Karine Sartelet

Evaluation of the Weather Research and Forecast/Urban Model Over Greater Paris

Meteorological modelling in the planetary boundary layer (PBL) over Greater Paris is performed using the Weather Research and Forecast (WRF) numerical model. The simulated meteorological fields are evaluated by comparison with mean diurnal observational data or mean vertical profiles of temperature, wind speed, humidity and boundary-layer height from 6 to 27 May 2005. Different PBL schemes, which parametrize the atmospheric turbulence in the PBL using different turbulence closure schemes, may be used in the WRF model. The sensitivity of the results to four PBL schemes (two non-local closure schemes and two local closure schemes) is estimated. Uncertainties in the PBL schemes are compared to the influence of the urban canopy model (UCM) and the updated Coordination of Information on the Environment (CORINE) land-use data. Using the UCM and the CORINE land-use data produces more realistic modelled meteorological fields. The wind speed, which is overestimated in the simulations without the UCM, is improved below 1,000 m height. Furthermore, the modelled PBL heights during nighttime are strongly modified, with an increase that may be as high as 200 %. At night, the impact of changing the PBL scheme is lower than the impact of using the UCM and the CORINE land-use data.

Comparison of different gas-phase mechanisms and aerosol modules for simulating particulate matter formation.

ABSTRACT The effects of two gas-phase chemical kinetic mechanisms, Regional Atmospheric Chemistry Mechanism version 2 (RACM2) and Carbon-Bond 05 (CB05), and two secondary organic aerosol (SOA) modules, the Secondary Organic Aerosoi Model (SORGAM) and AER/EPRI/Caltech model (AEC), on fine (aerodynamic diameter ≤2.5 μm) particulate matter (PM2.5) formation is studied. The major sources of uncertainty in the chemistry of SOA formation are investigated. The use of all major SOA precursors and the treatment of SOA oligomerization are found to be the most important factors for SOA formation, leading to 66% and 60% more SOA, respectively. The explicit representation of high-NOx and low-NOx gas-phase chemical regimes is also important with increases in SOA of 30–120% depending on the approach used to implement the distinct SOA yields within the gas-phase chemical kinetic mechanism; further work is needed to develop gas-phase mechanisms that are fully compatible with SOA formation algorithms. The treatment of isoprene SOA as hydrophobic or hydrophilic leads to a significant difference, with more SOA being formed in the latter case. The activity coefficients may also be a major source of uncertainty, as they may differ significantly between atmospheric particles, which contain a myriad of SOA, primary organic aerosol (POA), and inorganic aerosol species, and particles formed in a smog chamber from a single precursor under dry conditions. Significant interactions exist between the uncertainties of the gas-phase chemistry and those of the SOA module. IMPLICATIONS The current state of the science is more advanced for the gas-phase chemistry of ozone formation than for the chemistry and gas/particle partitioning of particulate matter (PM) formation. As a result, there are larger uncertainties associated with aerosol modules than with gas-phase chemical kinetic mechanisms. Nevertheless, the uncertainties associated with those modules are not additive in an air quality model and there are close interactions between the gas-phase chemical mechanism and the secondary aerosol formation. In particular, the effect of the NOx regime on SOA formation should be explicitly treated in air quality models.

Development and Preliminary Validation of a Modal Aerosol Model for Tropospheric Chemistry: MAM

This paper presents a modal aerosol model (MAM) developed to be used in three dimensional air quality models. MAM, which represents the aerosol distribution with four modes, has the advantage of simplicity and speed efficiency associated to modal models, while mass transfer is modeled with a dynamic approach. To assess the ability of MAM to represent mass transfer, MAM is compared to a size-resolved model based on the dynamic approach and to a version of MAM based on an equilibrium approach. Comparisons are done using measurements of inorganic species made in Japan as initial conditions. Furthermore, it is shown that MAM combined with a well chosen mode splitting scheme is able to deal accurately with the simultaneous occurrence of strong nucleation/condensation and coagulation, as may be observed in high nucleation episodes.

