxirane, 2-methyloxetane, 2,2'-bioxirane, vinyl oxirane, 3,4-epoxybutan-2-one, diacetyl, diethyl ether, ethyl vinyl ether, vinyl acetate, acetic anhydride, 1-butanol, 3-buten-1-ol, 1–hydroxy-butan-2-one, 1–hydroxy-butan-3-one, 2,3-epoxybutan-1-ol, 3,4-epoxybutan-1-ol, 2-oxetanemethanol, butanone, methyl vinyl ketone, 4H-1,3-dioxine, allyl formate, 2-oxobutanal, 4-hydroxybutanal, 2-methyloxetan-3-one, cis–but-2-en-1-ol, and trans-2–but-enal. Uncertainties were quantified in all cases by accounting for errors in gas-phase concentration, experimental repeatability, and signal-to-noise ratio as a function of photon energy. With the exception of 2-oxobutanal, which is reported with an uncertainty of 10%, convolving the sources of error using the root-sum-square method led to an upper limit of 5% uncertainty above the detection limit, which is largely attributable to chemical purity. Here, the primary objective of the present work is to provide absolute cross-sections along with quantified uncertainty limits. The majority of the absorption spectra, which reflect electronic transitions such as σ → σ* and n → σ*, are reported for the first time and provide insight into fundamental chemical physics, such as vibrational band structure and Rydberg transitions. The quantitative spectra in the present work facilitates the discovery of chemical intermediates that support improvement in the accuracy of computational models for low-temperature combustion and atmospheric chemistry.
Ozone Depletion Potential of CH3Br
The ozone depletion potential (ODP) of methyl bromide (CH3Br) can be determined by combining the model-calculated bromine efficiency factor (BEF) for CH3Br and its atmospheric lifetime. This paper examines how changes in several key kinetic data affect BEF. The key reactions highlighted in this study include the reaction of BrO + H02, the absorption cross section of HOBr, the absorption cross section and the photolysis products of BrON02, and the heterogeneous conversion of BrON02 to HOBR and HN03 on aerosol particles. By combining the calculated BEF with the latest estimate of 0.7 year for the atmospheric lifetime of CH3Br, the likely value of ODP for CH3Br is 0.39. The model-calculated concentration of HBr (approximately 0.3 pptv) in the lower stratosphere is substantially smaller than the reported measured value of about I pptv. Recent publications suggested models can reproduce the measured value if one assumes a yield for HBr from the reaction of BrO + OH or from the reaction of BrO + H02. Although the DeAlore et al. evaluation concluded any substantial yield of HBr from BrO + HO2 is unlikely, for completeness, we calculate the effects of these assumed yields on BEF for CH3Br. Our calculations show that the effects are minimal: practically no impact for an assumed 1.3% yield of HBr from BrO + OH and 10% smaller for an assumed 0.6% yield from BrO + H02.
Ozone Depletion Potential of CH3Br
The ozone depletion potential (ODP) of methyl bromide (CH3Br) can be determined by combining the model-calculated bromine efficiency factor (BEF) for CH3Br and its atmospheric lifetime. This paper examines how changes in several key kinetic data affect BEF. The key reactions highlighted in this study include the reaction of BrO + HO2, the absorption cross section of HOBr, the absorption cross section and the photolysis products of BrONO2, and the heterogeneous conversion of BrONO2 to HOBr and HNO3 on aerosol particles. By combining the calculated BEF with the latest estimate of 0.7 year for the atmospheric lifetime of CH3Br, the likely value of ODP for CH3Br is 0.39. The model-calculated concentration of HBr (approx. 0.3 pptv) in the lower stratosphere is substantially smaller than the reported measured value of about 1 pptv. Recent publications suggested models can reproduce the measured value if one assumes a yield for HBr from the reaction of BrO + OH or from the reaction of BrO + HO2. Although the evaluation concluded any substantial yield of HBr from BrO + HO2 is unlikely, for completeness, we calculate the effects of these assumed yields on BEF for CH3Br. Our calculations show that the effects are minimal: practically no impact for an assumed 1.3% yield of HBr from BrO + OH and 10% smaller for an assumed 0.6% yield from BrO + HO2.
Derivation of water vapour absorption cross-sections in the red region
Absorption spectrum in 436 to 448 nm wavelength region gives NO2 and O3 column densities. This spectrum can also give H2O column density. The spectrum in the range of 655 to 667 nm contains absorption due to NO3 and H2O. Combining the absorption spectra in the wavelength ranges of 436 to 448 and 655 to 667 nm, water vapor absorption cross-sections in this range comes out to be of the order of 2.0 x 10(exp -24) cm(exp -2).
