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At least 487 records · Page 27

On the role of ozone in the stability of Rossby normal modes

The role of ozone in the linear stability of Rossby normal modes is examined in a continuously stratified, extratropical baroclinic atmosphere. The flow is described by coupled equations for the quasi-geostraphic potential vorticity and ozone volume mixing ratio. A perturbation analysis is carried out under the assumption of weak diabatic heating, which is generated by Newtonian cooling and dynamics-ozone interaction. An expression for the propagation and growth characteristics is obtained analytically in terms of the vertically averaged wave activity, which depends explicitly on the wave spatial structure, photochemistry, and basic state distributions of wind, temperature, and ozone mixing ratio. Calculations show that stationary internal modes, whose amplitudes are largest in the stratosphre, are destabilized by dynamics-ozone interaction and Newtonian cooling, with e-folding times on the order of 20-40 days.

Nathan, Terrence R.↗

Deriving Global OH Abundance and Atmospheric Lifetimes for Long-Lived Gases: A Search for CH3CCl3 Alternatives

An accurate estimate of global hydroxyl radical (OH) abundance is important for projections of air quality, climate, and stratospheric ozone recovery. As the atmospheric mixing ratios of methyl chloroform (CH3CCl3) (MCF), the commonly used OH reference gas, approaches zero, it is important to find alternative approaches to infer atmospheric OH abundance and variability. The lack of global bottom-up emission inventories is the primary obstacle in choosing a MCF alternative. We illustrate that global emissions of long-lived trace gases can be inferred from their observed mixing ratio differences between the Northern Hemisphere (NH) and Southern Hemisphere (SH), given realistic estimates of their NH-SH exchange time, the emission partitioning between the two hemispheres, and the NH versus SH OH abundance ratio. Using the observed long-term trend and emissions derived from the measured hemispheric gradient, the combination of HFC-32 (CH2F2), HFC-134a (CH2FCF3, HFC-152a (CH3CHF2), and HCFC-22 (CHClF2), instead of a single gas, will be useful as a MCF alternative to infer global and hemispheric OH abundance and trace gas lifetimes. The primary assumption on which this multispecies approach relies is that the OH lifetimes can be estimated by scaling the thermal reaction rates of a reference gas at 272 K on global and hemispheric scales. Thus, the derived hemispheric and global OH estimates are forced to reconcile the observed trends and gradient for all four compounds simultaneously. However, currently, observations of these gases from the surface networks do not provide more accurate OH abundance estimate than that from MCF.

Lifetime↗

Concentrations of carbonyl sulfide and hydrogen cyanide in the free upper troposphere and lower stratosphere deduced from ATMOS/Spacelab 3 infrared solar occultation spectra

This paper presents the results on the volume mixing ratio profiles of carbonyl sulfide and hydrogen cyanide, deduced from the spectroscopic analysis of IR solar absorption spectra obtained in the occultation mode with the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during its mission aboard Spacelab 3. A comparison of the ATMOS measurements for both northern and southern latitudes with previous field investigations at low midlatitudes shows a relatively good agreement. Southern Hemisphere volume mixing ratio profiles for both molecules were obtained for the first time, as were the profiles for the Northern Hemisphere covering the upper troposphere and the lower stratosphere simultaneously.

Zander, R.↗

H2O-H2SO4 system in Venus' clouds and OCS, CO, and H2SO4 profiles in Venus' troposphere

A coupled problem of diffusion and condensation is solved for the H2SO4-H2O system in Venus' cloud layer. The position of the lower cloud boundary, profiles of the H2O and H2SO vapor mixing ratios, and of the H2O/H2SO4 ratio of sulfuric acid aerosol and its flux are calculated as functions of the column photochemical production rate of sulfuric acid. Variations of the lower cloud boundary are considered. Our basic model, which is constrained to yield f(sub H2O)(30km) = 30 ppm, predicts the position of the lower cloud boundary at 48.4 km coinciding with the mean Pioneer Venus value, the peak H2SO4 mixing ratio of 5.4 ppm, and the H2SO4 production rate phi(sub H2SO4) = 2.2 x 10(exp 12) cm(exp -2)s(exp -1).

