Items

Advanced search

Simultaneous Retrievals of Polar Mesospheric Clouds (PMCs) with Ozone from OMI UV measurements

The presence of polar mesospheric clouds (PMCs) at high latitudes could affect the retrieval of ozone profiles using backscattered ultraviolet (BUV) measurements. PMC-induced errors in ozone profile retrievals from Ozone Monitoring Instrument (OMI) BUV measurements are investigated through comparisons with Microwave Limb Sounder (MLS) ozone measurements. This comparison demonstrates that the presence of PMCs leads to systematic biases at altitudes above 6 hPa in summer high latitudes; the biases increase from ~ −2 % at 2 hPa to ~ −20 % at 0.5 hPa on average, and are significantly correlated with brightness of PMCs. Sensitivity studies show that the radiance sensitivity to PMCs strongly depends on wavelengths, increasing by a factor of ~ 4 from 300 to 265 nm. It also strongly depends on the PMC scattering, thus depending on viewing geometry. The optimal estimation-based retrieval sensitivity analysis shows that PMCs located at 80–85 km have the greatest effect on ozone retrievals at ~ 0.2 hPa (~ 60 km), where the retrieval errors range from −2.5 % with PMC optical depth (POD) of 10−4 to −20 % with 10−3 at back scattering angles, and the impacts increase by a factor of ~ 5 at forward scattering angles due to stronger PMC sensitivities. To reduce the interference of PMCs on ozone retrievals, we perform simultaneous retrievals of POD and ozone with a loose constraint of 10−3 for POD, which results in retrieval errors of 1–4 × 10−4. It is demonstrated that the negative bias of OMI ozone retrievals relative to MLS could be improved by including the PMC in the forward model calculation and retrieval.
Global OZone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS): methodology and sample results with a focus on HCl, H2O, and O3

We describe the publicly available data from the Global OZone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS) project and provide some results, with a focus on hydrogen chloride (HCl), water vapor (H2O), and ozone (O3). This data set is a global long-term stratospheric Earth system data record, consisting of monthly zonal mean time series starting as early as 1979. The data records are based on high-quality measurements from several NASA satellite instruments and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT. We examine consistency aspects between the various data sets. To merge ozone records, the time series are debiased relative to SAGE II (Stratospheric Aerosol and Gas Experiments) values by calculating average offsets versus SAGE II during measurement overlap periods, whereas for other species the merging derives from an averaging procedure during overlap periods. The GOZCARDS files contain mixing ratios on a common pressure–latitude grid, as well as standard errors and other diagnostics; we also present estimates of systematic uncertainties in the merged products. Monthly mean temperatures for GOZCARDS were also produced, based directly on data from the Modern-Era Retrospective analysis for Research and Applications. The GOZCARDS HCl merged product comes from the Halogen Occultation Experiment (HALOE), ACE-FTS and lower-stratospheric Aura Microwave Limb Sounder (MLS) data. After a rapid rise in upper-stratospheric HCl in the early 1990s, the rate of decrease in this region for 1997–2010 was between 0.4 and 0.7 % yr−1. On 6–8-year timescales, the rate of decrease peaked in 2004–2005 at about 1 % yr−1, and it has since levelled off, at ~ 0.5 % yr−1. With a delay of 6–7 years, these changes roughly follow total surface chlorine, whose behavior versus time arises from inhomogeneous changes in the source gases. Since the late 1990s, HCl decreases in the lower stratosphere have occurred with pronounced latitudinal variability at rates sometimes exceeding 1–2 % yr−1. Recent short-term tendencies of lower-stratospheric and column HCl vary substantially, with increases from 2005 to 2010 for northern midlatitudes and deep tropics, but decreases (increases) after 2011 at northern (southern) midlatitudes. For H2O, the GOZCARDS product covers both stratosphere and mesosphere, and the same instruments as for HCl are used, along with Upper Atmosphere Research Satellite (UARS) MLS stratospheric H2O data (1991–1993). We display seasonal to decadal-type variability in H2O from 22 years of data. In the upper mesosphere, the anticorrelation between H2O and solar flux is now clearly visible over two full solar cycles. Lower-stratospheric tropical H2O has exhibited two periods of increasing values, followed by fairly sharp drops (the well-documented 2000–2001 decrease and a recent drop in 2011–2013). Tropical decadal variability peaks just above the tropopause. Between 1991 and 2013, both in the tropics and on a near-global basis, H2O has decreased by ~ 5–10 % in the lower stratosphere, but about a 10 % increase is observed in the upper stratosphere and lower mesosphere. However, such tendencies may not represent longer-term trends. For ozone, we used SAGE I, SAGE II, HALOE, UARS and Aura MLS, and ACE-FTS data to produce a merged record from late 1979 onward, using SAGE II as the primary reference. Unlike the 2 to 3 % increase in near-global column ozone after the late 1990s reported by some, GOZCARDS stratospheric column O3 values do not show a recent upturn of more than 0.5 to 1 %; long-term interannual column ozone variations from GOZCARDS are generally in very good agreement with interannual changes in merged total column ozone (Version 8.6) data from SBUV instruments. A brief mention is also made of other currently available, commonly formatted GOZCARDS satellite data records for stratospheric composition, namely those for N2O and HNO3.
Ice phase in altocumulus clouds over Leipzig: remote sensing observations and detailed modeling

