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Variability of NOx in the polar middle atmosphere from October 2003 to March 2004: vertical transport vs. local production by energetic particles

We use NO, NO2 and CO from MIPAS/ENVISAT to investigate the impact of energetic particle precipitation onto the NOx budget from the stratosphere to the lower mesosphere in the period from October 2003 to March 2004, a time of high solar and geomagnetic activity. We find that in the winter hemisphere the indirect effect of auroral electron precipitation due to downwelling of upper mesospheric/lower thermospheric air into the stratosphere prevails. Its effect exceeds even the direct impact of the very large solar proton event in October/November 2003 by nearly 1 order of magnitude. Correlations of NOx and CO show that the unprecedented high NOx values observed in the Northern Hemisphere lower mesosphere and upper stratosphere in late January and early February are fully consistent with transport from the upper mesosphere/lower thermosphere and subsequent mixing at lower altitudes. In the polar summer Southern Hemisphere, we observed an enhanced variability of NO and NO2 on days with enhanced geomagnetic activity, but this seems to indicate enhanced instrument noise rather than a direct increase due to electron precipitation. A direct effect of electron precipitation onto NOx can not be ruled out, but, if any, it is lower than 3 ppbv in the altitude range 40–56 km and lower than 6 ppbv in the altitude range 56–64 km. An additional significant source of NOx due to local production by precipitating electrons below 70 km exceeding several parts per billion as discussed in previous publications appears unlikely.
Evidence for an earlier greenhouse cooling effect in the stratosphere before 1980 over the Northern Hemisphere

This study provides a new look at the observed and calculated long-term temperature changes from the lower troposphere to the lower stratosphere since 1958 over the Northern Hemisphere. The data sets include the NCEP/NCAR reanalysis, the Free University of Berlin (FU-Berlin) and the RICH radiosonde data sets as well as historical simulations with the CESM1-WACCM global model participating in CMIP5. The analysis is mainly based on monthly layer mean temperatures derived from geopotential height thicknesses in order to take advantage of the use of the independent FU-Berlin stratospheric data set of geopotential height data since 1957. This approach was followed to extend the records for the investigation of the stratospheric temperature trends to the earliest possible time. After removing the natural variability with an autoregressive multiple regression model our analysis shows that the period 1958–2011 can be divided into two distinct sub-periods of long-term temperature variability and trends: before and after 1980. By calculating trends for the summer time to reduce interannual variability, the two periods are as follows. From 1958 until 1979, a non-significant trend (0.06 ± 0.06 °C decade−1 for NCEP) and slightly cooling trends (−0.12 ± 0.06 °C decade−1 for RICH) are found in the lower troposphere. The second period from 1980 to the end of the records shows significant warming (0.25 ± 0.05 °C decade−1 for both NCEP and RICH). Above the tropopause a significant cooling trend is clearly seen in the lower stratosphere both in the pre-1980 period (−0.58 ± 0.17 °C decade−1 for NCEP, −0.30 ± 0.16 °C decade−1 for RICH and −0.48 ± 0.20 °C decade−1 for FU-Berlin) and the post-1980 period (−0.79 ± 0.18 °C decade−1 for NCEP, −0.66 ± 0.16 °C decade−1 for RICH and −0.82 ± 0.19 °C decade−1 for FU-Berlin). The cooling in the lower stratosphere persists throughout the year from the tropics up to 60° N. At polar latitudes competing dynamical and radiative processes reduce the statistical significance of these trends. Model results are in line with reanalysis and the observations, indicating a persistent cooling (−0.33 °C decade−1) in the lower stratosphere during summer before and after 1980; a feature that is also seen throughout the year. However, the lower stratosphere CESM1-WACCM modelled trends are generally lower than reanalysis and the observations. The contrasting effects of ozone depletion at polar latitudes in winter/spring and the anticipated strengthening of the Brewer–Dobson circulation from man-made global warming at polar latitudes are discussed. Our results provide additional evidence for an early greenhouse cooling signal in the lower stratosphere before 1980, which appears well in advance relative to the tropospheric greenhouse warming signal. The suitability of early warning signals in the stratosphere relative to the troposphere is supported by the fact that the stratosphere is less sensitive to changes due to cloudiness, humidity and man-made aerosols. Our analysis also indicates that the relative contribution of the lower stratosphere versus the upper troposphere low-frequency variability is important for understanding the added value of the long-term tropopause variability related to human-induced global warming.
Improved model of isoprene emissions in Africa using Ozone Monitoring Instrument (OMI) satellite observations of formaldehyde: implications for oxidants and particulate matter

