scholarly journals Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC<sup>4</sup>RS) and ground-based (SOAS) observations in the Southeast US

2016 ◽  
Author(s):  
J. A. Fisher ◽  
D. J. Jacob ◽  
K. R. Travis ◽  
P. S. Kim ◽  
E. A. Marais ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Transport Model ◽  
Oxidation Mechanism ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Nox Emissions ◽  
Particle Phase ◽  
Chemical Transport Model ◽  
Southeast Us

Abstract. Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with ∼ 25 × 25 km2 resolution over North America. We evaluate the model using aircraft (SEAC4RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25–50 % of observed RONO2 in surface air, and we find that another 10 % is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10 % of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60 % of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20 % by photolysis to recycle NOx and 15 % by dry deposition. RONO2 production accounts for 20 % of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline.

scholarly journals Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC<sup>4</sup>RS) and ground-based (SOAS) observations in the Southeast US

2016 ◽  
Vol 16 (9) ◽  
pp. 5969-5991 ◽  
Author(s):  
Jenny A. Fisher ◽  
Daniel J. Jacob ◽  
Katherine R. Travis ◽  
Patrick S. Kim ◽  
Eloise A. Marais ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Transport Model ◽  
Oxidation Mechanism ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Nox Emissions ◽  
Particle Phase ◽  
Chemical Transport Model ◽  
Southeast Us

Abstract. Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with  ∼  25  ×  25 km2 resolution over North America. We evaluate the model using aircraft (SEAC4RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25–50 % of observed RONO2 in surface air, and we find that another 10 % is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10 % of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60 % of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20 % by photolysis to recycle NOx and 15 % by dry deposition. RONO2 production accounts for 20 % of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline.

scholarly journals Effect of changing NO<sub><i>x</i></sub> lifetime on the seasonality and long-term trends of satellite-observed tropospheric NO<sub>2</sub> columns over China

2019 ◽  
Author(s):  
Viral Shah ◽  
Daniel J. Jacob ◽  
Ke Li ◽  
Rachel F. Silvern ◽  
Shixian Zhai ◽  
...  
Keyword(s):  
Transport Model ◽  
Eastern China ◽  
Anthropogenic Emissions ◽  
Organic Nitrates ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Volatile Organic ◽  
Tropospheric No2 ◽  
Long Term Trends

Abstract. Satellite observations of tropospheric NO2 columns are extensively used to infer trends in anthropogenic emissions of nitrogen oxides (NOx ≡ NO + NO2), but this may be complicated by trends in NOx lifetime. Here we use 2004–2018 observations from the OMI satellite-based instrument (QA4ECV and POMINO v2 retrievals) to examine the seasonality and trends of tropospheric NO2 columns over central-eastern China, and we interpret the results with the GEOS-Chem chemical transport model. The observations show a factor of 3 increase in NO2 columns from summer to winter, which we explain in GEOS-Chem as reflecting a longer NOx lifetime in winter than in summer (21 h versus 5.9 h in 2017). The 2005–2018 summer trends of OMI NO2 closely follow the trends in the Multi-resolution Emission Inventory for China (MEIC), with a rise over the 2005–2011 period and a 25 % decrease since. We find in GEOS-Chem no significant trend of the NOx lifetime in summer, supporting the emission trend reported by MEIC. The winter trend of OMI NO2 is steeper than in summer over the entire period, which we attribute to a decrease in NOx lifetime at lower NOx emissions. Half of the NOx sink in winter is from N2O5 hydrolysis, which counterintuitively becomes more efficient as NOx emissions decrease due to less titration of ozone at night. Formation of organic nitrates also becomes an increasing sink of NOx as NOx emissions decrease but emissions of volatile organic compounds (VOCs) do not.

scholarly journals The effect of particle acidity on secondary organic aerosol formation from <i>α</i>-pinene photooxidation under atmospherically relevant conditions

2016 ◽  
Vol 16 (21) ◽  
pp. 13929-13944 ◽  
Author(s):  
Yuemei Han ◽  
Craig A. Stroud ◽  
John Liggio ◽  
Shao-Meng Li
Keyword(s):  
Gas Phase ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Strong Increase ◽  
Nitrate Content ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Particle Phase ◽  
Aerosol Formation

