The objective of this study is to document and evaluate recent changes and updates to the module for aerosols and aerosol-cloud-radiation interactions in the atmospheric module CAM4-Oslo of the core version of the Norwegian Earth System Model (NorESM), NorESM1-M. Particular attention is paid to the role of natural organics, sea salt, and mineral dust in determining the gross aerosol properties as well as the anthropogenic contribution to these properties and the associated direct and indirect radiative forcing. The aerosol module is extended from earlier versions that have been published, and includes life-cycling of sea salt, mineral dust, particulate sulphate, black carbon, and primary and secondary organics. The impacts of most of the numerous changes since previous versions are thoroughly explored by sensitivity experiments. The most important changes are: modified prognostic sea salt emissions; updated treatment of precipitation scavenging and gravitational settling; inclusion of biogenic primary organics and methane sulphonic acid (MSA) from oceans; almost doubled production of land-based biogenic secondary organic aerosols (SOA); and increased ratio of organic matter to organic carbon (OM/OC) for biomass burning aerosols from 1.4 to 2.6. Compared with in situ measurements and remotely sensed data, the new treatments of sea salt and dust aerosols give smaller biases in near-surface mass concentrations and aerosol optical depth than in the earlier model version. The model biases for mass concentrations are approximately unchanged for sulphate and BC. The enhanced levels of modeled OM yield improved overall statistics, even though OM is still underestimated in Europe and overestimated in North America. The global anthropogenic aerosol direct radiative forcing (DRF) at the top of the atmosphere has changed from a small positive value to -0.08 W m(-2) in CAM4-Oslo. The sensitivity tests suggest that this change can be attributed to the new treatment of biomass burning aerosols and gravitational settling. Although it has not been a goal in this study, the new DRF estimate is closer both to the median model estimate from the AeroCom intercomparison and the best estimate in IPCC AR4. Estimated DRF at the ground surface has increased by ca. 60 %, to -1.89 W m(-2). We show that this can be explained by new emission data and omitted mixing of constituents between updrafts and downdrafts in convective clouds. The increased abundance of natural OM and the introduction of a cloud droplet spectral dispersion formulation are the most important contributions to a considerably decreased estimate of the indirect radiative forcing (IndRF). The IndRF is also found to be sensitive to assumptions about the coating of insoluble aerosols by sulphate and OM. The IndRF of -1.2 W m(-2), which is closer to the IPCC AR4 estimates than the previous estimate of -1.9 W m(-2), has thus been obtained without imposing unrealistic artificial lower bounds on cloud droplet number concentrations.

Global climate model output is combined with an emission parameterization to estimate the change in the global and regional sea salt aerosol number emission from 1870 to 2100. Global average results suggest a general increase in sea salt aerosol number emission due to increasing surface wind speed. However, the emission changes are not uniform over the aerosol size spectrum due to an increase in sea surface temperature. From 1870 to 2100 the emission of coarse mode particles (dry diameter D-P > 655 nm) increase by approximately 10 % (global average), whereas no significant change in the emission of ultrafine mode aerosols (dry diameter D-p < 76 nm) was found over the same period. Significant regional differences in the number emission trends were also found. Based on CAM-Oslo global climate model output, no straight-forward relationship was found between the change in the number emissions and changes in the sea salt aerosol burden or optical thickness. This is attributed to a change in the simulated residence time of the sea salt aerosol. For the 21st century, a decrease in the residence time leads to a weaker sea salt aerosol-climate feedback that what would be inferred based on changes in number emissions alone. Finally, quantifying any potential impact on marine stratocumulus cloud microphysical and radiative properties due to changes in sea salt aerosol number emissions is likely to be complicated by commensurate changes in anthropogenic aerosol emissions and changes in meteorology.

From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 mu m diameter (D-p) from a 105m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass < 1 mu m D-p (PM1) with water soluble soil contributing 11% and water insoluble soil 47%. Carbonaceous compounds were at the most 27% of PM1 mass. It was found that heating the air from the tower to 200 degrees C resulted in the loss of approximately 60% of the aerosol volume at 0.25 mu m D-p whereas only 40% of the aerosol volume was removed at 0.6 mu m D-p. Further heating to 300 degrees C caused very little additional losses < 0.6 mu m D-p. The chemical analysis did not include carbonaceous compounds, but based on the difference between the total mass concentration and the sum of the analyzed non-carbonaceous materials, it can be assumed that the non-volatile particulate material (heated to 300 degrees C) consists mainly of carbonaceous compounds, including elemental carbon. Furthermore, it was found that the nonvolatile particle fraction < 0.6 mu m D-p correlated (r(2) = 0.4) with the BC concentration at roof level in the city, supporting the assumption that the non-volatile material consists of carbonaceous compounds. The average diurnal cycles of the BC emissions from road traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx) and BC measured on a densely trafficked street) and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs) for non-volatile particles < 0.6 mu m D-p to be 2.4 +/- 1.4 mg veh(-1) km(-1) based on either CO2 fluxes or traffic activity data. Light (LDV) and heavy duty vehicle (HDV) EFs were estimated using multiple linear regression and reveal that for non-volatile particulate matter in the 0.25 to 0.6 mu m D-p range, the EFHDV is approximately twice as high as the EFLDV, the difference not being statistically significant.