We use a 2005–2009 record of isoprene emissions over Africa derived from Ozone Monitoring Instrument (OMI) satellite observations of formaldehyde (HCHO) to better understand the factors controlling isoprene emission in the continent and evaluate the impact on atmospheric composition. OMI-derived isoprene emissions show large seasonality over savannas driven by temperature and leaf area index (LAI), and much weaker seasonality over equatorial forests driven by temperature. The commonly used MEGAN (Model of Emissions of Gases and Aerosols from Nature, version 2.1) global isoprene emission model reproduces this seasonality but is biased high, particularly for equatorial forests, when compared to OMI and relaxed-eddy accumulation measurements. Isoprene emissions in MEGAN are computed as the product of an emission factor Eo, LAI, and activity factors dependent on environmental variables. We use the OMI-derived emissions to provide improved estimates of Eo that are in good agreement with direct leaf measurements from field campaigns (r = 0.55, bias = −19%). The largest downward corrections to MEGAN Eo values are for equatorial forests and semi-arid environments, and this is consistent with latitudinal transects of isoprene over western Africa from the African Monsoon Multidisciplinary Analysis (AMMA) aircraft campaign. Total emission of isoprene in Africa is estimated to be 77 Tg C a−1, compared to 104 Tg C a−1 in MEGAN. Simulations with the GEOS-Chem oxidant–aerosol model suggest that isoprene emissions increase mean surface ozone in western Africa by up to 8 ppbv, and particulate matter by up to 1.5 μg m−3, due to coupling with anthropogenic influences.
Climatic controls on water vapor deuterium excess in the marine boundary layer of the North Atlantic based on 500 days of in situ, continuous measurements

Continuous, in situ measurements of water vapor isotopic composition have been conducted in the North Atlantic, at the Bermuda Islands (32.26° N, 64.88° W), between November 2011 and June 2013, using a cavity ring-down spectrometer water vapor isotope analyzer and an autonomous self-designed calibration system. Meticulous calibration allows us to reach an accuracy and precision on 10 min average of δ18O, δ D, and d-excess of, 0.14, 0.85, and 1.1&permil;, verified using two parallel instruments with independent calibration. As a result of more than 500 days with 6-hourly data the relationships between deuterium excess, relative humidity (RH), sea surface temperature (SST), wind speed, and wind direction are assessed. From the whole data set, 84 % of d-excess variance is explained by a strong linear relationship with relative humidity. The slope of this relationship (−42.6 ± 0.4&permil; % (RH)) is similar to the theoretical prediction of Merlivat and Jouzel (1979) for SST between 20 and 30 °C. However, in contrast with theory, no effect of wind speed could be detected on the relationship between d-excess and relative humidity. Separating the data set into winter, spring, summer, and autumn seasons reveals different linear relationships between d-excess and humidity. Changes in wind directions are observed to affect the relationships between d-excess and humidity. The observed seasonal variability in the relationship between d-excess and relative humidity underlines the importance of long-term monitoring to make accurate conclusions.
SO2 noontime-peak phenomenon in the North China Plain

A phenomenon of frequent noontime SO2 concentration peaks was discovered in a detailed analysis of the SO2 concentrations in the North China Plain (NCP). The possible causes and their contributions are analyzed. The impacts of such a phenomenon on the sulphur cycle were studied and the implications of the phenomenon for atmospheric chemistry, cloud physics, and climate were discussed. Different from the more common SO2 diurnal patterns with high nighttime concentrations, NCP witnessed high frequencies of noontime SO2 peaks, with an occurrence frequency of 50 to 72% at four stations. Down mixing of elevated pollution layers, plume transport processes, mountain-valley winds, and fog/high RH haze events were the possible causes. The contribution of each process varies from day to day and from station to station, however, none of those four processes can be neglected. SO2 peaks occurring during noontime instead of nighttime will lead to a 13 to 35% increase in sulphur dry deposition, a 9 to 23% increase in gas phase oxidation, and an 8 to 33% increase in aqueous phase conversions, which will increase the hygroscopicity and the light scattering of aerosols, thus having important impacts on atmospheric chemistry, cloud physics, and climate.
Skill in forecasting extreme ozone pollution episodes with a global atmospheric chemistry model