Measurement of the ozone absorption cross-section at the 253.7 nm mercury line
The absorption cross-section of ozone at 253.7 nm is frequently used as a standard for the entire UV wavelength range. The presently accepted value is 1.147 x 10 to the -17th/sq cm, which is known with an uncertainty of about 2 percent. The cross-section has been recently measured by simultaneously monitoring the ozone pressure, the impurities in the ozone gas, the gas temperature, and the UV beam intensity. The cross-section at room temperature was found to be 1.137 x 10 to the -17th/sq cm having an uncertainty of + or - .7 percent. The improved accuracy will aid a number of ozone experiments including the in situ photometers and Solar Backscatter Ultraviolet instruments.
Absorption Cross-Sections of Ozone in the Ultraviolet and Visible Spectral Regions: Status report 2015
The activity Absorption Cross-Sections of Ozone (ACSO) started in 2008 as a joint initiative of the International Ozone Commission (IO3C), the World Meteorological Organization (WMO) and the IGACO (Integrated Global Atmospheric Chemistry Observations) O3/UV subgroup to study, evaluate, and recommend the most suitable ozone absorption cross-section laboratory data to be used in atmospheric ozone measurements. The evaluation was basically restricted to ozone absorption cross-sections in the UV range with particular focus on the Huggins band. Up until now, the data of Bass and Paur published in 1985 (BP, 1985) are still officially recommended for such measurements. During the last decade it became obvious that BP (1985) cross-section data have deficits for use in advanced space-borne ozone measurements. At the same time, it was recognized that the origin of systematic differences in ground-based measurements of ozone required further investigation, in particular whether the BP (1985) cross-section data might contribute to these differences. In ACSO, different sets of laboratory ozone absorption cross-section data (including their dependence on temperature) of the group of Reims (France) (Brion et al., 1993, 1998, 1992, 1995, abbreviated as BDM, 1995) and those of Serdyuchenko et al. (2014), and Gorshelev et al. (2014), (abbreviated as SER, 2014) were examined for use in atmospheric ozone measurements in the Huggins band. In conclusion, ACSO recommends:(a) The spectroscopic data of BP (1985) should no longer be used for retrieval of atmospheric ozone measurements.(b) For retrieval of ground-based instruments of total ozone and ozone profile measurements by the Umkehr method performed by Brewer and Dobson instruments data of SER (2014) are recommended to be used. When SER (2014) is used, the difference between total ozone measurements of Brewer and Dobson instruments are very small and the difference between Dobson measurements at AD and CD wavelength pairs are diminished.(c) For ground-based Light Detection and Ranging (LIDAR) measurements the use of BDM (1995) or SER (2014) is recommended.(d) For satellite retrieval the presently widely used data of BDM (1995) should be used because SER (2014) seems less suitable for retrievals that use wavelengths close to 300 nm due to a deficiency in the signal-to-noise ratio in the SER (2014) dataset.The work of ACSO also showed: The need to continue laboratory cross-section measurements of ozone of highest quality. The importance of careful characterization of the uncertainties of the laboratory measurements. The need to extend the scope of such studies to other wavelength ranges (particularly to cover not only the Huggins band but also the comparison with the mid-infrared region). The need for regular cooperation of experts in spectral laboratory measurements and specialists in atmospheric (ozone) measurements.
High resolution absorption cross-sections and band oscillator strengths of the Schumann-Runge absorption bands of isotopic oxygen, (O-18)2, at 79 K
Cross-sections of (O-18)2 at 79 K have been obtained from photoabsorption measurements at various pressures throughout the wavelength region 177.8-197.8 nm with a 6.65 m photoelectric scanning spectrometer equipped with a 2400 lines/mm grating and having an instrumental width (FWHM) of 0.0013 nm. The measured absorption cross-sections of the Schumann-Runge bands (14,0) through (2,0) are, with the exception of the (12,0) band, independent of the instrumental width. The measured cross-sections are presented graphically here and are available at wavenumber intervals of about 0.1/cm as numerical compilations stored on magnetic tape. Band oscillator strengths of those bands have been determined by direct numerical integration of the measured absolute cross-sections and are in excellent agreement with these theoretically calculated values.
