Global modeling of the nitrate radical (NO3) for present and pre-industrial scenarios

Khan, M. Anwar H.; Cooke, Michael; Utembe, Steven R.; Archibald, Alexander T.; Derwent, R.G.; Xiao, Peng; Percival, Carl J.; Jenkin, Michael E.; Morris, William C.; Shallcross, Dudley E.

doi:10.1016/j.atmosres.2015.06.006

Cited by 44 publications

(40 citation statements)

References 90 publications

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“…1. NO 3 experiences a very large change between PI and PD (up to more than 1000 % in the Northern Hemisphere), which is also seen in other model studies that show good agreement between modeled presentday concentrations of NO 3 and observations (Khan et al, 2015). The prescribed PI values of surface layer O 3 in the region around Paris used in this study are around a factor of 2 higher than the measured PI values at a station near Paris in the study of Volz and Kley (1988) corresponds with findings from other studies (Parrish et al, 2014).…”

Section: Reaction Reactionsupporting

confidence: 82%

“…Lohmann (2017) shows that model estimates of ERF ari+aci (ari is aerosol-radiation interactions and aci is aerosol-cloud interactions) vary from −0.07 to −3.41 W m −2 , while the Fifth Assessment Report (AR5) from the Intergovernmental Panel on Climate Change (IPCC) gives an expert judgement of ERF ari+aci of −0.9 W m −2 , with a 5 to 95 % uncertainty range of −1.9 to −0.1 W m −2 mostly coming from the uncertainties in the aci component (Boucher et al, 2013). Uncertainties in the natural background emissions have been highlighted as a large contributor to the uncertainty in the indirect effects (Lohmann et al, 2000;Kirkevåg et al, 2008;Hoose et al, 2009;Carslaw et al, 2013), while pointed out that its sensitivity to parameterizations of microphysical processes in global models is even higher. In this study, we examine a third factor, namely the oxidants involved in the formation of aerosols.…”

Section: Introductionmentioning

confidence: 99%

“…This is especially the case for the time period before the industrial era, where it is limited to simple measurements of surface ozone from a few European stations (Volz and Kley, 1988). Despite this limitation, results from model simulations based on information about emission changes, in combination with the few oxidant measurements that exist, give an indication of how the oxidative power of the atmosphere has changed since preindustrial time (Prinn, 2003;Berntsen et al, 1997;Wang and Jacob, 1998;Tsigaridis et al, 2006;Naik et al, 2013a;Naik et al, 2013b;Young et al, 2013;Murray et al, 2014;Khan et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

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Strong impacts on aerosol indirect effects from historical oxidant changes

Karset,

Berntsen,

Storelvmo

et al. 2018

Atmos. Chem. Phys.

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Abstract. Uncertainties in effective radiative forcings through aerosol–cloud interactions (ERFaci, also called aerosol indirect effects) contribute strongly to the uncertainty in the total preindustrial-to-present-day anthropogenic forcing. Some forcing estimates of the total aerosol indirect effect are so negative that they even offset the greenhouse gas forcing. This study highlights the role of oxidants in modeling of preindustrial-to-present-day aerosol indirect effects. We argue that the aerosol precursor gases should be exposed to oxidants of its era to get a more correct representation of secondary aerosol formation. Our model simulations show that the total aerosol indirect effect changes from −1.32 to −1.07 W m−2 when the precursor gases in the preindustrial simulation are exposed to preindustrial instead of present-day oxidants. This happens because of a brightening of the clouds in the preindustrial simulation, mainly due to large changes in the nitrate radical (NO3). The weaker oxidative power of the preindustrial atmosphere extends the lifetime of the precursor gases, enabling them to be transported higher up in the atmosphere and towards more remote areas where the susceptibility of the cloud albedo to aerosol changes is high. The oxidation changes also shift the importance of different chemical reactions and produce more condensate, thus increasing the size of the aerosols and making it easier for them to activate as cloud condensation nuclei.

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Section: Reaction Reactionsupporting

confidence: 82%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Strong impacts on aerosol indirect effects from historical oxidant changes

Karset,

Berntsen,

Storelvmo

et al. 2018

Atmos. Chem. Phys.

