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Decadal-scale responses in middle and upper stratospheric ozone from SAGE II version 7 data

Stratospheric Aerosol and Gas Experiment (SAGE II) version 7 (v7) ozone profiles are analyzed for their decadal-scale responses in the middle and upper stratosphere for 1991 and 1992–2005 and compared with those from its previous version 6.2 (v6.2). Multiple linear regression (MLR) analysis is applied to time series of its ozone number density vs. altitude data for a range of latitudes and altitudes. The MLR models that are fit to the time series data include a periodic 11 yr term, and it is in-phase with that of the 11 yr, solar UV (Ultraviolet)-flux throughout most of the latitude/altitude domain of the middle and upper stratosphere. Several regions that have a response that is not quite in-phase are interpreted as being affected by decadal-scale, dynamical forcings. The maximum minus minimum, solar cycle (SC-like) responses for the ozone at the low latitudes are similar from the two SAGE II data versions and vary from about 5 to 2.5% from 35 to 50 km, although they are resolved better with v7. SAGE II v7 ozone is also analyzed for 1984–1998, in order to mitigate effects of end-point anomalies that bias its ozone in 1991 and the analyzed results for 1991–2005 or following the Pinatubo eruption. Its SC-like ozone response in the upper stratosphere is of the order of 4% for 1984–1998 vs. 2.5 to 3% for 1991–2005. The SAGE II v7 results are also recompared with the responses in ozone from the Halogen Occultation Experiment (HALOE) that are in terms of mixing ratio vs. pressure for 1991–2005 and then for late 1992–2005 to avoid any effects following Pinatubo. Shapes of their respective response profiles agree very well for 1992–2005. The associated linear trends of the ozone are not as negative in 1992–2005 as in 1984–1998, in accord with a leveling off of the effects of reactive chlorine on ozone. It is concluded that the SAGE II v7 ozone yields SC-like ozone responses and trends that are of better quality than those from v6.2.
Nitric acid trihydrate nucleation and denitrification in the Arctic stratosphere

Nitric acid trihydrate (NAT) particles in the polar stratosphere have been shown to be responsible for vertical redistribution of reactive nitrogen (NOy). Recent observations by Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the CALIPSO satellite have been explained in terms of heterogeneous nucleation of NAT on foreign nuclei, revealing this to be an important formation pathway for the NAT particles. In state of the art global- or regional-scale models, heterogeneous NAT nucleation is currently simulated in a very coarse manner using a constant, saturation-independent nucleation rate. Here we present first simulations for the Arctic winter 2009/2010 applying a new saturation-dependent parametrisation of heterogeneous NAT nucleation rates within the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulation shows good agreement of chemical trace species with in situ and remote sensing observations. The simulated polar stratospheric cloud (PSC) optical properties agree much better with CALIOP observations than those simulated with a constant nucleation rate model. A comparison of the simulated particle size distributions with observations made using the Forward Scattering Spectrometer Probe (FSSP) aboard the high altitude research aircraft Geophysica, shows that the model reproduces the observed size distribution, except for the very largest particles above 15 μm diameter. The vertical NOy redistribution caused by the sedimentation of the NAT particles, in particular the denitrification and nitrification signals observed by the ACE-FTS satellite instrument and the in situ SIOUX instrument aboard the Geophysica, are reproduced by the improved model, and a small improvement with respect to the constant nucleation rate model is found.
Analysis of the global atmospheric methane budget using ECHAM-MOZ simulations for present-day, pre-industrial time and the Last Glacial Maximum

Atmospheric methane concentrations increased considerably from pre-industrial (PI) to present times largely due to anthropogenic emissions. However, firn and ice core records also document a notable rise of methane levels between the Last Glacial Maximum (LGM) and the pre-industrial era, the exact cause of which is not entirely clear. This study investigates these changes by analyzing the methane sources and sinks at each of these climatic periods. Wetlands are the largest natural source of methane and play a key role in determining methane budget changes in particular in the absence of anthropogenic sources. Here, a simple wetland parameterization suitable for coarse-scale climate simulations over long periods is introduced, which is derived from a high-resolution map of surface slopes together with various soil hydrology parameters from the CARAIB vegetation model. This parameterization was implemented in the chemistry general circulation model ECHAM5-MOZ and multi-year time slices were run for LGM, PI and present-day (PD) climate conditions. Global wetland emissions from our parameterization are 72 Tg yr−1 (LGM), 115 Tg yr−1 (PI), and 132 Tg yr−1 (PD). These estimates are lower than most previous studies, and we find a stronger increase of methane emissions between LGM and PI. Taking into account recent findings that suggest more stable OH concentrations than assumed in previous studies, the observed methane distributions are nevertheless well reproduced under the different climates. Hence, this is one of the first studies where a consistent model approach has been successfully applied for simulating methane concentrations over a wide range of climate conditions.
Increased absorption by coarse aerosol particles over the Gangetic–Himalayan region

Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be < 1 μm in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October–November), suggesting the presence of absorbing aerosols sized 1–10 μm. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by larger particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Hence, large absorbing particles could be an important component of the regional-scale atmospheric energy balance.
Satellite observations of cloud regime development: the role of aerosol processes

Many different interactions between aerosols and clouds have been postulated, based on correlations between satellite retrieved aerosol and cloud properties. Previous studies highlighted the importance of meteorological covariations to the observed correlations. In this work, we make use of multiple temporally-spaced satellite retrievals to observe the development of cloud regimes. The observation of cloud regime development allows us to account for the influences of cloud fraction (CF) and meteorological factors on the aerosol retrieval. By accounting for the aerosol index (AI)-CF relationship, we reduce the influence of meteorological correlations compared to "snapshot" studies, finding that simple correlations overestimate any aerosol effect on CF by at least a factor of two. We find an increased occurrence of transitions into the stratocumulus regime over ocean with increases in MODIS AI, consistent with the hypothesis that aerosols increase stratocumulus persistence. We also observe an increase in transitions into the deep convective regime over land, consistent with the aerosol invigoration hypothesis. We find changes in the transitions from the shallow cumulus regime in different aerosol environments. The strength of these changes is strongly dependent on Low Troposphere Static Stability and 10 m windspeed, but less so on other meteorological factors. Whilst we have reduced the error due to meteorological and CF effects on the aerosol retrieval, meteorological covariation with the cloud and aerosol properties is harder to remove, so these results likely represent an upper bound on the effect of aerosols on cloud development and CF.
On the role of monoterpene chemistry in the remote continental boundary layer

The formation of organic nitrates (RONO2) represents an important NOx (NOx = NO + NO2) sink in the remote and rural continental atmosphere, thus impacting ozone production and secondary organic aerosol (SOA) formation. In these remote and rural environments, the organic nitrates are primarily derived from biogenic volatile organic compounds (BVOCs) such as isoprene and monoterpenes. Although there are numerous studies investigating the formation of SOA from monoterpenes, there are few studies investigating monoterpene gas-phase chemistry. Using a regional chemical transport model with an extended representation of organic nitrate chemistry, we investigate the processes controlling the production and fate of monoterpene nitrates (MTNs) over the boreal forest of Canada. MTNs account for 5–12% of total oxidized nitrogen over the boreal forest, and production via NO3 chemistry is more important than production via OH when the NOx mixing ratio is greater than 75 pptv. The regional responses are investigated for two oxidation pathways of MTNs: one that returns NOx to the atmosphere and one that converts MTNs into a nitrate that behaves like HNO3. The likely situation is in between, and these two assumptions bracket the uncertainty about this chemistry. In the case where the MTNs return NOx after oxidation, their formation represents a net chemical NOx loss that exceeds the net loss to peroxy nitrate formation. When oxidation of MTNs produces a molecule that behaves like HNO3, HNO3 and MTNs are nearly equal chemical sinks for NOx. This uncertainty in the oxidative fate of MTNs results in changes in NOx of 8–14%, in O3 of up to 3%, and in OH of 3–6% between the two model simulations.
Global and regional impacts of HONO on the chemical composition of clouds and aerosols

Recently, realistic simulation of nitrous acid (HONO) based on the HONO / NOx ratio of 0.02 was found to have a significant impact on the global budgets of HOx (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model-measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation.
A review of sea-spray aerosol source functions using a large global set of sea salt aerosol concentration measurements