Krasnopolsky, V. A.↗

Validation of SAGE II NO2 measurements

The validity of NO2 measurements from the stratospheric aerosol and gas experiment (SAGE) II is examined by comparing the data with climatological distributions of NO2 and by examining the consistency of the observations themselves. The precision at high altitudes is found to be 5 percent, which is also the case at specific low altitudes for certain latitudes where the mixing ratio is 4 ppbv, and the precision is 0.2 ppbv at low altitudes. The autocorrelation distance of the smoothed profile measurement noise is 3-5 km and 10 km for 1-km and 5-km smoothing, respectively. The SAGE II measurements agree with spectroscopic measurements to within 10 percent, and the SAGE measurements are about 20 percent smaller than average limb monitor measurements at the mixing ratio peak. SAGE I and SAGE II measurements are slightly different, but the difference is not attributed to changes in atmospheric NO2.

Cunnold, D. M.↗

Optimization-based, property-preserving algorithm for passive tracer transport

Here we present a new optimization-based property-preserving algorithm for passive tracer transport. The algorithm utilizes a semi-Lagrangian approach based on incremental remapping of the mass and the total tracer. However, unlike traditional semi-Lagrangian schemes, which remap the density and the tracer mixing ratio through monotone reconstruction or flux correction, we utilize an optimization-based remapping that enforces conservation and local bounds as optimization constraints. In so doing we separate accuracy considerations from preservation of physical properties to obtain a conservative, second-order accurate transport scheme that also has a notion of optimality. Moreover, we prove that the optimization-based algorithm preserves linear relationships between tracer mixing ratios. We illustrate the properties of the new algorithm using a series of standard tracer transport test problems in a plane and on a sphere.

97 MATHEMATICS AND COMPUTING↗

Mesospheric ozone changes associated with 27-day solar ultraviolet flux variations

Solar ultraviolet flux changes associated with the 27-day solar rotational period cause corresponding variations in mesospheric ozone near the maximum of the 11-year sunspot cycle. This statement is based on a correlation and spectral analysis of ozone mixing ratios, deduced from Solar Mesospheric explorer satellite-based measurements of 1.27-micron O2 airglow emission and solar flux observations made from the same spacecraft in 1982. With the Lyman-alpha flux taken as an indicator of solar ultraviolet variability, spectral analysis shows a primary period of 27.1 days with a secondary period of 13.5 days. The 27.1-day period is observed in the ozone mixing ratio data together with other periods, including 13.5 days. Both a classical statistical analysis and a time series treatment show that, for 244 days, there is a correlation between ozone and solar flux near 50 km and between 65 and 70 km. Calculations predict a positive correlation over the entire mesosphere if there is no change in temperature accompanying the solar flux. Lack of correlation is temperature induced.

Aikin, A. C.↗

Identification and measurement of atmospheric ethane (C2H6) from a 1951 infrared solar spectrum

C2H6 absorption features in the 2980/cm spectral region of the solar spectrum recorded in April, 1951 were analyzed to determine the total vertical column amount and average free tropospheric mixing ratio of C2H6 above Jungfraujoch in the Swiss Alps. The PQ1 subbranch is the best isolated of the three C2H6 features in the 1951 spectrum, with an equivalent width of 0.0099 + or - 0.0025/cm. Results give a total vertical column amount of 9.7 x 10 to the 15th C2H6 molecules/sq cm, with an accuracy of + or - 30 percent. March 1981 measurements from this region give a mixing ratio of about 2.0 ppbv, 2.2 times larger than the 1951 value, suggesting a long-term increase in the free tropospheric C2H6 concentration over western Europe.

Rinsland, Curtis P.↗

Chemical Characteristics of Continental Outflow Over the Tropical South Atlantic Ocean from Brazil and Africa