MICS Asia Phase II - Sensitivity to the aerosol module

In the framework of the model inter-comparison study - Asia Phase II (MICS2), where eight models are compared over East Asia, this paper studies the influence of different parameterizations used in the aerosol module on the aerosol concentrations of sulfate and nitrate in PM10. An intracomparison of aerosol concentrations is done for March 2001 using different configurations of the aerosol module of one of the model used for the intercomparison. Single modifications of a reference setup for model configurations are performed and compared to a reference case. These modifications concern the size distribution, i.e. the number of sections, and physical processes, i.e. coagulation, condensation/evaporation, cloud chemistry, heterogeneous reactions and sea-salt emissions. Comparing monthly averaged concentrations at different stations, the importance of each parameterization is first assessed. It is found that sulfate concentrations are little sensitive to sea-salt emissions and to whether condensation is computed dynamically or by assuming thermodynamic equilibrium. Nitrate concentrations are little sensitive to cloud chemistry. However, a very high sensitivity to heterogeneous reactions is observed. Thereafter, the variability of the aerosol concentrations to the use of different chemistry transport models (CTMs) and the variability to the use of different parameterizations in the aerosol module are compared. For sulfate, the variability to the use of different parameterizations in the aerosol module is lower than the variability to the use of different CTMs. However, for nitrate, for monthly averaged concentrations averaged over four stations, these two variabilities have the same order of magnitude.

Decadal simulation and comprehensive evaluation of CESM/CAM5.1 with advanced chemistry, aerosol microphysics, and aerosol‐cloud interactions

Earth system models have been used for climate predictions in recent years due to their capabilities to include biogeochemical cycles, human impacts, as well as coupled and interactive representations of Earth system components (e.g., atmosphere, ocean, land, and sea ice). In this work, the Community Earth System Model (CESM) with advanced chemistry and aerosol treatments, referred to as CESM-NCSU, is applied for decadal (2001–2010) global climate predictions. A comprehensive evaluation is performed focusing on the atmospheric component—the Community Atmosphere Model version 5.1 (CAM5.1) by comparing simulation results with observations/reanalysis data and CESM ensemble simulations from the Coupled Model Intercomparison Project phase 5 (CMIP5). The improved model can predict most meteorological and radiative variables relatively well with normalized mean biases (NMBs) of −14.1 to −9.7% and 0.7–10.8%, respectively, although temperature at 2 m (T2) is slightly underpredicted. Cloud variables such as cloud fraction (CF) and precipitating water vapor (PWV) are well predicted, with NMBs of −10.5 to 0.4%, whereas cloud condensation nuclei (CCN), cloud liquid water path (LWP), and cloud optical thickness (COT) are moderately-to-largely underpredicted, with NMBs of −82.2 to −31.2%, and cloud droplet number concentration (CDNC) is overpredictd by 26.7%. These biases indicate the limitations and uncertainties associated with cloud microphysics (e.g., resolved clouds and subgrid-scale cumulus clouds). Chemical concentrations over the continental U.S. (CONUS) (e.g., SO42−, Cl−, OC, and PM2.5) are reasonably well predicted with NMBs of −12.8 to −1.18%. Concentrations of SO2, SO42−, and PM10 are also reasonably well predicted over Europe with NMBs of −20.8 to −5.2%, so are predictions of SO2 concentrations over the East Asia with an NMB of −18.2%, and the tropospheric ozone residual (TOR) over the globe with an NMB of −3.5%. Most meteorological and radiative variables predicted by CESM-NCSU agree well overall with those predicted by CESM-CMIP5. The performance of LWP and AOD predicted by CESM-NCSU is better than that of CESM-CMIP5 in terms of model bias and correlation coefficients. Large biases for some chemical predictions can be attributed to uncertainties in the emissions of precursor gases (e.g., SO2, NH3, and NOx) and primary aerosols (black carbon and primary organic matter) as well as uncertainties in formulations of some model components (e.g., online dust and sea-salt emissions, secondary organic aerosol formation, and cloud microphysics). Comparisons of CESM simulation with baseline emissions and 20% of anthropogenic emissions from the baseline emissions indicate that anthropogenic gas and aerosol species can decrease downwelling shortwave radiation (FSDS) by 4.7 W m−2 (or by 2.9%) and increase SWCF by 3.2 W m−2 (or by 3.1%) in the global mean.

