scholarly journals Modelling study of the impact of deep convection on the UTLS air composition – Part I: Analysis of ozone precursors

2005 ◽  
Vol 5 (5) ◽  
pp. 9127-9168 ◽  
Author(s):  
V. Marécal ◽  
E. D. Rivière ◽  
G. Held ◽  
S. Cautenet ◽  
S. Freitas

Abstract. The aim of this work is to study the local impact of deep convection on the upper troposphere/lower stratosphere air composition. For this purpose, we performed a 42-h simulation of a severe convective event near Bauru, in the central State of São Paulo (Brazil), with the 3-D mesoscale model RAMS coupled on-line with a chemistry model. The meteorological results of the simulation are evaluated using comparisons with near surface measurements of wind and temperature and with surface rainfall rates derived from radar observations. These comparisons show that the model produces meteorological fields consistent with the observations. This present paper (Part I) is devoted to the analysis of the ozone precursors in the upper troposphere/lower stratosphere: CO, NOx (=NO+NO2) and non-methane volatile organic compounds. The simulation results show that the distribution of CO with altitude is closely related to the upward convective motions and consecutive outflow at the top of the convective cells leading to a bulge of CO between 7 km altitude and the cold point tropopause (around 17km altitude). The model results for CO are consistent with satellite-borne measurements in the 700–500 hPa layer. The simulation also indicates enhanced amounts of NOx up to 2 ppbv in the 7–17 km altitude layer. These NOx concentrations are mainly produced by the lightning associated with the intense convective activity. Stratospheric NOx are not affected by the tropospheric NOx since there is, on average, no significant upward NOx flux through the tropopause. For non-methane volatile organic compounds, the convective activity tends to significantly increase the amount of ozone precursors in the 7–17 km layer by dynamical effects as for CO. During daytime, this bulge is largely reduced in the upper part of the layer for reactive species, such as isoprene, ethene and propene, since they undergo chemical loss. This loss is mainly due to their reactions with OH, OH mixing ratio being significantly increased during the daytime by the production of NOx by lightning. The bulges of ozone precursors in the upper troposphere are likely to be of importance in the ozone budget in the upper troposphere and lower stratosphere. This issue is discussed in Part II of this series of papers.

2006 ◽  
Vol 6 (6) ◽  
pp. 1567-1584 ◽  
Author(s):  
V. Marécal ◽  
E. D. Rivière ◽  
G. Held ◽  
S. Cautenet ◽  
S. Freitas

Abstract. The aim of this work is to study the local impact on the upper troposphere/lower stratosphere air composition of an extreme deep convective system. For this purpose, we performed a simulation of a convective cluster composed of many individual deep convective cells that occurred near Bauru (Brazil). The simulation is performed using the 3-D mesoscale model RAMS coupled on-line with a chemistry model. The comparisons with meteorological measurements show that the model produces meteorological fields generally consistent with the observations. The present paper (part I) is devoted to the analysis of the ozone precursors (CO, NOx and non-methane volatile organic compounds) and HOx in the UTLS. The simulation results show that the distribution of CO with altitude is closely related to the upward convective motions and consecutive outflow at the top of the convective cells leading to a bulge of CO between 7 km altitude and the tropopause (around 17 km altitude). The model results for CO are consistent with satellite-borne measurements at 700 hPa. The simulation also indicates enhanced amounts of NOx up to 2 ppbv in the 7–17 km altitude layer mainly produced by the lightning associated with the intense convective activity. For insoluble non-methane volatile organic compounds, the convective activity tends to significantly increase their amount in the 7–17 km layer by dynamical effects. During daytime in the presence of lightning NOx, this bulge is largely reduced in the upper part of the layer for reactive species (e.g. isoprene, ethene) because of their reactions with OH that is increased on average during daytime. Lightning NOx also impacts on the oxydizing capacity of the upper troposphere by reducing on average HOx, HO2, H2O2 and organic hydroperoxides. During the simulation time, the impact of convection on the air composition of the lower stratosphere is negligible for all ozone precursors although several of the simulated convective cells nearly reach the tropopause. There is no significant transport from the upper troposphere to the lower stratosphere, the isentropic barrier not being crossed by convection. The impact of the increase of ozone precursors and HOx in the upper troposphere on the ozone budget in the LS is discussed in part II of this series of papers.


2016 ◽  
Vol 9 (5) ◽  
pp. 1959-1976 ◽  
Author(s):  
Chun Zhao ◽  
Maoyi Huang ◽  
Jerome D. Fast ◽  
Larry K. Berg ◽  
Yun Qian ◽  
...  