The chemical characteristics of air parcels over the tropical South Atlantic during September - October 1992 are summarized by analysis of aged marine and continental outflow classifications. Positive correlations between CO and CH3CL and minimal enhancements of C2CL40, and various ChloroFluoroCarbon (CFC) species in air parcels recently advected over the South Atlantic basin strongly suggest an impact on tropospheric chemistry from biomass burning on adjacent continental areas of Brazil and Africa. Comparison of the composition of aged Pacific air with aged marine air over the South Atlantic basin from 0.3 to 12.5 km altitude indicates potential accumulation of long-lived species during the local dry season. This may amount to enhancements of up to two-fold for C2H6, 30% for CO, and 10% for CH3Cl. Nitric oxide and NO(x) were significantly enhanced (up to approx. 1 part per billion by volume (ppbv)) above 10 km altitude and poorly correlated with CO and CH3Cl. In addition, median mixing ratios of NO and NO(x) were essentially identical in aged marine and continental outflow air masses. It appears that in addition to biomass burning, lightning or recycled reactive nitrogen may be an important source of NO(x) to the upper troposphere. Methane exhibited a monotonic increase with altitude from approx. 1690 to 1720 ppbv in both aged marine and continental outflow air masses. The largest mixing ratios in the upper troposphere were often anticorrelated with CO, CH3Cl, and CO2, suggesting CH, contributions from natural sources. We also argue, based on CH4/CO ratios and relationships with various hydrocarbon and CFC species, that inputs from biomass burning and the northern hemisphere are unlikely to be the dominant sources of CO, CH4 and C2H6 in aged marine air. Emissions from urban areas would seem to be necessary to account for the distribution of at least CH4 and C2H6. Over the African and South American continents an efficient mechanism of convective vertical transport coupled with large-scale circulations conveys biomass burning, urban, and natural emissions to the upper troposphere over the South Atlantic basin. Slow subsidence over the eastern South Atlantic basin may play an important role in establishing and maintaining the rather uniform vertical distribution of long-lived species over this region. The common occurrence of values greater than 1 for the ratio CH3OOH/H2O2 in the upper troposphere suggests that precipitation scavenging effectively removed highly water soluble gases (H2O2, HNO3, HCOOH, and CH3COOH) and aerosols during vertical convective transport over the continents. However, horizontal injection of biomass burning products over the South Atlantic, particularly water soluble species and aerosol particles, was frequent below 6 km altitude.

Talbot, R. W.↗

The Liquid-Water Oscillation in Modeling Boundary-Layer Cumuli with Third-Order Turbulence Closure Models

A hierarchy of third-order turbulence closure models are used to simulate boundary-layer cumuli in this study. An unrealistically strong liquid-water oscillation (LWO) is found in the fully prognostic model, which predicts all third moments. The LWO propagates from cloud base to cloud top with a speed of 1 m/s. The period of the oscillation is about 1000 s. Liquid-water buoyancy terms in the third-moment equations contribute to the LWO. The LWO mainly affects the vertical profiles of cloud fraction, mean liquid-water mixing ratio and the fluxes of liquid-water potential temperature and total water, but has less impact on the vertical profiles of other second-moments and third-moments. In order to minimize the LWO, a moderate large diffusion coefficient and a large turbulent dissipation at its originating level are needed. However, this approach distorts the vertical distributions of cloud fraction and liquid-water mixing ratio. A better approach is to parameterize liquid-water buoyancy more reasonably. A minimally prognostic model, which diagnoses all third moments except for vertical velocity, is shown to produce better results, compared to a fully prognostic model.

Cheng, A.↗

First Measurements of the HCFC-142b Trend from Atmospheric Chemistry Experiment (ACE) Solar Occultation Spectra

The first measurement of the HCFC-142b (CH3CClF2) trend near the tropopause has been derived from volume mixing ratio (VMR) measurements at northern and southern hemisphere mid-latitudes for the 2004-2008 time period from spaceborne solar occultation observations recorded at 0.02/cm resolution with the ACE (atmospheric chemistry experiment) Fourier transform spectrometer. The HCFC-142b molecule is currently the third most abundant HCFC (hydrochlorofluorocarbon) in the atmosphere and ACE measurements over this time span show a continuous rise in its volume mixing ratio. Monthly average measurements at northern and southern hemisphere midlatitudes have similar increase rates that are consistent with surface trend measurements for a similar time span. A mean northern hemisphere profile for the time span shows a near constant VMR at 8-20km altitude range, consistent on average for the same time span with in situ results. The nearly constant vertical VMR profile also agrees with model predictions of a long lifetime in the lower atmosphere.

Rinsland, Curtis P.↗

Measurements of mesospheric water vapor in 1984 and 1985 - Results and implications for middle atmospheric transport

The detailed results of ground-based mesospheric water vapor measurements obtained by microwave spectroscopy at the Jet Propulsion Laboratory (JPL) from December 1984 to April 1985 (JPL 1984/85), and an overview of results obtained the previous year from April to June 1984 are presented. The JPL 1984/85 spectral data appeared to contain an instrumental baseline curvature which was bracketed and removed. In general, the JPL 1984/85 results are in good agreement with those of previous measurements. They indicate water vapor mixing ratios between 6 and 8 ppmv at 60 or 65 km and falling off steeply with height above this point to values of less than 2 ppmv at 80 km. In addition, there is a large amount of day-to-day variability indicated in the data. A major result of the study is that it is found that both the observed vertical gradient of water vapor mixing ratio and its seasonal variation are consistent with the hypothesis that vertical transport time scales are smaller, perhaps by an order of magnitude, than values currently used in both one- and two-dimensional photochemical/dynamical models.