Investigating the Impact of Aqueous-Phase Chemistry and Wet Deposition on Organic Aerosol Formation Using a Molecular Surrogate Modeling Approach

A molecular surrogate representation of secondary organic aerosol (SOA) formation is used to investigate the effect of aqueous-phase (in clouds and particles) chemical processing and wet deposition on SOA atmospheric concentrations. To that end, the hydrophilic/hydrophobic organic (H(2)O) model was augmented to account for several gas/aqueous-phase equilibria and aqueous-phase processes, including the formation of oxalic, glyoxilic and pyruvic acids, the oxidation of methyl vinyl ketone (MVK) and methacrolein (MACR), the formation of tetrols and organosulfates from epoxydiols (IEPOX), and further oxidation of water-soluble SOA (aging). Among those processes, SOA chemical aging and IEPOX reactions led to the most significant increases (up to 1 μg m(-3) in some areas) in SOA concentrations in a one-month summer simulation over Europe. However, large uncertainties remain in the gas/aqueous-phase partitioning of oxalic acid, MVK, and MACR. Below-cloud scavenging of SOA precursor gases and of gas-phase SVOC was found to affect SOA concentrations by up to 20%, which suggests that it should be taken into account in air quality models.

Precursors and formation of secondary organic aerosols fromwildfires in the Euro-Mediterranean region

This work aims at quantifying the relative contribution of secondary organic aerosol (SOA) precursors emitted by wildfires to organic aerosol (OA) formation, during summer 2007 over the Euro-Mediterranean region, where intense wildfires occurred. A new SOA formation mechanism, HOaro, including recently identified aromatic volatile organic compounds (VOCs) emitted from wildfires is developed based on smog chamber experiment measurements, under low and high-NOx regimes. The aromatic VOCs included in the mechanism are toluene, xylene, benzene, phenol, cresol, catechol, furan, naph5 thalene, methylnaphthalene, syringol, guaiacol and structurally assigned and unassigned compounds with at least 6 carbon atoms per molecule (USC>6). This mechanism HOaro is an extension of the HO (Hydrophilic/Hydrophobic organic) aerosol mechanism: the oxidation of the precursor forms surrogate species with specific thermodynamic properties (volatility, oxidation degree, affinity to water). The SOA concentrations over the Euro-Mediterranean region in summer 2007 are simulated using the chemistry transport model (CTM) Polair3D of the air-quality plateform Polyphemus, where the mechanism HOaro 10 was implemented. To estimate the relative contribution of the aromatic VOCs, intermediate, semi and low volatile organic compounds (I/S/L-VOCs) to wildfires OA concentrations, different estimations of the gaseous I/S/L-VOC emissions (from primary organic aerosol (POA) using a factor of 1.5 or from non-methanic organic gas (NMOG) using a factor of 0.36) and their ageing (one-step oxidation vs multi-generational oxidation), are also tested in the CTM. Most of the particle organic aerosol (OA) concentrations are formed from I/S/L-VOCs. In average during the summer 2007 15 and over the Euro-Mediterranean domain, they are about 10 times higher than the OA concentrations formed from VOCs. However, locally, the OA concentrations formed from VOCs can represent up to 30% of the OA concentrations from biomass burning. Amongst the VOCs, the main contributors to SOA formation are phenol, benzene and catechol (47%), USC>6 compounds (23%), and toluene and xylene (12%). Sensitivity studies of the influence of the VOCs and the I/S/L-VOCs emissions and chemical ageing mechanisms on PM2.5 concentrations show that surface PM2.5 concentrations are more sensitive to the 20 parameterization used for gaseous I/S/L-VOCs emissions than for ageing. Estimating the gaseous I/S/L-VOCs emissions from POA or from NMOG has a high impact on local surface PM2.5 concentrations (reaching -30% in Balkans, -8 to -16% in the fire plume and +8 to +16% in Greece). Considering the VOC emissions results in a moderate increase of PM2.5 concentrations 1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1065 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 22 October 2018 c

Impact of wildfires on particulate matter in the Euro-Mediterranean in 2007: sensitivity to the parameterization of emissions in air quality models