Abstract. Secondary organic aerosol (SOA) formation from photooxidation of α-pinene has been investigated in a photochemical reaction chamber under varied inorganic seed particle acidity levels at moderate relative humidity. The effect of particle acidity on SOA yield and chemical composition was examined under high- and low-NOx conditions. The SOA yield (4.2–7.6 %) increased nearly linearly with the increase in particle acidity under high-NOx conditions. In contrast, the SOA yield (28.6–36.3 %) was substantially higher under low-NOx conditions, but its dependency on particle acidity was insignificant. A relatively strong increase in SOA yield (up to 220 %) was observed in the first hour of α-pinene photooxidation under high-NOx conditions, suggesting that SOA formation was more effective for early α-pinene oxidation products in the presence of fresh acidic particles. The SOA yield decreased gradually with the increase in organic mass in the initial stage (approximately 0–1 h) under high-NOx conditions, which is likely due to the inaccessibility to the acidity over time with the coating of α-pinene SOA, assuming a slow particle-phase diffusion of organic molecules into the inorganic seeds. The formation of later-generation SOA was enhanced by particle acidity even under low-NOx conditions when introducing acidic seed particles after α-pinene photooxidation, suggesting a different acidity effect exists for α-pinene SOA derived from later oxidation stages. This effect could be important in the atmosphere under conditions where α-pinene oxidation products in the gas-phase originating in forested areas (with low NOx and SOx) are transported to regions abundant in acidic aerosols such as power plant plumes or urban regions. The fraction of oxygen-containing organic fragments (CxHyO1+ 33–35 % and CxHyO2+ 16–17 %) in the total organics and the O ∕ C ratio (0.52–0.56) of α-pinene SOA were lower under high-NOx conditions than those under low-NOx conditions (39–40, 17–19, and 0.61–0.64 %), suggesting that α-pinene SOA was less oxygenated in the studied high-NOx conditions. The fraction of nitrogen-containing organic fragments (CxHyNz+ and CxHyOzNp+) in the total organics was enhanced with the increases in particle acidity under high-NOx conditions, indicating that organic nitrates may be formed heterogeneously through a mechanism catalyzed by particle acidity or that acidic conditions facilitate the partitioning of gas-phase organic nitrates into particle phase. The results of this study suggest that inorganic acidity has a significant role to play in determining various organic aerosol chemical properties such as mass yields, oxidation state, and organic nitrate content. The acidity effect being further dependent on the timescale of SOA formation is also an important parameter in the modeling of SOA.

scholarly journals On the role of monoterpene chemistry in the remote continental boundary layer

2013 ◽  
Vol 13 (8) ◽  
pp. 22297-22335
Author(s):  
E. C. Browne ◽  
P. J. Wooldridge ◽  
K.-E. Min ◽  
R. C. Cohen
Keyword(s):  
Boreal Forest ◽  
Transport Model ◽  
Ozone Production ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Chemical Transport Model ◽  
Gas Phase Chemistry ◽  
Rural Environments ◽  
Phase Chemistry

Abstract. The formation of organic nitrates (RONO2) represents an important NOx (NOx = NO + NO2) sink in remote and rural continental atmosphere thus impacting ozone production and secondary organic aerosol (SOA) formation. In these remote and rural environments, the organic nitrates are primarily derived from biogenic volatile organic compounds (BVOCs) such as isoprene and monoterpenes. Although there are numerous studies investigating the formation of SOA from monoterpenes, there are few studies investigating monoterpene gas phase chemistry. Using a regional chemical transport model with an extended representation of organic nitrate chemistry we investigate the processes controlling the production and fate of monoterpene nitrates (MTNs) over the boreal forest of Canada. MTNs account for 5–12% of total oxidized nitrogen over the boreal forest and production via NO3 chemistry is more important than production via OH when the NOx mixing ratio is greater than 75 pptv. The regional responses are investigated for two oxidation pathways of MTNs: one that returns NOx to the atmosphere and one that converts MTNs to a nitrate that behaves like HNO3. The likely situation is in between and these two assumptions bracket the uncertainty about this chemistry. In the case where the MTNs return NOx after oxidation, their formation represents a net chemical NOx loss that exceeds the net loss to peroxy nitrate formation. When oxidation of MTNs produces a molecule that behaves like HNO3, HNO3 and MTNs are nearly equal chemical sinks for NOx. This uncertainty in the oxidative fate of MTNs results in changes in NOx of 8–14%, in O3 of up to 3%, and in OH of 3–6% between the two model simulations.