Bevilacqua, Richard M.↗

Simultaneous measurement of minor stratospheric constituents with emission far-infrared spectroscopy

The vertical mixing ratio profiles of H2O, HDO, O3, heavy ozone, HF, HCl, HCN, and OH in the stratosphere are retrieved from high-resolution far-infrared emission spectra. These spectra were obtained with a balloon-borne Fourier transform spectrometer in the spring of 1979 at 32 deg N. The nonlinear least squares fit method is used in the analysis. The results are obtained relative to the O2 mixing ratio, whose emission features can be found in the same spectra. The retrieval of OH together with other species should be particularly significant for the study of upper stratospheric photochemistry, although the errors are relatively large: 28 percent for OH and 16-19 percent for other species.

Carli, Bruno↗

Water Vapor in Titan's Stratosphere from Cassini/CIRS Far-infrared Spectra

Since the first detection of water vapor in Titan's stratosphere by disk-average observations from the Infrared Space Observatory (Coustenis et al. 1998) we report here the successful detection of stratospheric water vapor using the Cassini Composite Infrared Spectrometer (CIRS, Flasar et al. 2004). CIRS senses water emissions in the far infrared spectral region near 50 microns, which we have modeled using two independent radiative transfer codes (NEMESIS, Irwin et al 2008 and ART, Coustenis et al. 2007, 2010). From the analysis of nadir spectra we have derived a mixing ratio of (0.14 0.05) ppb at an altitude of 97 kilometers, which corresponds to an integrated (from 0 to 600 kilometers) surface normalized column abundance of (3.7 plus or minus 1.3) x 10(exp 14) molecules per square centimeter. In the latitude range 80 S to 30 N we see no evidence for latitudinal variations in these abundances within the error bars. Using limb observations, we obtained mixing ratios of (0.13 plus or minus 0.04) ppb at an altitude of 115 kilometers and (0.45 plus or minus 0.15) ppb at an altitude of 230 kilometers, confirming that the water abundance has a positive vertical gradient as predicted by photochemical models (e.g. Lara et al. 1996, Wilson and Atreya 2004, Horst et al. 2008); retrieved scaling factors (from approximately 0.1 to approximately 0.6) to the water profile suggested by these models show that water vapor is present in Titan stratosphere with less abundance than predicted.

Cottini, V.↗

Propagation of Radiosonde Pressure Sensor Errors to Ozonesonde Measurements

Several previous studies highlight pressure (or equivalently, pressure altitude) discrepancies between the radiosonde pressure sensor and that derived from a GPS flown with the radiosonde. The offsets vary during the ascent both in absolute and percent pressure differences. To investigate this problem further, a total of 731 radiosonde-ozonesonde launches from the Southern Hemisphere subtropics to Northern mid-latitudes are considered, with launches between 2005 - 2013 from both longer-term and campaign-based intensive stations. Five series of radiosondes from two manufacturers (International Met Systems: iMet, iMet-P, iMet-S, and Vaisala: RS80-15N and RS92-SGP) are analyzed to determine the magnitude of the pressure offset. Additionally, electrochemical concentration cell (ECC) ozonesondes from three manufacturers (Science Pump Corporation; SPC and ENSCI-Droplet Measurement Technologies; DMT) are analyzed to quantify the effects these offsets have on the calculation of ECC ozone (O3) mixing ratio profiles (O3MR) from the ozonesonde-measured partial pressure. Approximately half of all offsets are 0.6 hPa in the free troposphere, with nearly a third 1.0 hPa at 26 km, where the 1.0 hPa error represents 5 persent of the total atmospheric pressure. Pressure offsets have negligible effects on O3MR below 20 km (96 percent of launches lie within 5 percent O3MR error at 20 km). Ozone mixing ratio errors above 10 hPa (30 km), can approach greater than 10 percent ( 25 percent of launches that reach 30 km exceed this threshold). These errors cause disagreement between the integrated ozonesonde-only column O3 from the GPS and radiosonde pressure profile by an average of +6.5 DU. Comparisons of total column O3 between the GPS and radiosonde pressure profiles yield average differences of +1.1 DU when the O3 is integrated to burst with addition of the McPeters and Labow (2012) above-burst O3 column climatology. Total column differences are reduced to an average of -0.5 DU when the O3 profile is integrated to 10 hPa with subsequent addition of the O3 climatology above 10 hPa. The RS92 radiosondes are superior in performance compared to other radiosondes, with average 26 km errors of -0.12 hPa or +0.61 percent O3MR error. iMet-P radiosondes had average 26 km errors of -1.95 hPa or +8.75 percent O3MR error. Based on our analysis, we suggest that ozonesondes always be coupled with a GPS-enabled radiosonde and that pressure-dependent variables, such as O3MR, be recalculated-reprocessed using the GPS-measured altitude, especially when 26 km pressure offsets exceed 1.0 hPa 5 percent.

