Modeling secondary organic aerosol in an urban area: application to Paris, France

Couvidat, Florian; Kim, Youngseob; Sartelet, Karine; Seigneur, Christian; Marchand, Nicolas; Sciare, Jean

doi:10.5194/acp-13-983-2013

Cited by 74 publications

(102 citation statements)

References 63 publications

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“…POLAIR3D/SIREAM has been used for several applications. For example, it was compared to in situ surface measurements for gas and aerosols over Europe by Sartelet et al (2007Sartelet et al ( , 2012 and Couvidat et al (2012), and over Greater Paris by Couvidat et al (2013); it was compared to AERONET data over Europe by Tombette et al (2008) and to satellite data by Zhang et al (2013); and it was compared to lidar-derived PM 10 over Greater Paris during MEGAPOLI by Royer et al (2011).…”

Section: Polair3d Modelmentioning

confidence: 99%

Modelling and assimilation of lidar signals over Greater Paris during the MEGAPOLI summer campaign

et al. 2014

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Abstract. In this study, we investigate the ability of the chemistry transport model (CTM) POLAIR3D of the air quality modelling platform POLYPHEMUS to simulate lidar backscattered profiles from model aerosol concentration outputs. This investigation is an important preprocessing stage of data assimilation (validation of the observation operator). To do so, simulated lidar signals are compared to hourly lidar observations performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer experiment in July 2009, when a ground-based mobile lidar was deployed around Paris onboard a van. The comparison is performed for six different measurement days, 1, 4, 16, 21, 26 and 29 July 2009, corresponding to different levels of pollution and different atmospheric conditions. Overall, POLYPHEMUS well reproduces the vertical distribution of lidar signals and their temporal variability, especially for 1, 16, 26 and 29 July 2009. Discrepancies on 4 and 21 July 2009 are due to high-altitude aerosol layers, which are not well modelled. In the second part of this study, two new algorithms for assimilating lidar observations based on the optimal interpolation method are presented. One algorithm analyses PM 10 (particulate matter with diameter less than 10 µm) concentrations. Another analyses PM 2.5 (particulate matter with diameter less than 2.5 µm) and PM 2.5−10 (particulate matter with a diameter higher than 2.5 µm and lower than 10 µm) concentrations separately. The aerosol simulations without and with lidar data assimilation (DA) are evaluated using the Airparif (a regional operational network in charge of air quality survey around the Paris area) database to demonstrate the feasibility and usefulness of assimilating lidar profiles for aerosol forecasts. The evaluation shows that lidar DA is more efficient at correcting PM 10 than PM 2.5 , probably because PM 2.5 is better modelled than PM 10 . Furthermore, the algorithm which analyses both PM 2.5 and PM 2.5−10 provides the best scores for PM 10 . The averaged root-mean-square error (RMSE) of PM 10 is 11.63 µg m −3 with DA (PM 2.5 and PM 2.5−10 ), compared to 13.69 µg m −3 with DA (PM 10 ) and 17.74 µg m −3 without DA on 1 July 2009. The averaged RMSE of PM 10 is 4.73 µg m −3 with DA (PM 2.5 and PM 2.5−10 ), against 6.08 µg m −3 with DA (PM 10 ) and 6.67 µg m −3 without DA on 26 July 2009.

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Section: Polair3d Modelmentioning

confidence: 99%

Modelling and assimilation of lidar signals over Greater Paris during the MEGAPOLI summer campaign

et al. 2014

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“…Furthermore, they tend to converge as they continue to be developed and refined. For example, I/S-VOCs from anthropogenic emissions, which are usually specified by volatility classes, can be included in a mechanistic model (Albriet et al, 2010;Couvidat et al, 2013a); also, the VBS scheme can take into account the oxidative state of SOA (Jimenez et al, 2009), in particular its elemental O / C ratio Jathar et al, 2015). The recently developed 1.5-VBS (Koo et al, 2014) assigned a molecular structure to VBS products.…”