From the ensemble of stations that monitor surface air quality over the United States and Europe, we identify extreme ozone pollution events and find that they occur predominantly in clustered, multiday episodes with spatial extents of more than 1000 km. Such scales are amenable to forecasting with current global atmospheric chemistry models. We develop an objective mapping algorithm that uses the heterogeneous observations of the individual surface sites to calculate surface ozone averaged over 1° by 1° grid cells, matching the resolution of a global model. Air quality extreme (AQX) events are identified locally as statistical extremes of the ozone climatology and not as air quality exceedances. With the University of California, Irvine chemistry-transport model (UCI CTM) we find there is skill in hindcasting these extreme episodes, and thus identify a new diagnostic using global chemistry–climate models (CCMs) to identify changes in the characteristics of extreme pollution episodes in a warming climate.
A high ozone episode in winter 2013 in the Uinta Basin oil and gas region characterized by aircraft measurements

During the winter of 2012–2013 atmospheric surface ozone mole fractions exceeded the US 8 h standard of 75 ppb on 39 days in the Uinta Basin of Utah. As part of the Uinta Basin Winter Ozone Study (UBWOS) aircraft flights were conducted throughout the basin with continuous measurements of ozone (O3), methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), nitrogen dioxide (NO2), and discrete whole air flask samples for determination of &sim;50 trace gases including a number of non-methane hydrocarbons (NMHCs). During the course of seven flights conducted between 31 January and 7 February 2013, coinciding with strong, multi-day temperature inversions, O3 levels gradually built up in the shallow boundary layer from &sim;45 ppb to &sim;140 ppb. Near-surface CH4 mole fractions increased during the episode from near background levels of &sim;2 ppm to over 10 ppm. Based on elevated levels of CH4 across the basin and high correlations of CH4 with NMHCs from the discrete air samples, O3 precursor NMHCs were also inferred to be elevated throughout the basin. Discrete plumes of high NO2 were observed in the gas production region of the basin suggesting that gas processing plants and compressor facilities were important point sources of reactive nitrogen oxides (NOx). Vertical profiles obtained during the flights showed that the high O3 mole fractions (as well as other elevated constituents) were confined to a shallow layer from near the ground to 300–400 m above ground level (m a.g.l.) capped by a strong temperature inversion. The highest mole fractions of the measured constituents during the study period were in an isothermal cold layer that varied from &sim;300 m depth on 4 February to &sim;150 m on 5 February. A gradient layer with declining mole fractions with altitude extended above the isothermal layer to &sim;1900 m a.s.l. (300–400 m a.g.l.) indicative of some mixing of air out of the boundary layer. O3 mole fractions continued to increase within the basin as the high O3 episode developed over the course of a week. CH4 mole fractions, on the other hand, leveled off after several days. On several flights, the aircraft sampled the plume of a coal-fired power plant (located east of the main gas field) flowing above the inversion layer. These measurements ruled out the effluents of the power plant as a significant source of NOx for O3 production beneath the temperature inversion in the basin. The presence of elevated O3 precursors within the basin and the rapid daytime production of O3 in the atmosphere beneath the temperature inversion both indicated that O3 was being produced from precursors emitted within the basin beneath the temperature inversion. Although observations show that horizontal winds in the surface layer were relatively light during the high ozone event, they were sufficient to disperse precursors up to 80 km from primary sources in the main gas field in the southeast quadrant to the balance of the Uinta Basin.
Transport pathways of peroxyacetyl nitrate in the upper troposphere and lower stratosphere from different monsoon systems during the summer monsoon season