This study examines the uncertainties on air quality modeling associated with the integration of wildfire emissions in chemistry-transport models (CTMs). To do so, aerosol concentrations during the summer of 2007, which was marked by severe fire episodes in the EuroMediterranean region especially in the Balkans (20–31 July, 24–30 August 2007) and Greece (24–30 August 2007), are analyzed. Through comparisons to observations from surface networks and satellite remote sensing, we evaluate the abilities of two CTMs, Polyphemus/Polair3D and CHIMERE, to simulate the impact of fires on the regional particulate matter (PM) concentrations and optical properties. During the two main fire events, fire emissions may contribute up to 90 % of surface PM2.5 concentrations in the fire regions (Balkans and Greece), with a significant regional impact associated with long-range transport. Good general performances of the models and a clear improvement of PM2.5 and aerosol optical depth (AOD) are shown when fires are taken into account in the models with high correlation coefficients. Two sources of uncertainties are specifically analyzed in terms of surface PM2.5 concentrations and AOD using sensitivity simulations: secondary organic aerosol (SOA) formation from intermediate and semi-volatile organic compounds (I/S-VOCs) and emissions’ injection heights. The analysis highlights that surface PM2.5 concentrations are highly sensitive to injection heights (with a sensitivity that can be as high as 50 % compared to the sensitivity to I/S-VOC emissions which is lower than 30 %). However, AOD which is vertically integrated is less sensitive to the injection heights (mostly below 20 %) but highly sensitive to I/S-VOC emissions (with sensitivity that can be as high as 40 %). The maximum statistical dispersion, which quantifies uncertainties related to fire emission modeling, is up to 75 % for PM2.5 in the Balkans and Greece, and varies between 36 % and 45 % for AOD above fire regions. The simulated number of daily exceedance of World Health Organization (WHO) recommendations for PM2.5 over the considered region reaches 30 days in regions affected by fires and ∼ 10 days in fire plumes, which is slightly underestimated compared to available observations. The maximum statistical dispersion (σ ) on this indicator is also large (with σ reaching 15 days), showing the need for better understanding of the transport and evolution of fire plumes in addition to fire emissions.

Modeling organic aerosol concentrations and properties duringwinter 2014 in the northwestern Mediterranean region

Organic aerosols are measured at a remote site (Ersa) on Corsica Cape in the northwestern Mediterranean basin during the Chemistry-Aerosol Mediterranean Experiment (CharMEx) winter campaign of 2014, when high organic concentrations from anthropogenic origin are observed. This work aims at representing the observed organic aerosol concentrations and properties (oxidation state) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Because intermediate/semi-volatile organic compounds (I/S-VOC) are the main precursors of SOA at Ersa 5 during the winter 2014, different parameterizations to represent the emission and ageing of I/S-VOC were implemented in the chemistry-transport model of the air-quality platform Polyphemus (different volatility distribution emissions, single-step oxidation vs multi-step oxidation within a Volatility Basis Set framework, inclusion of non-traditional volatile organic compounds NTVOC). Simulations using the different parameterizations are compared to each other and to the measurements (concentration and oxidation state). The high observed organic concentrations are well reproduced whatever the parameterizations. They 10 are slightly under-estimated with most parameterizations, but they are slightly over-estimated when the ageing of NTVOC is taken into account. The volatility distribution at emissions influences more strongly the concentrations than the choice of the parameterization that may be used for ageing (single-step oxidation vs multi-step oxidation), stressing the importance of an accurate characterization of emissions. Assuming the volatility distribution of sectors other than residential heating to be the same as residential heating may lead to a strong under-estimation of organic concentrations. The observed organic oxidation 15 and oxygenation states are strongly under-estimated in all simulations, even when a recently developed parameterization for modeling the ageing of I/S-VOC from residential heating is used. This suggests that uncertainties in the ageing of I/S-VOC emissions remain to be elucidated, with a potential role of organic nitrate from anthropogenic precursors and highly oxygenated organic molecules. 1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-149 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 26 April 2018 c

Modelling of Externally-Mixed Particles in the Atmosphere

This study presents the development of a new 3D size-composition resolved aerosol model (SCRAM). It solves the aerosol dynamic evolution for external mixtures taking into account the processes of coagulation, condensation/evaporation and nucleation. Both the size of particles and the mass fraction of each chemical compound are discretised. For a given particle size, particles of different chemical compositions may co-exist. Chemical components can be grouped into aggregates to reduce computational cost. SCRAM is coupled to the air quality model Polair3d/Polyphemus, and its performance to model air quality over Greater Paris is evaluated, as well as the consequences of the internally mixed assumption on aerosol distribution, composition and optical properties.