Two semi-empirical models were developed for the Antarctic stratosphere to relate the shift of species within total chlorine (Cl-y = HCl + ClONO2 + HOCl + 2 x Cl-2 + 2xCl(2)O(2) + ClO + Cl) into the active forms (here: ClOx = 2xCl(2)O(2) + ClO), and to relate the rate of ozone destruction to ClOx. These two models provide a fast and computationally inexpensive way to describe the inter- and intra-annual evolution of ClOx and ozone mass deficit (OMD) in the Antarctic spring. The models are based on the underlying physics/chemistry of the system and capture the key chemical and physical processes in the Antarctic stratosphere that determine the interaction between climate change and Antarctic ozone depletion. They were developed considering bulk effects of chemical mechanisms for the duration of the Antarctic vortex period and quantities averaged over the vortex area. The model equations were regressed against observations of daytime ClO and OMD providing a set of empirical fit coefficients. Both semi-empirical models are able to explain much of the intra-and inter-annual variability observed in daily ClOx and OMD time series. This proof-of-concept paper outlines the semi-empirical approach to describing the evolution of Antarctic chlorine activation and ozone depletion.

This paper presents a novel approach to investigate cloud-aerosol interactions by coupling a Markov Chain Monte Carlo (MCMC) algorithm to a pseudo-adiabatic cloud parcel model. Despite the number of numerical cloud-aerosol sensitivity studies previously conducted few have used statistical analysis tools to investigate the sensitivity of a cloud model to input aerosol physiochemical parameters. Using synthetic data as observed values of cloud droplet number concentration (CDNC) distribution, this inverse modelling framework is shown to successfully converge to the correct calibration parameters. The employed analysis method provides a new, integrative framework to evaluate the sensitivity of the derived CDNC distribution to the input parameters describing the lognormal properties of the accumulation mode and the particle chemistry. To a large extent, results from prior studies are confirmed, but the present study also provides some additional insightful findings. There is a clear transition from very clean marine Arctic conditions where the aerosol parameters representing the mean radius and geometric standard deviation of the accumulation mode are found to be most important for determining the CDNC distribution to very polluted continental environments (aerosol concentration in the accumulation mode >1000 cm⁻³) where particle chemistry is more important than both number concentration and size of the accumulation mode. The competition and compensation between the cloud model input parameters illustrate that if the soluble mass fraction is reduced, both the number of particles and geometric standard deviation must increase and the mean radius of the accumulation mode must increase in order to achieve the same CDNC distribution. For more polluted aerosol conditions, with a reduction in soluble mass fraction the parameter correlation becomes weaker and more non-linear over the range of possible solutions (indicative of the sensitivity). This indicates that for the cloud parcel model used herein, the relative importance of the soluble mass fraction appears to decrease if the number or geometric standard deviation of the accumulation mode is increased. This study demonstrates that inverse modelling provides a flexible, transparent and integrative method for efficiently exploring cloud-aerosol interactions efficiently with respect to parameter sensitivity and correlation.

We present observations of methane (CH4) mixing ratio and C-13/C-12 isotopic ratios in CH4 (delta C-13) data from a collaborative shipboard project using bulk carrier ships sailing between Nelson, New Zealand, and Osaka, Japan, in the western Pacific Ocean. Measurements of the CH4 mixing ratio and delta C-13 in CH4 were obtained from large clean-air samples collected in each 2.5 degrees to 5 degrees of latitude between 30 degrees S and 30 degrees N on eight voyages from 2004 to 2007. The data show large variations in CH4 mixing ratio in the tropical western Pacific, and data analysis suggests that these large variations are related to the positions and strengths of the South Pacific Convergence Zone and the Intertropical Convergence Zone, with variability in the sources playing a much smaller role. These measurements are compared with results from a modified version of the Unified Model (UMeth) general circulation model along two transects, one similar to the ship transects and another 18.75 degrees to the east. Although UMeth was run to a steady state with the same sources and sinks each year, the gradient structures varied considerably from year to year, supporting our conclusion that variability in transport is a major driver for the observed variations in CH4. Simulations forced with an idealized representation of the El Nino-Southern Oscillation (ENSO) suggest that a large component of the observed variability in latitudinal gradients of CH4 and its delta C-13 arises from intrinsic variability in the climate system that does not occur on ENSO time scales.