scholarly journals Effect of changing NO<sub><i>x</i></sub> lifetime on the seasonality and long-term trends of satellite-observed tropospheric NO<sub>2</sub> columns over China

2020 ◽  
Vol 20 (3) ◽  
pp. 1483-1495 ◽  
Author(s):  
Viral Shah ◽  
Daniel J. Jacob ◽  
Ke Li ◽  
Rachel F. Silvern ◽  
Shixian Zhai ◽  
...  
Keyword(s):  
Transport Model ◽  
Eastern China ◽  
Organic Nitrates ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Volatile Organic ◽  
Tropospheric No2 ◽  
Long Term Trends

Abstract. Satellite observations of tropospheric NO2 columns are extensively used to infer trends in anthropogenic emissions of nitrogen oxides (NOx≡NO+NO2), but this may be complicated by trends in NOx lifetime. Here we use 2004–2018 observations from the Ozone Monitoring Instrument (OMI) satellite-based instrument (QA4ECV and POMINO v2 retrievals) to examine the seasonality and trends of tropospheric NO2 columns over central–eastern China, and we interpret the results with the GEOS-Chem chemical transport model. The observations show a factor of 3 increase in NO2 columns from summer to winter, which we explain in GEOS-Chem as reflecting a longer NOx lifetime in winter than in summer (21 h versus 5.9 h in 2017). The 2005–2018 summer trends of OMI NO2 closely follow the trends in the Multi-resolution Emission Inventory for China (MEIC), with a rise over the 2005–2011 period and a 25 % decrease since. We find in GEOS-Chem no significant trend of the NOx lifetime in summer, supporting the emission trend reported by the MEIC. The winter trend of OMI NO2 is steeper than in summer over the entire period, which we attribute to a decrease in NOx lifetime at lower NOx emissions. Half of the NOx sink in winter is from N2O5 hydrolysis, which counterintuitively becomes more efficient as NOx emissions decrease due to less titration of ozone at night. The formation of organic nitrates also becomes an increasing sink of NOx as NOx emissions decrease but emissions of volatile organic compounds (VOCs) do not.

scholarly journals The acid-catalyzed hydrolysis of an <i>α</i>-pinene-derived organic nitrate: kinetics, products, reaction mechanisms, and atmospheric impact

2016 ◽  
Vol 16 (23) ◽  
pp. 15425-15432 ◽  
Author(s):  
Joel D. Rindelaub ◽  
Carlos H. Borca ◽  
Matthew A. Hostetler ◽  
Jonathan H. Slade ◽  
Mark A. Lipton ◽  
...  
Keyword(s):  
Gas Phase ◽  
Rate Constants ◽  
Reaction Mechanisms ◽  
Tropospheric Ozone ◽  
Organic Aerosol ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Particle Phase ◽  
Fine Aerosol ◽  
Acid Catalyzed

Abstract. The production of atmospheric organic nitrates (RONO2) has a large impact on air quality and climate due to their contribution to secondary organic aerosol and influence on tropospheric ozone concentrations. Since organic nitrates control the fate of gas phase NOx (NO + NO2), a byproduct of anthropogenic combustion processes, their atmospheric production and reactivity is of great interest. While the atmospheric reactivity of many relevant organic nitrates is still uncertain, one significant reactive pathway, condensed phase hydrolysis, has recently been identified as a potential sink for organic nitrate species. The partitioning of gas phase organic nitrates to aerosol particles and subsequent hydrolysis likely removes the oxidized nitrogen from further atmospheric processing, due to large organic nitrate uptake to aerosols and proposed hydrolysis lifetimes, which may impact long-range transport of NOx, a tropospheric ozone precursor. Despite the atmospheric importance, the hydrolysis rates and reaction mechanisms for atmospherically derived organic nitrates are almost completely unknown, including those derived from α-pinene, a biogenic volatile organic compound (BVOC) that is one of the most significant precursors to biogenic secondary organic aerosol (BSOA). To better understand the chemistry that governs the fate of particle phase organic nitrates, the hydrolysis mechanism and rate constants were elucidated for several organic nitrates, including an α-pinene-derived organic nitrate (APN). A positive trend in hydrolysis rate constants was observed with increasing solution acidity for all organic nitrates studied, with the tertiary APN lifetime ranging from 8.3 min at acidic pH (0.25) to 8.8 h at neutral pH (6.9). Since ambient fine aerosol pH values are observed to be acidic, the reported lifetimes, which are much shorter than that of atmospheric fine aerosol, provide important insight into the fate of particle phase organic nitrates. Along with rate constant data, product identification confirms that a unimolecular specific acid-catalyzed mechanism is responsible for organic nitrate hydrolysis under acidic conditions. The free energies and enthalpies of the isobutyl nitrate hydrolysis intermediates and products were calculated using a hybrid density functional (ωB97X-V) to support the proposed mechanisms. These findings provide valuable information regarding the organic nitrate hydrolysis mechanism and its contribution to the fate of atmospheric NOx, aerosol phase processing, and BSOA composition.