Measuring Two Key Parameters of H3 Color Centers in Diamond
A method of measuring two key parameters of H3 color centers in diamond has been created as part of a continuing effort to develop tunable, continuous-wave, visible lasers that would utilize diamond as the lasing medium. (An H3 color center in a diamond crystal lattice comprises two nitrogen atoms substituted for two carbon atoms bonded to a third carbon atom. H3 color centers can be induced artificially; they also occur naturally. If present in sufficient density, they impart a yellow hue.) The method may also be applicable to the corresponding parameters of other candidate lasing media. One of the parameters is the number density of color centers, which is needed for designing an efficient laser. The other parameter is an optical-absorption cross section, which, as explained below, is needed for determining the number density. The present method represents an improvement over prior methods in which optical-absorption measurements have been used to determine absorption cross sections or number densities. Heretofore, in order to determine a number density from such measurements, it has been necessary to know the applicable absorption cross section; alternatively, to determine the absorption cross section from such measurements, it has been necessary to know the number density. If, as in this case, both the number density and the absorption cross section are initially unknown, then it is impossible to determine either parameter in the absence of additional information.
Fabrication and Atomic Force Microscopy Characterization of Molecular Composites of Fullerenes in Aerogel Matrix for Optical Limiting
An optical limiter is a device which exhibits a decrease in the transmittance in a material with an increase in intensity of light. Sol-gel techniques offer many advantages in the fabrication of materials. These materials possess many desirable properties for nonlinear optical (NLO) device applications which include transparency, high thermal and chemical stabilities, very low refractive index and dielectric constants. C60 shows a higher excited state absorption cross section than the ground state absorption cross section over the complete visible spectrum, and the spectrum of the excited state absorption of C60 has the same general shape as the ground state absorption. This fact suggests that fullerenes are ideal optical limiting materials. Aerogels are fabricated by sol-gel processing. One of the key issues is the dispersion of fullerenes into small and uniform pores of silica aerogel host matrices. The aerogel network was characterized by Raman spectroscopy. Atomic force microscopy is a technique with many advantages to characterize the aerogel materials. The morphology of the cleaved surface for a C60/aerogel sample shows that there are long paralleled shaped stripes with 20-30 nm in width and about 500 nm in length on the cleaved surface. The cleaved surface also was etched by 5% HF solution for one minutes, and it became smoother after HF etching. The main feature in on the surface is the spherical particles with the size of few nanometers, and no aggregated fullerenes appear. The fullerenes are well dispersed in the aerogel matrices.
High resolution absorption cross-sections and band oscillator strengths of the Schumann-Runge absorption bands of isotopic oxygen, (0-16)(0-18), at 79 K
Cross-sections of (0-16)(0-18) at 79 K have been obtained from photoabsorption measurements on mixtures of (0-16)2, (0-18)2, and (0-16)(0-18) at various pressures throughout the wavelength region 180.5-195.3 nm with a 6.65 m photoelectric scanning spectrometer equipped with a 2400 lines/mm grating and having an instrumental width (FWHM) of 0.0013 nm. The measured absorption cross-sections of the (0-16)(0-18) Schumann-Runge bands (11.0)-(3.0) are independent of the instrumental width. The measured cross-sections are presented graphically.
Ultraviolet absorption cross-sections of some carbonyl compounds and their temperature dependence
Ultraviolet absorption cross-section of phosgene (CCl2O), trichloroacetylchloride (CCl3-CClO) and trichloroacetaldehyde (CCl3-CHO) have been measured between 170 and 320 nm for temperature ranging from 210 to 295 K with classical double beam equipment. These data are compared with other available determinations performed at room temperature. Photodissociation coefficients are estimated and their temperature dependence is discussed. Impact of the photodissociation on the total atmospheric destruction of these compounds is illustrated.
Measurement of the absorption cross-sections of CFC-11 at conditions representing various model atmospheres
Absorption cross-sections, K(sub V)(/(cm)(atm)), have been measured in the 9.2 and 11.8 micrometer bands of CFC-11 (CCl3F) using a high-resolution Fourier transform spectrometer. Temperature and total (N2-broadening) pressure have been varied to obtain results at conditions representative of the atmosphere. The measured absolute intensities (in units of 10(exp -17) cm/molecule of the 9.2 and 11.8 micrometer bands are 2.591 +/- 0.013 and 6.974 +/- 0.038, respectively.
