Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis

International audienceA global 3-dimensional chemistry/transport model able to describe O3, NOx, Volatile Organic Compounds (VOC), sulphur and NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA) formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. The studied uncertainties in the SOA budget have been evaluated to be in decreasing importance: the potentially irreversible sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols, the chemical fate of the first generation products and finally the activity coefficient of the condensable species. The large uncertainties associated with the emissions of VOC and the adopted simplification of chemistry have not been investigated in this study. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the lower ones

Formation of secondary organic aerosol from isoprene oxidation over Europe

The role of isoprene as a precursor to secondary organic aerosol (SOA) over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr<sup>−1</sup> and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter (OM) during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC) emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning) of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr<sup>−1</sup>). The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights in isoprene SOA formation mechanisms reduces the tropospheric production of isoprene derived SOA over Europe from 0.4 Tg yr<sup>−1</sup> in our reference simulation to 0.1 Tg yr<sup>−1</sup>

Evaluating Ammonium, Nitrate and Sulfate Aerosols in 3-Dimensions

The effect aerosols have on climate and air quality is a func-on of their chemical composi-on, concentra-on and spa-al distribu-on. These parameters are controlled by emissions, heterogeneous and homogeneous chemistry, where thermodynamics plays a key role, transport, which includes stratospheric- tropospheric exchange, and deposi-onal sinks. In this work we demonstrate the effect of some of these processes on the SO4NH4NO3 system using the GISS ModelE2 Global Circula-on Model (GCM)

Regional and global temperature response to anthropogenic SO2 emissions from China in three climate models

We use the HadGEM3-GA4, CESM1, and GISS ModelE2 climate models to investigate the global and regional aerosol burden, radiative flux, and surface temperature responses to removing anthropogenic sulfur dioxide (SO2) emissions from China. We find that the models differ by up to a factor of six in the simulated change in aerosol optical depth (AOD) and shortwave radiative flux over China that results from reduced sulfate aerosol, leading to a large range of magnitudes in the regional and global temperature responses. Two of the three models simulate a near-ubiquitous hemispheric warming due to the regional SO2 removal, with similarities in the local and remote pattern of response, but overall with a substantially different magnitude. The third model simulates almost no significant temperature response. We attribute the discrepancies in the response to a combination of substantial differences in the chemical conversion of SO2 to sulfate, translation of sulfate mass into AOD, cloud radiative interactions, and differences in the radiative forcing efficiency of sulfate aerosol in the models. The model with the strongest response (HadGEM3-GA4) compares best with observations of AOD regionally, however the other two models compare similarly (albeit poorly) and still disagree substantially in their simulated climate response, indicating th at total AOD observations are far from sufficient to determine which model response is more plausible. Our results highlight that there remains a large uncertainty in the representation of both aerosol chemistry as well as direct and indirect aerosol radiative effects in current climate models, and reinforces that caution must be applied when interpreting the results of modelling studies of aerosol influences on climate. Model studies that implicate aerosols in climate responses should ideally explore a range of radiative forcing strengths representative of this uncertainty, in addition to thoroughly evaluating the models used against observations

Impact of Improvements in Volcanic Implementation on Atmospheric Chemistry and Climate in the GISS-E2 Model

The representation of volcanic eruptions in climate models introduces some of the largest errors when evaluating historical simulations, partly due to the crude model parameterizations. We will show preliminary results from the Goddard Institute for Space Studies (GISS)-E2 model comparing traditional highly parameterized volcanic implementation (specified Aerosol Optical Depth, Effective Radius) to deploying the full aerosol microphysics module MATRIX and directly emitting SO2 allowing us the prognosically determine the chemistry and climate impact. We show a reasonable match in aerosol optical depth, effective radius, and forcing between the full aerosol implementation and reconstructions/observations of the Mt. Pinatubo 1991 eruption, with a few areas as targets for future improvement. This allows us to investigate not only the climate impact of the injection of volcanic aerosols, but also influences on regional water vapor, O3, and OH distributions. With the skill of the MATRIX volcano implementation established, we explore (1) how the height of the injection column of SO2 influence atmospheric chemistry and climate response, (2) how the initial condition of the atmosphere influences the climate and chemistry impact of the eruption with a particular focus on how ENSO and QBO and (3) how the coupled chemistry could mitigate the climate signal for much larger eruptions (i.e. the 1258 eruption, reconstructed to be approximately 10x Pinatubo). During each sensitivity experiment we assess the impact on profiles of water vapor, O3, and OH, and assess how the eruption impacts the budget of each

Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics 1.0: A General Circulation Model for Simulating the Climates of Rocky Planets

Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics (ROCKE-3D) is a 3-Dimensional General Circulation Model (GCM) developed at the NASA Goddard Institute for Space Studies for the modeling of atmospheres of Solar System and exoplanetary terrestrial planets. Its parent model, known as ModelE2 (Schmidt et al. 2014), is used to simulate modern and 21st Century Earth and near-term paleo-Earth climates. ROCKE-3D is an ongoing effort to expand the capabilities of ModelE2 to handle a broader range of atmospheric conditions including higher and lower atmospheric pressures, more diverse chemistries and compositions, larger and smaller planet radii and gravity, different rotation rates (slowly rotating to more rapidly rotating than modern Earth, including synchronous rotation), diverse ocean and land distributions and topographies, and potential basic biosphere functions. The first aim of ROCKE-3D is to model planetary atmospheres on terrestrial worlds within the Solar System such as paleo-Earth, modern and paleo-Mars, paleo-Venus, and Saturn's moon Titan. By validating the model for a broad range of temperatures, pressures, and atmospheric constituents we can then expand its capabilities further to those exoplanetary rocky worlds that have been discovered in the past and those to be discovered in the future. We discuss the current and near-future capabilities of ROCKE-3D as a community model for studying planetary and exoplanetary atmospheres.Comment: Revisions since previous draft. Now submitted to Astrophysical Journal Supplement Serie

Formation of Secondary Organic Aerosol from Isoprene Oxidation over Europe

The role of isoprene as a precursor to secondary organic aerosol (SOA) over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr-1 and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of particulate organic matter (POM) during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC) emissions from vegetation. However, during winter, our model strongly underestimates POM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning) of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr-1). The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Tropospheric isoprene SOA production over Europe in summer more than doubles when, in addition to preexisting carbonaceous aerosols, condensation of semi volatile vapours on ammonium and sulphate aerosols is considered. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights in isoprene SOA formation mechanisms reduces the tropospheric production of isoprene derived SOA over Europe from 0.4 Tg yr-1 in our reference simulation to 0.1 Tg yr-1JRC.DDG.H.2-Climate chang

Model-Based Estimation of Sampling-Caused Uncertainty in Aerosol Remote Sensing for Climate Research Applications

To evaluate the effect of sampling frequency on the global monthly mean aerosol optical thickness (AOT), we use 6 years of geographical coordinates of Moderate Resolution Imaging Spectroradiometer (MODIS) L2 aerosol data, daily global aerosol fields generated by the Goddard Institute for Space Studies General Circulation Model and the chemical transport models Global Ozone Chemistry Aerosol Radiation and Transport, Spectral Radiationtransport Model for Aerosol Species and Transport Model 5, at a spatial resolution between 1.125 deg 1.125 deg and 2 deg 3: the analysis is restricted to 60 deg S-60 deg N geographical latitude. We found that, in general, the MODIS coverage causes an underestimate of the global mean AOT over the ocean. The long-term mean absolute monthly difference between all and dark target (DT) pixels was 0.01-0.02 over the ocean and 0.03-0.09 over the land, depending on the model dataset. Negative DT biases peak during boreal summers, reaching 0.07-0.12 (30-45% of the global long-term mean AOT). Addition of the Deep Blue pixels tempers the seasonal dependence of the DT biases and reduces the mean AOT difference over land by 0.01-0.02. These results provide a quantitative measure of the effect the pixel exclusion due to cloud contamination, ocean sun-glint and land type has on the MODIS estimates of the global monthly mean AOT. We also simulate global monthly mean AOT estimates from measurements provided by pixel-wide along-track instruments such as the Aerosol Polarimetry Sensor and the Cloud-Aerosol LiDAR with Orthogonal Polarization. We estimate the probable range of the global AOT standard error for an along-track sensor to be 0.0005-0.0015 (ocean) and 0.0029-0.01 (land) or 0.5-1.2% and 1.1-4% of the corresponding global means. These estimates represent errors due to sampling only and do not include potential retrieval errors. They are smaller than or comparable to the published estimate of 0.01 as being a climatologically significant change in the global mean AOT, suggesting that sampling density is unlikely to limit the use of such instruments for climate applications at least on a global, monthly scale

Reconciling Warming Trends

Climate models projected stronger warming over the past 15 years than has been seen in observations. Conspiring factors of errors in volcanic and solar inputs, representations of aerosols, and El NiNo evolution, may explain most of the discrepancy

MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range