scholarly journals On the role of monoterpene chemistry in the remote continental boundary layer

2014 ◽  
Vol 14 (3) ◽  
pp. 1225-1238 ◽  
Author(s):  
E. C. Browne ◽  
P. J. Wooldridge ◽  
K.-E. Min ◽  
R. C. Cohen
Keyword(s):  
Boreal Forest ◽  
Transport Model ◽  
Ozone Production ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Chemical Transport Model ◽  
Gas Phase Chemistry ◽  
Rural Environments ◽  
Phase Chemistry

Abstract. The formation of organic nitrates (RONO2) represents an important NOx (NOx = NO + NO2) sink in the remote and rural continental atmosphere, thus impacting ozone production and secondary organic aerosol (SOA) formation. In these remote and rural environments, the organic nitrates are primarily derived from biogenic volatile organic compounds (BVOCs) such as isoprene and monoterpenes. Although there are numerous studies investigating the formation of SOA from monoterpenes, there are few studies investigating monoterpene gas-phase chemistry. Using a regional chemical transport model with an extended representation of organic nitrate chemistry, we investigate the processes controlling the production and fate of monoterpene nitrates (MTNs) over the boreal forest of Canada. MTNs account for 5–12% of total oxidized nitrogen over the boreal forest, and production via NO3 chemistry is more important than production via OH when the NOx mixing ratio is greater than 75 pptv. The regional responses are investigated for two oxidation pathways of MTNs: one that returns NOx to the atmosphere and one that converts MTNs into a nitrate that behaves like HNO3. The likely situation is in between, and these two assumptions bracket the uncertainty about this chemistry. In the case where the MTNs return NOx after oxidation, their formation represents a net chemical NOx loss that exceeds the net loss to peroxy nitrate formation. When oxidation of MTNs produces a molecule that behaves like HNO3, HNO3 and MTNs are nearly equal chemical sinks for NOx. This uncertainty in the oxidative fate of MTNs results in changes in NOx of 8–14%, in O3 of up to 3%, and in OH of 3–6% between the two model simulations.

scholarly journals The Acid-Catalyzed Hydrolysis of an α-Pinene-Derived Organic Nitrate: Kinetics, Products, Reaction Mechanisms, and Atmospheric Impact

2016 ◽  
Author(s):  
Joel D. Rindelaub ◽  
Carlos H. Borca ◽  
Matthew A. Hostetler ◽  
Mark A. Lipton ◽  
Lyudmila V. Slipchenko ◽  
...  
Keyword(s):  
Gas Phase ◽  
Reaction Mechanisms ◽  
Tropospheric Ozone ◽  
Organic Aerosol ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Particle Phase ◽  
Fine Aerosol ◽  
Acid Catalyzed ◽  
Insight Into