Abstract. Current climate models still have large uncertainties in estimating biogenic trace gases, which can significantly affect atmospheric chemistry and secondary aerosol formation that ultimately influences air quality and aerosol radiative forcing. These uncertainties result from many factors, including uncertainties in land surface processes and specification of vegetation types, both of which can affect the simulated near-surface fluxes of biogenic volatile organic compounds (BVOCs). In this study, the latest version of Model of Emissions of Gases and Aerosols from Nature (MEGAN v2.1) is coupled within the land surface scheme CLM4 (Community Land Model version 4.0) in the Weather Research and Forecasting model with chemistry (WRF-Chem). In this implementation, MEGAN v2.1 shares a consistent vegetation map with CLM4 for estimating BVOC emissions. This is unlike MEGAN v2.0 in the public version of WRF-Chem that uses a stand-alone vegetation map that differs from what is used by land surface schemes. This improved modeling framework is used to investigate the impact of two land surface schemes, CLM4 and Noah, on BVOCs and examine the sensitivity of BVOCs to vegetation distributions in California. The measurements collected during the Carbonaceous Aerosol and Radiative Effects Study (CARES) and the California Nexus of Air Quality and Climate Experiment (CalNex) conducted in June of 2010 provided an opportunity to evaluate the simulated BVOCs. Sensitivity experiments show that land surface schemes do influence the simulated BVOCs, but the impact is much smaller than that of vegetation distributions. This study indicates that more effort is needed to obtain the most appropriate and accurate land cover data sets for climate and air quality models in terms of simulating BVOCs, oxidant chemistry and, consequently, secondary organic aerosol formation.


2010 ◽  
Vol 10 (21) ◽  
pp. 10321-10334 ◽  
Author(s):  
J. Bechara ◽  
A. Borbon ◽  
C. Jambert ◽  
A. Colomb ◽  
P. E. Perros

Abstract. A large dataset of reactive trace gases was collected for the first time over West Africa during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment in August 2006. Volatile Organic Compounds (VOC from C5–C9) were measured onboard the two French aircrafts the ATR-42 and the Falcon-20 by a new instrument AMOVOC (Airborne Measurement Of Volatile Organic Compounds). The goal of this study is (i) to characterize VOC distribution in the tropical region of West Africa (ii) to determine the impact of deep convection on VOC distribution and chemistry in the tropical upper troposphere (UT) and (iii) to characterize its spatial and temporal extensions. Experimental strategy consisted in sampling at altitudes between 0 and 12 km downwind of Mesoscale Convective Systems (MCS) and at cloud base. Biogenic and anthropogenic VOC distribution in West Africa is clearly affected by North to South emission gradient. Isoprene, the most abundant VOC, is at maximum level over the forest (1.26 ppb) while benzene reaches its maximum over the urban areas (0.11 ppb). First, a multiple physical and chemical tracers approach using CO, O3 and relative humidity was implemented to distinguish between convective and non-convective air masses. Then, additional tools based on VOC observations (tracer ratios, proxy of emissions and photochemical clocks) were adapted to characterize deep convection on a chemical, spatial and temporal basis. VOC vertical profiles show a "C-shaped" trend indicating that VOC-rich air masses are transported from the surface to the UT by deep convective systems. VOC mixing ratios in convective outflow are up to two times higher than background levels even for reactive and short-lived VOC (e.g. isoprene up to 0.19 ppb at 12 km-altitude) and are dependent on surface emission type. As a consequence, UT air mass reactivity increases from 0.52 s−1 in non-convective conditions to 0.95 s−1 in convective conditions. Fractions of boundary layer air contained in convective outflow are estimated to be 40 ± 15%. Vertical transport timescale is calculated to be 25 ± 10 min between 0 to 12 km altitude. These results characterize deep convection occurring over West Africa and provide relevant information for tropical convection parameterization in regional/global models.


2009 ◽  
Vol 9 (5) ◽  
pp. 20309-20346 ◽  
Author(s):  
J. Bechara ◽  
A. Borbon ◽  
C. Jambert ◽  
A. Colomb ◽  
P. E. Perros

Abstract. A large dataset of reactive trace gases was collected for the first time over West Africa during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment in August 2006. Volatile Organic Compounds (VOC from C5–C9) were measured onboard the two French aircrafts the ATR-42 and the Falcon-20 by a new instrument AMOVOC. The goal of this study is (i) to characterize VOC distribution in the tropical region of West Africa (ii) to determine the impact of deep convection on VOC distribution and chemistry in the tropical upper troposphere (UT) and (iii) to characterize its spatial and temporal extensions. Experimental strategy consisted in sampling at altitudes between 0 and 12 km downwind of Mesoscale Convective Systems (MCS) and at cloud base. Biogenic and anthropogenic VOC distribution in West Africa is clearly affected by North to South emission gradient. Isoprene, the most abundant VOC, is at maximum level over the forest (1.26 ppb) while benzene reaches its maximum over the urban areas (0.11 ppb). First, a multiple physical and chemical tracers approach using CO, O3 and relative humidity was implemented to distinguish between convective and non-convective air masses. Then, additional tools based on VOC observations (tracer ratios, proxy of emissions and photochemical clocks) were adapted to characterize deep convection on a chemical, spatial and temporal basis. VOC vertical profiles show a "C-shaped" trend indicating that VOC-rich air masses are transported from the surface to the UT by deep convective systems. VOC mixing ratios in convective outflow are up to two times higher than background levels even for reactive and short-lived VOC (e.g. isoprene up to 0.19 ppb at 12 km-altitude) and are dependent on surface emission type. As a consequence, UT air mass reactivity increases from 0.52 s−1 in non-convective conditions to 0.95 s−1 in convective conditions. Fractions of boundary layer air contained in convective outflow are estimated to be 40±15%. Vertical transport timescale is calculated to be 25±10 min. These results characterize deep convection occurring over West Africa and provide relevant information for tropical convection parameterization in regional/global models.