The present work combines remote sensing observations and detailed cloud modeling to investigate two altocumulus cloud cases observed over Leipzig, Germany. A suite of remote sensing instruments was able to detect primary ice at rather high temperatures of −6 °C. For comparison, a second mixed phase case at about −25 °C is introduced. To further look into the details of cloud microphysical processes, a simple dynamics model of the Asai-Kasahara (AK) type is combined with detailed spectral microphysics (SPECS) forming the model system AK-SPECS. Vertical velocities are prescribed to force the dynamics, as well as main cloud features, to be close to the observations. Subsequently, sensitivity studies with respect to ice microphysical parameters are carried out with the aim to quantify the most important sensitivities for the cases investigated. For the cases selected, the liquid phase is mainly determined by the model dynamics (location and strength of vertical velocity), whereas the ice phase is much more sensitive to the microphysical parameters (ice nucleating particle (INP) number, ice particle shape). The choice of ice particle shape may induce large uncertainties that are on the same order as those for the temperature-dependent INP number distribution.
Strong aerosol–cloud interaction in altocumulus during updraft periods: lidar observations over central Europe

For the first time, a liquid-water cloud study of the aerosol–cloud-dynamics relationship, solely based on lidar, was conducted. Twenty-nine cases of pure liquid-water altocumulus layers were observed with a novel dual-field-of-view Raman lidar over the polluted central European site of Leipzig, Germany, between September 2010 and September 2012. By means of the novel Raman lidar technique, cloud properties such as the droplet effective radius and cloud droplet number concentration (CDNC) in the lower part of altocumulus layers are obtained. The conventional aerosol Raman lidar technique provides the aerosol extinction coefficient (used as aerosol proxy) below cloud base. A collocated Doppler lidar measures the vertical velocity at cloud base and thus updraft and downdraft occurrence. Here, we present the key results of our statistical analysis of the 2010–2012 observations. Besides a clear aerosol effect on cloud droplet number concentration in the lower part of the altocumulus layers during updraft periods, turbulent mixing and entrainment of dry air is assumed to be the main reason for the found weak correlation between aerosol proxy and CDNC higher up in the cloud. The corresponding aerosol–cloud interaction parameter based on changes in cloud droplet number concentration with aerosol loading was found to be close to 0.8 at 30–70 m above cloud base during updraft periods and below 0.4 when ignoring vertical-wind information in the analysis. Our findings are extensively compared with literature values and agree well with airborne observations.
Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3− aerosol during the 2013 Southern Oxidant and Aerosol Study

Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3−) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. Calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3− is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3− and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.
The impact of observing characteristics on the ability to predict ozone under varying polluted photochemical regimes

We conduct analyses to assess how characteristics of observations of ozone and its precursors affect air quality forecasting and research. To carry out this investigation, we use a photochemical box model and its adjoint integrated with a Lagrangian 4D-variational data assimilation system. Using this framework in conjunction with pseudo-observations, we perform an ozone precursor source inversion and estimate surface emissions. We then assess the resulting improvement in ozone air quality prediction. We use an analytical model to conduct uncertainty analyses. Using this analytical tool, we address some key questions regarding how the characteristics of observations affect ozone precursor emission inversion and in turn ozone prediction. These questions include what the effect is of choosing which species to observe, of varying amounts of observation noise, of changing the observing frequency and the observation time during the diurnal cycle, and of how these different scenarios interact with different photochemical regimes. In our investigation we use three observed species scenarios: CO and NO2; ozone, CO, and NO2; and HCHO, CO and NO2. The photochemical model was set up to simulate a range of summertime polluted environments spanning NOx-(NO and NO2)-limited to volatile organic compound (VOC)-limited conditions. We find that as the photochemical regime changes, here is a variation in the relative importance of trace gas observations to be able to constrain emission estimates and to improve the subsequent ozone forecasts. For example, adding ozone observations to an NO2 and CO observing system is found to decrease ozone prediction error under NOx- and VOC-limited regimes, and complementing the NO2 and CO system with HCHO observations would improve ozone prediction in the transitional regime and under VOC-limited conditions. We found that scenarios observing ozone and HCHO with a relative observing noise of lower than 33 % were able to achieve ozone prediction errors of lower than 5 ppbv (parts per billion by volume). Further, only observing intervals of 3 h or shorter were able to consistently achieve ozone prediction errors of 5 ppbv or lower across all photochemical regimes. Making observations closer to the prediction period and either in the morning or afternoon rush hour periods made greater improvements for ozone prediction: 0.2–0.3 ppbv for the morning rush hour and from 0.3 to 0.8 ppbv for the afternoon compared to only 0–0.1 ppbv for other times of the day. Finally, we made two complementary analyses that show that our conclusions are insensitive to the assumed diurnal emission cycle and to the choice of which VOC species emission to estimate using our framework. These questions will address how different types of observing platform, e.g. geostationary satellites or ground monitoring networks, could support future air quality research and forecasting.
NO2 seasonal evolution in the north subtropical free troposphere