Abstract. The production of atmospheric organic nitrates (RONO2) has a large impact on air quality and climate, due to their contribution to secondary organic aerosol and influence on tropospheric ozone concentrations. Since organic nitrates control the fate of gas phase NOx (NO+NO2), a byproduct of anthropogenic combustion processes, their atmospheric production and reactivity is of great interest. While the atmospheric reactivity of many relevant organic nitrates is still very uncertain, one significant reactive pathway, condensed phase hydrolysis, has recently been identified as a potential sink for organic nitrate species. The partitioning of gas phase organic nitrates to aerosol particles and subsequent hydrolysis likely removes the oxidized nitrogen from further atmospheric processing, due to large organic nitrate uptake to aerosols and proposed hydrolysis lifetimes, which may impact long range transport of NOx, a tropospheric ozone precursor. Despite the atmospheric importance, the hydrolysis rates and reaction mechanisms for atmospherically-derived organic nitrates are almost completely unknown, including those derived from α-pinene, a biogenic volatile organic compound (BVOC) that is one of the most significant precursors to biogenic secondary organic aerosol (BSOA). To better understand the chemistry that governs the fate of particle phase organic nitrates, this study elucidated the hydrolysis mechanism and rate constants for several organic nitrates, including an α-pinene-derived organic nitrate (APN). A positive trend in hydrolysis rate constants was observed with increasing solution acidity for all organic nitrates studied, with the APN lifetime ranging from 8.3 minutes at acidic pH (0.25) to 8.8 hours at neutral pH (6.9). Since ambient fine aerosol pH values are observed to be acidic, the reported lifetimes, which are much shorter than that of atmospheric fine aerosol, provide important insight into the fate of particle phase organic nitrates. Along with rate constant data, the identification of the products campholenic aldehyde, pinol, and pinocamphone confirms a unimolecular specific acid-catalyzed mechanism is responsible for organic nitrate hydrolysis under acidic conditions, where carbocation rearrangement is favored for α-pinene-derived species. The free energies and enthalpies of the isobutyl nitrate hydrolysis intermediates and products were calculated using a hybrid density functional (ωB97X-V) to support the proposed mechanisms. These findings provide valuable insight into the organic nitrate hydrolysis mechanism and its contribution to the fate of atmospheric NOx, aerosol phase processing, and BSOA composition.

scholarly journals A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

2005 ◽  
Vol 5 (8) ◽  
pp. 2227-2252 ◽  
Author(s):  
D. V. Spracklen ◽  
K. J. Pringle ◽  
K. S. Carslaw ◽  
M. P. Chipperfield ◽  
G. W. Mann
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
Size Distribution ◽  
Marine Boundary Layer ◽  
Transport Model ◽  
Model Development ◽  
Aerosol Size Distribution ◽  
Chemical Transport Model ◽  
Cloud Processing ◽  
Nucleation Mechanisms

Abstract. A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN>3nm) vary between about 250–500 cm-3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acid-water particles. Remote marine CN concentrations increase to around 2000–10 000 cm

scholarly journals Observing atmospheric formaldehyde (HCHO) from space: validation and intercomparison of six retrievals from four satellites (OMI, GOME2A, GOME2B, OMPS) with SEAC<sup>4</sup>RS aircraft observations over the Southeast US

2016 ◽  
Author(s):  
Lei Zhu ◽  
Daniel J. Jacob ◽  
Patrick S. Kim ◽  
Jenny A. Fisher ◽  
Karen Yu ◽  
...  
Keyword(s):  
Transport Model ◽  
Research Groups ◽  
Chemical Transport Model ◽  
Shape Factors ◽  
Aircraft Observations ◽  
Volatile Organic ◽  
Satellite Retrievals ◽  
Mass Factor ◽  
The Mean ◽  
Southeast Us

Abstract. Formaldehyde (HCHO) column data from satellites are widely used as a proxy for emissions of volatile organic compounds (VOCs), but validation of the data has been extremely limited. Here we use highly accurate HCHO aircraft observations from the NASA SEAC4RS campaign over the Southeast US in August–September 2013 to validate and intercompare six operational and research retrievals of HCHO columns from four different satellite instruments (OMI, GOME2A, GOME2B and OMPS) and three different research groups. The GEOS-Chem chemical transport model provides a common intercomparison platform. We find that all retrievals capture the HCHO maximum over Arkansas and Louisiana, reflecting high emissions of biogenic isoprene, and are consistent in their spatial variability over the Southeast US (r = 0.4–0.8 on a 0.5° × 0.5° grid) as well as their day-to-day variability (r = 0.5–0.8). However, all satellite retrievals are biased low in the mean by 20–51 %, which would lead to corresponding bias in estimates of isoprene emissions from the satellite data. The smallest bias is for OMI-BIRA, which has the highest corrected slant columns and the lowest scattering weights in its air mass factor (AMF) calculation. Correcting the assumed HCHO vertical profiles (shape factors) used in the AMF calculation would further reduce the bias in the OMI-BIRA data. We conclude that current satellite HCHO data provide a reliable proxy for isoprene emission variability but with a low mean bias due both to the corrected slant columns and the scattering weights used in the retrievals.

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