Section: Introductionmentioning

confidence: 99%

Modelling organic aerosol concentrations and properties during ChArMEx summer campaigns of 2012 and 2013 in the western Mediterranean region

et al. 2017

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Abstract. In the framework of the Chemistry-Aerosol Mediterranean Experiment, a measurement site was set up at a remote site (Ersa) on Corsica Island in the northwestern Mediterranean Sea. Measurement campaigns performed during the summers of 2012 and 2013 showed high organic aerosol concentrations, mostly from biogenic origin. This work aims to represent the organic aerosol concentrations and properties (oxidation state and hydrophilicity) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Biogenic precursors are isoprene, monoterpenes and sesquiterpenes. In this work, the following model oxidation products of monoterpenes are added: (i) a carboxylic acid (MBTCA) to represent multi-generation oxidation products in the low-NO x regime, (ii) organic nitrate chemistry and (iii) extremely low-volatility organic compounds (ELVOCs) formed by ozonolysis. The model shows good agreement of measurements of organic concentrations for both 2012 and 2013 summer campaigns. The modelled oxidation property and hydrophilic organic carbon properties of the organic aerosols also agree reasonably well with the measurements. The influence of the different chemical processes added to the model on the oxidation level of organics is studied. Measured and simulated water-soluble organic carbon (WSOC) concentrations show that even at a remote site next to the sea, about 64 % of the organic carbon is soluble. The concentrations of WSOC vary with the origins of the air masses and the composition of organic aerosols. The marine organic emissions only contribute to a few percent of the organic mass in PM 1 , with maxima above the sea.

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“…28 Therefore it is found in detectable concentrations within aerosol in cities and urban areas. 29,30 In the presence of strong oxidants such as ozone, squalene yields high molecular weight products such as polyunsaturated aldehydes, similar to those found in the very complex naturally occurring secondary organic aerosols (SOA) in the atmosphere 27,31 . The initial step of squalene ozonolysis will be via the well-known Criegee mechanism which generates carbonyls and carbonyl oxides also known as "Criegee intermediates" via a primary ozonide.…”

Section: Introductionmentioning

confidence: 99%

Dynamic viscosity mapping of the oxidation of squalene aerosol particles

Athanasiadis

Fitzgerald

Davidson

et al. 2016

Phys. Chem. Chem. Phys.

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Organic aerosols (OA) play important roles in multiple atmospheric processes, including climate change, and can impact on human health. The physico-chemical properties of OA are important for all these processes and can evolve through reactions with various atmospheric components, including oxidants. The dynamic nature of these reactions makes it challenging to obtain a true representation of their composition and surface chemistry. Here we investigate the microscopic viscosity of model OA composed of squalene, undergoing chemical aging. We employ Fluorescent Lifetime Imaging Microscopy (FLIM) in conjunction with viscosity sensitive probes termed molecular rotors, in order to image changes in microviscosity in real time during oxidation with ozone and hydroxyl radicals, which are two key oxidising species in the troposphere. We also recorded Raman spectra of levitated particles to follow the reactivity during particle ozonolysis . The levitation of droplets was achieved via optical trapping that enabled simultaneous levitation and measurement via FLIM or Raman spectroscopy and allowed the true aerosol phase to be probed. Our data revealed a very significant increase in viscosity of levitated squalene droplets upon ozonolysis, following their transformation from liquid to solid phase that was not observable when the oxidation was carried out on coverslip mounted droplets. FLIM imaging with sub-micron spatial resolution also revealed spatial heterogeneity in viscosity distribution of oxidised droplets. Overall, a combination of molecular rotors, FLIM and optical trapping is able to provide powerful insights into OA chemistry and the microscopic structure that enables the dynamic monitoring of microscopic viscosity in aerosol particles in its true phase.

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Modeling secondary organic aerosol in an urban area: application to Paris, France

Cited by 74 publications

References 63 publications

Modelling and assimilation of lidar signals over Greater Paris during the MEGAPOLI summer campaign

Modelling and assimilation of lidar signals over Greater Paris during the MEGAPOLI summer campaign

Modelling organic aerosol concentrations and properties during ChArMEx summer campaigns of 2012 and 2013 in the western Mediterranean region

Dynamic viscosity mapping of the oxidation of squalene aerosol particles

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