Airborne differential absorption lidar system for measurements of atmospheric water vapor and aerosols
An airborne differential absorption lidar (DIAL) system has been developed at the NASA Langley Research Center for remote measurements of atmospheric water vapor (H2O) and aerosols. A solid-state alexandrite laser with a 1-pm linewidth and greater than 99.85% spectral purity was used as the on-line transmitter. Solid-state avalanche photodiode detector technology has replaced photomultiplier tubes in the receiver system, providing an average increase by a factor of 1.5-2.5 in the signal-to-noise ratio of the H2O measurement. By incorporating advanced diagnostic and data-acquisition instrumentation into other subsystems, we achieved additional improvements in system operational reliability and measurement accuracy. Laboratory spectroscopic measurements of H2O absorption-line parameters were performed to reduce the uncertainties in our knowledge of the absorption cross sections. Line-center H2O absorption cross sections were determined, with errors of 3-6%, for more than 120 lines in the 720-nm region. Flight tests of the system were conducted during 1989-1991 on the NASA Wallops Flight Facility Electra aircraft, and extensive intercomparison measurements were performed with dew-point hygrometers and H2O radiosondes. The H2O distributions measured with the DIAL system differed by less than 10% from the profiles determined with the in situ probes in a variety of atmospheric conditions.
Estimating mass-absorption cross-section of ambient black carbon aerosols: theoretical, empirical, and machine learning models
The mass-absorption cross-section of black carbon (MAC BC ) is an essential parameter to link the atmospheric concentration of black carbon (BC) with its radiative forcing. When a direct calculation of MAC BC based on observations of aerosol light absorption and BC mass concentration is impossible, we rely on modeling and simulations to estimate MAC BC , but currently, there is no consensus model that can be relied on for accurate predictions across all atmospheric environments when BC particles have different coating thicknesses. Here, we applied five MAC BC prediction models (including three light scattering theories, an empirical model based on observations of particle mass concentrations, and a machine learning model developed in our previous work) to aerosols from three Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) field campaigns. While many studies have found that increasing the complexity of the models helps to constrain biases of the estimated MAC BC , our effort is to evaluate the models based on the criteria of simplicity and accuracy. We find that our machine learning model (support vector machine for regression, SVM) generally performs well across all DOE ARM field campaign data, while the accuracy of core-shell Mie theory depends on the bias correction algorithm applied to filter-based light absorption data. Generally, the empirical model for internally-mixed particles that we considered tends to over-predict MAC BC , while Mie theory for externally-mixed particles tends to under-predict MAC BC . An examination of the influence of coating material on BC cores suggests that the performance of our current SVM model is degraded when the BC is thickly-coated (e.g., it has undergone aging and mixing with other materials in the atmosphere).
High resolution absorption cross-sections and band oscillator strengths of the Schumann-Runge bands of oxygen at 79 K
Cross sections of O2 at 79 K have been obtained from photoabsorption measurements at various pressures throughout the wavelength region 179.3-198.0 nm with a 6.65-m photoelectric scanning spectrometer equipped with a 2400-lines/mm grating and having an instrumental width (FWHM) of 0.0013 nm. The measured absorption cross sections of the Schumann-Runge bands (12,0) through (2,0) are independent of the instrumental width. The measured cross-sections are presented graphically here and are available at wavenumber intervals of about 0.1/cm as numerical compilations stored on magnetic tape from the National Space Science Data Center, NASA/Goddard. Band oscillator strengths of these bands have been determined by direct numerical integration of the measured cross sections.
Absolute absorption cross-section measurements of ozone in the wavelength region 238-335 nm and the temperature dependence
The absolute absorption cross-section of ozone has been experimentally determined at the temperatures 195, 228, and 295 K at several discrete wavelengths in the 238-335-nm region. The present results for ozone at 295 K are found to be in agreement with those of Hearn (1961). Absolute cross-section measurements of ozone at 195 K have confirmed previous (Freeman et al., 1984) relative cross-section measurements throughout the 240-335-nm region.
Improved absorption cross-sections of oxygen in the wavelength region 205-240 nm of the Herzberg continuum
The laboratory values of the Herzberg continuum absorption cross-section of oxygen at room temperature from Cheung et al. (1986) and Jenouvrier et al. (1986) are compared and analyzed. It is found that there is no discrepancy between the absolute values of these two sets of independent measurements. The values are combined in a linear least-squares fit to obtain improved values of the Herzberg continuum cross-section of oxygen at room temperature throughout the wavelength region 205-240 nm. The results are compared with in situ and other laboratory measurements.