Recently, it was shown that of the ozone-depleting substances currently emitted, N2O emissions (the primary source of stratospheric NOx) dominate, and are likely to do so throughout the 21st century. To investigate the links between N2O and NOx concentrations, and the effects of NOx on ozone in a changing climate, the evolution of stratospheric ozone from 1960 to 2100 was simulated using the NIWA-SOCOL chemistry-climate model. The yield of NOx from N2O is reduced due to stratospheric cooling and a strengthening of the Brewer-Dobson circulation. After accounting for the reduced NOx yield, additional weakening of the primary NOx cycle is attributed to reduced availability of atomic oxygen, due to a) stratospheric cooling decreasing the atomic oxygen/ozone ratio, and b) enhanced rates of chlorine-catalyzed ozone loss cycles around 2000 and enhanced rates of HOx-induced ozone depletion. Our results suggest that the effects of N2O on ozone depend on both the radiative and chemical environment of the upper stratosphere, specifically CO2-induced cooling of the stratosphere and elevated CH4 emissions which enhance HOx-induced ozone loss and remove the availability of atomic oxygen to participate in NOx ozone loss cycles. Citation: Revell, L. E., G. E. Bodeker, D. Smale, R. Lehmann, P. E. Huck, B. E. Williamson, E. Rozanov, and H. Struthers (2012), The effectiveness of N2O in depleting stratospheric ozone, Geophys. Res. Lett., 39, L15806, doi:10.1029/2012GL052143.

Understanding Arctic climate change requires knowledge of both the external and the local drivers of Arctic climate as well as local feedbacks within the system. An Arctic feedback mechanism relating changes in sea ice extent to an alteration of the emission of sea salt aerosol and the consequent change in radiative balance is examined. A set of idealized climate model simulations were performed to quantify the radiative effects of changes in sea salt aerosol emissions induced by prescribed changes in sea ice extent. The model was forced using sea ice concentrations consistent with present day conditions and projections of sea ice extent for 2100. Sea salt aerosol emissions increase in response to a decrease in sea ice, the model results showing an annual average increase in number emission over the polar cap (70-90 degrees N) of 86 x 10(6) m(-2) s(-1) (mass emission increase of 23 mu g m(-2) s(-1)). This in turn leads to an increase in the natural aerosol optical depth of approximately 23%. In response to changes in aerosol optical depth, the natural component of the aerosol direct forcing over the Arctic polar cap is estimated to be between -0.2 and -0.4 W M(-2) for the summer months, which results in a negative feedback on the system. The model predicts that the change in first indirect aerosol effect (cloud albedo effect) is approximately a factor of ten greater than the change in direct aerosol forcing although this result is highly uncertain due to the crude representation of Arctic clouds and aerosol-cloud interactions in the model. This study shows that both the natural aerosol direct and first indirect effects are strongly dependent on the surface albedo, highlighting the strong coupling between sea ice, aerosols, Arctic clouds and their radiative effects.

Size-resolved aerosol vertical number fluxes were measured using the eddy covariance method, 105 meters above the ground over the city of Stockholm, Sweden, between 1st April 2008 and 15th April 2009. The size range of the measurements cover particles from 0.25 to 2.5 μm diameter (D_p). Emission velocities (v_e) were calculated for the same size range and were found to be well correlated with friction velocity (u_*) and CO₂ fluxes (F_CO2). These variables were used to parameterize the emission velocity aswhere v_e and u_* are given in [m s⁻¹], D_p in [μm], and F_CO2 in [mmol m⁻²s⁻¹].

The parameterization reproduces the average diurnal cycle from the observations well for particles sizes up to 0.6 μm D_p. For larger particles the parameterization tends to over predict the emission velocity. These larger particles are not believed to be produced by combustion and therefore not well represented by F_CO2, which represents the traffic source through its fossil fuel consumption and the related CO₂ emissions.

Coupled chemistry-climate model simulations covering the recent past and continuing throughout the 21st century have been completed with a range of different models. Common forcings are used for the halogen amounts and greenhouse gas concentrations, as expected under the Montreal Protocol (with amendments) and Intergovernmental Panel on Climate Change A1b Scenario. The simulations of the Antarctic ozone hole are compared using commonly used diagnostics: the minimum ozone, the maximum area of ozone below 220 DU, and the ozone mass deficit below 220 DU. Despite the fact that the processes responsible for ozone depletion are reasonably well understood, a wide range of results is obtained. Comparisons with observations indicate that one of the reasons for the model underprediction in ozone hole area is the tendency for models to underpredict, by up to 35%, the area of low temperatures responsible for polar stratospheric cloud formation. Models also typically have species gradients that are too weak at the edge of the polar vortex, suggesting that there is too much mixing of air across the vortex edge. Other models show a high bias in total column ozone which restricts the size of the ozone hole (defined by a 220 DU threshold). The results of those models which agree best with observations are examined in more detail. For several models the ozone hole does not disappear this century but a small ozone hole of up to three million square kilometers continues to occur in most springs even after 2070.