Modeling the Current and Future Roles of Particulate Organic Nitrates in the Southeastern United States

Pye, Havala O. T.; Luecken, Deborah; Xu, Lu; Boyd, Christopher M.; Ng, N. L.; Baker, Kirk R.; Ayres, B. R.; Bash, Jesse O.; Baumann, Karsten; Carter, William; Edgerton, Eric S.; Fry, Juliane L.; Hutzell, William T.; Schwede, Donna; Shepson, P. B.

doi:10.1021/acs.est.5b03738

Cited by 188 publications

(275 citation statements)

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“…These ELVOCs have been observed during both chamber and in situ measurements in Germany (Mutzel et al, 2015). Several studies showed the importance of nighttime SOA formation from MT via nitrate radical oxidation, resulting in the formation of organic nitrates (Pye et al, 2015;Bean and Ruiz, 2016;Xu et al, 2015;Nah et al, 2016). Pye et al (2010) showed the importance of reactive nitrogen and pointed out the fact that organic nitrate accounts for more than a half of the monoterpene oxidation products in the particle phase over the US.…”

Section: Introductionmentioning

confidence: 83%

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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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Section: Introductionmentioning

confidence: 83%

“…Organic nitrates are formed where biogenic VOCs and anthropogenic NO x sources interact (Pye et al, 2015;Xu et al, 2015;Bean and Ruiz, 2016;Nah et al, 2016). We used here the parameterisation of Pye et al (2015) to account for the formation of organic nitrate compounds from the oxidation by OH and NO 3 of MT.…”

Section: Organic Nitrates Formation Mechanismmentioning

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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“…Next to the current 1-D VBS scheme, 2-D schemes have been developed, taking into account not only the saturation vapour pressure but also the O : C ratio (oxygenation state) (Donahue et al, 2011). In addition, the importance and pathways of reactive nitrogen were demonstrated by Pye et al (2010Pye et al ( , 2015. Reactive nitrogen is not yet taken into account.…”

Section: Discussion and Outlookmentioning

confidence: 99%

Curriculum vitae of the LOTOS–EUROS (v2.0) chemistry transport model

et al. 2017

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Abstract. The development and application of chemistry transport models has a long tradition. Within the Netherlands the LOTOS-EUROS model has been developed by a consortium of institutes, after combining its independently developed predecessors in 2005. Recently, version 2.0 of the model was released as an open-source version. This paper presents the curriculum vitae of the model system, describing the model's history, model philosophy, basic features and a validation with EMEP stations for the new benchmark year 2012, and presents cases with the model's most recent and key developments. By setting the model developments in context and providing an outlook for directions for further development, the paper goes beyond the common model description.With an origin in ozone and sulfur modelling for the models LOTOS and EUROS, the application areas were gradually extended with persistent organic pollutants, reactive nitrogen, and primary and secondary particulate matter. After the combination of the models to LOTOS-EUROS in 2005, the model was further developed to include new source parametrizations (e.g. road resuspension, desert dust, wildfires), applied for operational smog forecasts in the Netherlands and Europe, and has been used for emission scenarios, source apportionment, and long-term hindcast and climate change scenarios. LOTOS-EUROS has been a front-runner in data assimilation of ground-based and satellite observations and has participated in many model intercomparison studies. The model is no longer confined to applications over Europe but is also applied to other regions of the world, e.g. China. The increasing interaction with emission experts has also contributed to the improvement of the model's performance. The philosophy for model development has always been to use knowledge that is state of the art and proven, to keep a good balance in the level of detail of process description and accuracy of input and output, and to keep a good record on the effect of model changes using benchmarking and validation. The performance of v2.0 with respect to EMEP observations is good, with spatial correlations around 0.8 or higher for concentrations and wet deposition. Temporal correlations are around 0.5 or higher. Recent innovative applications include source apportionment and data assimilation, particle number modelling, and energy transition scenarios including corresponding land use changes as well as Saharan dust forecasting. Future developments would enable more flexibility with respect to model horizontal and vertical resolution and further detailing of model input data.Published by Copernicus Publications on behalf of the European Geosciences Union.

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“…6). This suggests that isoprene OA formation may be only half of the value found by Kim et al (2015), implying that other sources such as terpenes may make more important contributions to OA (Pye et al, 2010(Pye et al, , 2015Xu et al, 2015).…”

Section: Implications For Surface Air Qualitymentioning

confidence: 92%

High-resolution inversion of OMI formaldehyde columns to quantify isoprene emission on ecosystem-relevant scales: application to the Southeast US

Kaiser¹,

Jacob²,

Zhu³

et al. 2017

Preprint

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Abstract. Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. isoprene emission inventories used in atmospheric models are based on limited vegetation information and uncertain land cover data, leading to potentially large errors. Satellite observations of atmospheric formaldehyde (HCHO), a high-yield isoprene oxidation product, provide 'top-down' information to evaluate isoprene emission inventories through inverse analyses. Past inverse analyses have however been hampered by uncertainty in the HCHO satellite data, uncertainty in the time-and NO x -dependent yield of HCHO from isoprene oxidation, and coarse resolution of the atmospheric models used for 30 the inversion. Here we demonstrate the ability to use HCHO satellite data from OMI in a high-resolution inversion to 2 to correct model NO x biases, which was done here using SEAC 4 RS observations but can be done more generally using satellite NO 2 data concurrently with HCHO. We find in our inversion that isoprene emissions from the widely-used MEGAN v2.1 inventory are biased high over the Southeast US by 40% on average, although the broad-scale distributions are correct including maximum emissions in Arkansas/Louisiana and high base emission factors in the oak-covered Ozarks of Southeast Missouri. A particularly large discrepancy is in the Edwards Plateau of Central Texas where MEGAN v2.1 is too high by a 5 factor of 3, possibly reflecting errors in land cover. The lower isoprene emissions inferred from our inversion, when implemented into GEOS-Chem, decrease surface ozone over the Southeast US by 1-3 ppb and decrease the isoprene contribution to organic aerosol from 40% to 20%.

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Modeling the Current and Future Roles of Particulate Organic Nitrates in the Southeastern United States

Cited by 188 publications

References 75 publications

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

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

Curriculum vitae of the LOTOS–EUROS (v2.0) chemistry transport model

High-resolution inversion of OMI formaldehyde columns to quantify isoprene emission on ecosystem-relevant scales: application to the Southeast US

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