Sea-spray aerosols (SSA) are an important part of the climate system because of their effects on the global radiative budget – both directly as scatterers and absorbers of solar and terrestrial radiation, and indirectly as cloud condensation nuclei (CCN) influencing cloud formation, lifetime, and precipitation. In terms of their global mass, SSA have the largest uncertainty of all aerosols. In this study we review 21 SSA source functions from the literature, several of which are used in current climate models. In addition, we propose a~new function. Even excluding outliers, the global annual SSA mass produced spans roughly 3–70 Pg yr−1 for the different source functions, for particles with dry diameter Dp < 10 μm, with relatively little interannual variability for a given function. The FLEXPART Lagrangian particle dispersion model was run in backward mode for a large global set of observed SSA concentrations, comprised of several station networks and ship cruise measurement campaigns. FLEXPART backward calculations produce gridded emission sensitivity fields, which can subsequently be multiplied with gridded SSA production fluxes in order to obtain modeled SSA concentrations. This allowed us to efficiently and simultaneously evaluate all 21 source functions against the measurements. Another advantage of this method is that source-region information on wind speed and sea surface temperatures (SSTs) could be stored and used for improving the SSA source function parameterizations. The best source functions reproduced as much as 70% of the observed SSA concentration variability at several stations, which is comparable with "state of the art" aerosol models. The main driver of SSA production is wind, and we found that the best fit to the observation data could be obtained when the SSA production is proportional to U103.5, where U10 is the source region averaged 10 m wind speed. A strong influence of SST on SSA production, with higher temperatures leading to higher production, could be detected as well, although the underlying physical mechanisms of the SST influence remains unclear. Our new source function with wind speed and temperature dependence gives a global SSA production for particles smaller than Dp < 10 μm of 9 Pg yr−1, and is the best fit to the observed concentrations.
Source, transport and impacts of a heavy dust event in the Yangtze River Delta, China, in 2011

Dust invasion is an important type of particle pollution in China. During 1 to 6 May in 2011, a dust event was observed in the Yangtze River Delta region (YRD). The highest PM10 (particles up to 10 μ in diameter) concentration reached over 1000 μg m−3 and the visibility was below 3 km. In this study, the Community Multi-scale Air Quality modeling system (CMAQ5.0) coupled with an in-line windblown dust model was used to simulate the formation, spatial and temporal characteristics of this dust event, and analyze its impacts. The threshold friction velocity for loose, fine-grained soil with low surface roughness in the dust model was revised based on Chinese data to improve the model performance. This dust storm broke out in Xinjiang and Mongolia during 28 to 30 April and arrived in the YRD region on 1 May. The transported dust particles contributed to the mean surface layer concentrations of PM10 in the YRD region 78.9% during 1 to 6 May with their impact weakening from north to south due to the removal of dust particles along the path. The dry deposition, wet deposition and total deposition of PM10 in the YRD reached 184.7 kt, 172.6 kt and 357.32 kt, respectively. The dust particles also had significant impacts on optical/radiative characteristics by absorption and scattering. In Shanghai, the largest perturbations of aerosol optical depth (AOD) and irradiance were about 0.8 DU and −130 W m−2, which could obviously influence the radiation balance in this region. The decrease of actinic fluxes impacts future photochemistry. In Shanghai, the negative effects on the NO2 and O3 photolysis could be −35% when dust particles arrived. The concentrations of O3 and OH were reduced by 1.5% and 3.1% in the whole of China, and by 9.4% and 12.1% in the YRD region, respectively. Such changes in O3 and OH levels can affect the future formation of secondary aerosols in the atmosphere by directly determining the oxidation rate of their precursors. The work of this manuscript is meaningful for understanding the dust emissions in China as well as for the application of CMAQ in Asia. It is also helpful for understanding the formation mechanism and impacts of dust pollution in the YRD.
On the relationship between Arctic ice clouds and polluted air masses over the North Slope of Alaska in April 2008

Recently, two types of ice clouds (TICs) properties have been characterized using the Indirect and Semi-Direct Aerosol Campaign (ISDAC) airborne measurements (Alaska, April 2008). TIC-2B were characterized by fewer (< 10 L−1) and larger (> 110 μm) ice crystals, and a larger ice supersaturation (> 15%) compared to TIC-1/2A. It has been hypothesized that emissions of SO2 may reduce the ice nucleating properties of ice nuclei (IN) through acidification, resulting in a smaller concentration of larger ice crystals and leading to precipitation (e.g., cloud regime TIC-2B). Here, the origin of air masses forming the ISDAC TIC-1/2A (1 April 2008) and TIC-2B (15 April 2008) is investigated using trajectory tools and satellite data. Results show that the synoptic conditions favor air masses transport from three potential SO2 emission sources into Alaska: eastern China and Siberia where anthropogenic and biomass burning emissions, respectively, are produced, and the volcanic region of the Kamchatka/Aleutians. Weather conditions allow the accumulation of pollutants from eastern China and Siberia over Alaska, most probably with the contribution of acidic volcanic aerosol during the TIC-2B period. Observation Monitoring Instrument (OMI) satellite observations reveal that SO2 concentrations in air masses forming the TIC-2B were larger than in air masses forming the TIC-1/2A. Airborne measurements show high acidity near the TIC-2B flight where humidity was low. These results support the hypothesis that acidic coating on IN could be at the origin of the formation of TIC-2B.