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“…Biomass burning emissions of CH 4 , CO, SO 2 , NO x , and nonmethane VOCs (Table S4) have been scaled by using global scaling factors from the Edgar‐Hyde emissions database [ van Aardenne et al , ]. More details about the preindustrial scenario can be found in Khan et al []. All simulations were run with meteorology from 1998 for a period of 24 months with the initial 12 months being discarded as a spin‐up year.…”

Section: Model Descriptionmentioning

confidence: 99%

A modeling study of secondary organic aerosol formation from sesquiterpenes using the STOCHEM global chemistry and transport model

et al. 2017

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Sesquiterpenes are one of the precursors of secondary organic aerosol (SOA) which can be an important global sources of organic aerosol (OA). Updating the chemistry scheme in the global chemistry transport model by incorporating an oxidation mechanism for β‐caryophyllene (representing all sesquiterpenes), adding global sesquiterpene emissions of 29 Tg/yr, and revising global monoterpene emissions up to 162 Tg/yr [Guenther et al., 2012] led to an increase of SOA burden by 95% and SOA production rate by 106% relative to the base case described in Utembe et al. [2011]. Including the emissions of sesquiterpenes resulted in increase of SOA burden of 0.11 Tg and SOA production rate of 12.9 Tg/yr relative to the base case. The highest concentrations of sesquiterpene‐derived SOA (by up to 1.2 μg/m3) were found over central Africa and South America, the regions having high levels of biogenic emissions with significant biomass burning. In the updated model simulation, the multigeneration oxidation products from sesquiterpenes and monoterpenes transported above the boundary layer and condensed to the aerosol phase at higher altitude led to an increase of OA by up to 30% over the tropics and northern midlatitude to higher altitude. The model evaluation showed an underestimation of model OA mostly for the campaigns dominated by regional anthropogenic pollution. The increase of SOA production from sesquiterpenes reduced the discrepancies between modeled and observed OA concentrations over the remote and rural areas. The increase of SOA concentrations by up to 200% from preindustrial to present scenarios was found over the tropical oceans.

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“…Two further experiments (referred to as 'B1800' and 'ISOP1800') were performed for a preindustrial scenario described in Khan et al [71]. All simulations were conducted with meteorology from 1998 for a period of 24 months with the first 12 allowing the model to spin up.…”

Section: Model Descriptionmentioning

confidence: 99%

Global Budget and Distribution of Peroxyacetyl Nitrate (PAN) for Present and Preindustrial Scenarios

Khan¹,

Cooke²,

Utembe³

et al. 2017

Int J Earth Environ Sci

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A global 3-D chemistry and transport model, STOCHEM integrated with a detailed VOC oxidation scheme (CRI v2-R5) has been employed to study the important NO x reservoir compound, peroxyacetyl nitrate (PAN). Globally, PAN is produced entirely by the reaction of acetyl peroxy radicals (CH 3 CO 3 ) with NO 2 and up to 2.0 ppb of PAN is found over the polluted regions of North America during JuneJuly-August for the present scenario. The imbalances between model and measurement data are noted, with STOCHEM-CRI overestimating PAN mixing ratios relative to the measurement data by +17 and +80 pptv for the lower and upper troposphere, respectively. The inclusion of additional HO x recycling mechanisms (e.g. related to isoprene oxidation) in STOCHEM-CRI causes a decrease in PAN in a present scenario by as much as 40% over sink regions and reduces the model-measurement disagreement by 90% for the lower troposphere and 40% for the upper troposphere. The lower NO x emissions and CH 3 CO 3 formation upon including HO x recycling in a preindustrial scenario led to a decrease in PAN formation by as much as 40%. The decrease in PAN formation results in less nitrogen being transported to remote regions which in turn leads to the greatest percentage change in O 3 concentration (9% decrease) in the equatorial regions.

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Global modeling of the nitrate radical (NO3) for present and pre-industrial scenarios

Cited by 44 publications

References 90 publications

Strong impacts on aerosol indirect effects from historical oxidant changes

Strong impacts on aerosol indirect effects from historical oxidant changes

A modeling study of secondary organic aerosol formation from sesquiterpenes using the STOCHEM global chemistry and transport model

Global Budget and Distribution of Peroxyacetyl Nitrate (PAN) for Present and Preindustrial Scenarios

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