pressure measurements↗

Water Vapor Measurements by Howard University Raman Lidar during the WAVES 2006 Campaign

Retrieval of water vapor mixing ratio using the Howard University Raman Lidar is presented with emphasis on three aspects: i) performance of the lidar against collocated radiosondes and Raman lidar, ii) investigation of the atmospheric state variables when poor agreement between lidar and radiosondes values occurred and iii) a comparison with satellite-based measurements. The measurements were acquired during the Water Vapor Validation Experiment Sondes/Satellites 2006 field campaign. Ensemble averaging of water vapor mixing ratio data from ten night-time comparisons with Vaisala RS92 radiosondes shows on average an agreement within 10 % up to approx. 8 km. A similar analysis of lidar-to-lidar data of over 700 profiles revealed an agreement to within 20 % over the first 7 km (10 % below 4 km). A grid analysis, defined in the temperature - relative humidity space, was developed to characterize the lidar - radiosonde agreement and quantitatively localizes regions of strong and weak correlations as a function of altitude, temperature or relative humidity. Three main regions of weak correlation emerge: i) regions of low relative humidity and low temperature, ii) moderate relative humidity at low temperatures and iii) low relative humidity at moderate temperatures. Comparison of Atmospheric InfraRed Sounder and Tropospheric Emission Sounder satellites retrievals of moisture with that of Howard University Raman Lidar showed a general agreement in the trend but the formers miss a lot of the details in atmospheric structure due to their low resolution. A relative difference of about 20 % is usually found between lidar and satellites measurements.

Adam, M.↗

Measurements of nitric oxide in the boundary layer and free troposphere over the Pacific Ocean

Measurements of NO and O3 are presented from 13 aircraft flights made over the Pacific Ocean in the autumn of 1983 during one phase of the NASA Global Tropospheric Experiment. All of the flights were made between 15 deg and 42 deg N and from the coast of California to west of the Hawaiian Islands. Within the upper marine boundary layer the median daytime mixing ratio of NO was near 1 part per trillion by volume (pptv). Values of NO less than 10 pptv were often observed up to altitudes near 6 km. Thus for the location and season of the measurements, a net photochemical destruction of O3 would be anticipated for the boundary layer region and to altitudes of 2-3 km. At higher altitudes of 7-11 km in the free troposphere, larger mixing ratios and greater variability were usually observed for NO. Both features are consistent with observed examples of injection of NO and O3 from the lower stratosphere and with the injection of NO from towering, electrically active, cumulonimbus clouds.

Ridley, B. A.↗

Infrared spectroscopic measurements of the total column abundance of ethan (C2H6) above Lauder, New Zealand

Total vertical column aboundances of atmospheric ethane (C2H6) have been retrieved form more than 350 high-resolution infrared solar spectra recorded on 129 days between December 1992 and March 1994 at the Network for the Detection of Stratospheric Change (NDSC) station in Lauder, New Zealand (latitude 45.04 deg S, 169.68 deg E, 0.37 km altitude). The results are based on nonlinear least squares fits to narrow spectral intervals containing the unresolved C2H6 nu (sub 7) band (P)Q(sub 3) and (R)Q(sub 0) subbranches at 2976.8 and 2986.7/cm. The measured Lauder column abundances show a pronounced seasonal cycle with a maximum value of (8.6 +/- 0.5) x 10(exp 15) molecules/sq cm in September and a minimum value of (3.8 +/- 0.5) x 10 (exp 15) molecules/sq cm in February. Assuming a realistic vertical distribution for C2H6, these values correspond to surface level volume-mixing ratios of 0.52 and 0.23 ppbv (parts per billion by volume), respectively. The phase and relative amplitude of the Lauder C2H6 seasonal cycle are similar to corresponding values determined from infrared measurements at the Jungfraujoch (46.55 deg N, 7.98 deg E, 3.58 km altitude) and Mauna Loa (latitude 19.5 deg N, longitude 155.6 deg W, 3.5 km altitude) NDSC stations, but the inferred absolute magnitudes of the Lauder surface level mixing ratios during the same season are significantly lower. The Lauder C2H6 measurements are also compared with published southern hemisphere surface level sampling measurements and two-dimensional model calculations.

Rinsland, Curtis P.↗