Three years of multi-axis differential optical absorption spectroscopy (MAXDOAS) measurements (2011–2013) have been used for estimating the NO2 mixing ratio along a horizontal line of sight from the high mountain subtropical observatory of Izaña, at 2370 m a.s.l. (NDACC station, 28.3° N, 16.5° W). The method is based on horizontal path calculation from the O2–O2 collisional complex at the 477 nm absorption band which is measured simultaneously to the NO2 column density, and is applicable under low aerosol-loading conditions. The MAXDOAS technique, applied in horizontal mode in the free troposphere, minimizes the impact of the NO2 contamination resulting from the arrival of marine boundary layer (MBL) air masses from thermally forced upwelling breeze during middle hours of the day. Comparisons with in situ observations show that during most of the measuring period, the MAXDOAS is insensitive or very slightly sensitive to the upwelling breeze. Exceptions are found for pollution events during southern wind conditions. On these occasions, evidence of fast, efficient and irreversible transport from the surface to the free troposphere is found. Background NO2 volume mixing ratio (vmr), representative of the remote free troposphere, is in the range of 20–45 pptv. The observed seasonal evolution shows an annual wave where the peak is in phase with the solar radiation. Model simulations with the chemistry–climate CAM-Chem model are in good agreement with the NO2 measurements, and are used to further investigate the possible drivers of the NO2 seasonality observed at Izaña.
Use of North American and European air quality networks to evaluate global chemistry–climate modeling of surface ozone

We test the current generation of global chemistry–climate models in their ability to simulate observed, present-day surface ozone. Models are evaluated against hourly surface ozone from 4217 stations in North America and Europe that are averaged over 1° × 1° grid cells, allowing commensurate model–measurement comparison. Models are generally biased high during all hours of the day and in all regions. Most models simulate the shape of regional summertime diurnal and annual cycles well, correctly matching the timing of hourly (~ 15:00 local time (LT)) and monthly (mid-June) peak surface ozone abundance. The amplitude of these cycles is less successfully matched. The observed summertime diurnal range (~ 25 ppb) is underestimated in all regions by about 7 ppb, and the observed seasonal range (~ 21 ppb) is underestimated by about 5 ppb except in the most polluted regions, where it is overestimated by about 5 ppb. The models generally match the pattern of the observed summertime ozone enhancement, but they overestimate its magnitude in most regions. Most models capture the observed distribution of extreme episode sizes, correctly showing that about 80 % of individual extreme events occur in large-scale, multi-day episodes of more than 100 grid cells. The models also match the observed linear relationship between episode size and a measure of episode intensity, which shows increases in ozone abundance by up to 6 ppb for larger-sized episodes. We conclude that the skill of the models evaluated here provides confidence in their projections of future surface ozone.
Thermodynamics of the formation of sulfuric acid dimers in the binary (H2SO4–H2O) and ternary (H2SO4–H2O–NH3) system

Sulfuric acid is an important gas influencing atmospheric new particle formation (NPF). Both the binary (H2SO4–H2O) system and the ternary system involving ammonia (H2SO4–H2O–NH3) may be important in the free troposphere. An essential step in the nucleation of aerosol particles from gas-phase precursors is the formation of a dimer, so an understanding of the thermodynamics of dimer formation over a wide range of atmospheric conditions is essential to describe NPF. We have used the CLOUD chamber to conduct nucleation experiments for these systems at temperatures from 208 to 248 K. Neutral monomer and dimer concentrations of sulfuric acid were measured using a chemical ionization mass spectrometer (CIMS). From these measurements, dimer evaporation rates in the binary system were derived for temperatures of 208 and 223 K. We compare these results to literature data from a previous study that was conducted at higher temperatures but is in good agreement with the present study. For the ternary system the formation of H2SO4·NH3 is very likely an essential step in the formation of sulfuric acid dimers, which were measured at 210, 223, and 248 K. We estimate the thermodynamic properties (dH and dS) of the H2SO4·NH3 cluster using a simple heuristic model and the measured data. Furthermore, we report the first measurements of large neutral sulfuric acid clusters containing as many as 10 sulfuric acid molecules for the binary system using chemical ionization–atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometry.
The role of ice nuclei recycling in the maintenance of cloud ice in Arctic mixed-phase stratocumulus

This study investigates the maintenance of cloud ice production in Arctic mixed-phase stratocumulus in large eddy simulations that include a prognostic ice nuclei (IN) formulation and a diurnal cycle. Balances derived from a mixed-layer model and phase analyses are used to provide insight into buffering mechanisms that maintain ice in these cloud systems. We find that, for the case under investigation, IN recycling through subcloud sublimation considerably prolongs ice production over a multi-day integration. This effective source of IN to the cloud dominates over mixing sources from above or below the cloud-driven mixed layer. Competing feedbacks between dynamical mixing and recycling are found to slow the rate of ice lost from the mixed layer when a diurnal cycle is simulated. The results of this study have important implications for maintaining phase partitioning of cloud ice and liquid that determine the radiative forcing of Arctic mixed-phase clouds.