The Asian summer monsoon involves complex transport patterns with large scale redistribution of trace gases in the upper troposphere and lower stratosphere (UTLS). We employ the global chemistry–climate model ECHAM5-HAMMOZ in order to evaluate the transport pathways and the contributions of nitrogen oxide reservoir species PAN, NOx, and HNO3 from various monsoon regions, to the UTLS over Southern Asia and vice versa. The model is evaluated with trace gas retrievals from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-E) and aircraft campaigns during the monsoon season (June–September). There are three regions which contribute substantial pollution to the UTLS during the monsoon: the Asian summer monsoon (ASM), the North American Monsoon (NAM) and the West African monsoon (WAM). However, penetration due to ASM convection is deeper into the UTLS as compared to NAM and WAM outflow. The circulation in these monsoon regions distributes PAN into the tropical latitude belt in the upper troposphere. Remote transport also occurs in the extratropical upper troposphere where westerly winds drive North American and European pollutants eastward to partly merge with the ASM plume. Strong ASM convection transports these remote and regional pollutants into the lower stratosphere. In the lower stratosphere the injected pollutants are transported westward by easterly winds. The intense convective activity in the monsoon regions is associated with lightning generation and thereby the emission of NOy species. This will affect the distribution of PAN in the UTLS. The estimates of lightning produced PAN, HNO3, NOx and ozone obtained from control and lightning-off simulations shows high percentage changes over the regions of convective transport especially equatorial Africa and America and comparatively less over the ASM. This indicates higher anthropogenic pollution transport from the ASM region into the UTLS.
Absorption and scattering properties of organic carbon versus sulfate dominant aerosols at Gosan climate observatory in Northeast Asia

Carbonaceous and soluble ionic species of PM1.0 and PM10 were measured along with the absorption and scattering properties and aerosol number size distributions at Gosan Climate Observatory (GCO) from January to September 2008. The daily averaged equivalent black carbon (EBC) measured as aerosol absorption exhibited two types of spectral dependence with a distinct maximum (peak) at either 370 nm or 880 nm, by which two subsets were extracted and classified into the respective groups (370 and 880 nm). The 370 nm group was distinguished by high organic carbon (OC) concentrations relative to elemental carbon (EC) and sulfate, but sulfate was predominant for the 880 nm group. The PM1.0 OC of the 370 nm group was mainly composed of refractory and pyrolized components that correlated well with PM1.0 EC1, referred to as char EC, which suggests biofuel and biomass combustion as the source of these OC fractions, particularly during winter. The scanning electron microscope (SEM) images and the number size distributions implied that aerosols of the 370 nm group were externally mixed upon transport in fast-moving air masses that passed through the Beijing area in about one day. In contrast, the aerosols of the 880 nm group were characterized by high sulfate concentrations, and seemed to be internally mixed during slow transport over the Yellow Sea region over approximately 2 to 4 days. The absorption and scattering coefficients of the 880 nm group were noticeably higher compared to those of the 370 nm group. The average absorption ångström exponent (AAE) was estimated to be 1.29 and 1.0 for the 370 and 880 nm groups, respectively, in the range 370–950 nm. These results demonstrated that the optical properties of aerosols were intimately linked to chemical composition and mixing state, characteristics determined both by source and atmospheric aging processes. In OC dominant aerosols, absorption was enhanced in the UV region, which was possibly due to refractory and pyrolized OC compounds. Under sulfate dominant conditions, the sulfate coating on BC particles likely contributed to the absorption of the longer visible light. Consequently, single scattering albedo (SSA) was higher for the 880 nm group than for the 370 nm group, emphasizing that the relative abundances of absorbing and scattering constituents are also important in estimating the climate effect of aerosols.
Sensitivity of simulated climate to latitudinal distribution of solar insolation reduction in solar radiation management

Solar radiation management (SRM) geoengineering has been proposed as a potential option to counteract climate change. We perform a set of idealized geoengineering simulations using Community Atmosphere Model version 3.1 developed at the National Center for Atmospheric Research to investigate the global hydrological implications of varying the latitudinal distribution of solar insolation reduction in SRM methods. To reduce the solar insolation we have prescribed sulfate aerosols in the stratosphere. The radiative forcing in the geoengineering simulations is the net forcing from a doubling of CO2 and the prescribed stratospheric aerosols. We find that for a fixed total mass of sulfate aerosols (12.6 Mt of SO4), relative to a uniform distribution which nearly offsets changes in global mean temperature from a doubling of CO2, global mean radiative forcing is larger when aerosol concentration is maximum at the poles leading to a warmer global mean climate and consequently an intensified hydrological cycle. Opposite changes are simulated when aerosol concentration is maximized in the tropics. We obtain a range of 1 K in global mean temperature and 3% in precipitation changes by varying the distribution pattern in our simulations: this range is about 50% of the climate change from a doubling of CO2. Hence, our study demonstrates that a range of global mean climate states, determined by the global mean radiative forcing, are possible for a fixed total amount of aerosols but with differing latitudinal distribution. However, it is important to note that this is an idealized study and thus not all important realistic climate processes are modeled.