2011 ◽  
Vol 11 (1) ◽  
pp. 121-162 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.


2011 ◽  
Vol 11 (6) ◽  
pp. 2671-2687 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform convective detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.


2021 ◽  
Vol 13 (12) ◽  
pp. 6570
Author(s):  
Asma Akter Parlin ◽  
Monami Kondo ◽  
Noriaki Watanabe ◽  
Kengo Nakamura ◽  
Mizuki Yamada ◽  
...  

The quantitative understanding of the transport behavior of volatile organic compounds (VOCs) in near-surface soils is highly important in light of the potential impacts of soil VOC emissions on the air quality and climate. Previous studies have suggested that temperature changes affect the transport behavior; however, the effects are not well understood. Indeed, much larger changes in the VOC flux under in situ dynamic temperatures than those expected from the temperature dependence of the diffusion coefficients of VOCs in the air have been suggested but rarely investigated experimentally. Here, we present the results of a set of experiments on the upward vertical vapor-phase diffusive transport of benzene and trichloroethylene (TCE) in sandy soils with water contents ranging from an air-dried value to 10 wt% during sinusoidal temperature variation between 20 and 30 °C. In all experiments, the flux from the soil surface was correlated with the temperature, as expected. However, the changes in flux under wet conditions were unexpectedly large and increased with increasing water content; they were also larger for TCE, the volatility of which depended more strongly on the temperature. Additionally, the larger flux changes were accompanied by a recently discovered water-induced inverse correlation between temperature and flux into the overlying soil. These results demonstrated that the flux changes of VOCs under dynamic temperatures could be increased by volatilization-dissolution interactions of VOCs with water. Future extensive studies on this newly discovered phenomenon would contribute to a better understanding of the impacts of soil VOC emissions on the air quality and climate.


2018 ◽  
Vol 18 (13) ◽  
pp. 9527-9545 ◽  
Author(s):  
Qian Xiao ◽  
Mei Li ◽  
Huan Liu ◽  
Mingliang Fu ◽  
Fanyuan Deng ◽  
...  

Abstract. Emissions from ships at berth play an important role regarding the exposure of high density human populations to atmospheric pollutants in port areas; however, these emissions are not well understood. In this study, volatile organic compounds (VOCs) and particle emissions from 20 container ships at berth were sampled and analyzed during the “fuel switch” period at Jingtang Port in Hebei Province, China. VOCs and particles were analyzed using a gas chromatography-mass spectrometer (GC-MS) and a single particle aerosol mass spectrometer (SPAMS), respectively. VOC analysis showed that alkanes and aromatics, especially benzene, toluene and heavier compounds e.g., n-heptane, n-octane and n-nonane, dominated the total identified species. Secondary organic aerosol (SOA) yields and ozone (O3) forming potential were 0.017 ± 0.007 g SOA g−1 VOCs and 2.63 ± 0.37 g O3 g−1 VOCs, respectively. Both positive and negative ion mass spectra from individual ships were derived and the intensity of specific ions were quantified. Results showed that elemental carbon (35.74 %), elemental carbon–organic carbon mixtures (33.95 %) and Na-rich particles (21.12 %) were major classes, comprising 90.7 % of the particles observed. Particles from ship auxiliary engines were in the 0.2 to 2.5 µm size range, with a peak occurring at around 0.4 µm. The issue of using vanadium (V) as tracer element was examined, and it was found that V was not a proper tracer of ship emissions when using low sulfur content diesel oil. The average percentage of sulfate particles observed in shipping emissions before and after switching to marine diesel oil remained unchanged at 24 %. Under certain wind conditions, when berths were upwind of emission sources, the ratios before and after 1 January were 35 and 27 % respectively. The impact of atmospheric stability was discussed based on PM2.5 and primary pollutant (carbon monoxide) concentration. With a background of frequent haze episodes and complex mechanisms of particulate accumulation and secondary formation, the impact of atmospheric stability is believed to have been weak on the sulfate contribution from shipping emissions. The results from this study provide robust support for port area air quality assessment and source apportionment.


2010 ◽  
Vol 10 (2) ◽  
pp. 3861-3892 ◽  
Author(s):  
J. G. Murphy ◽  
D. E. Oram ◽  
C. E. Reeves

Abstract. In this paper we describe measurements of volatile organic compounds (VOCs) made using a Proton Transfer Reaction Mass Spectrometer (PTR-MS) aboard the UK Facility for Atmospheric Airborne Measurements during the African Monsoon Multidisciplinary Analyses (AMMA) campaign. Observations were made during approximately 85 h of flying time between 17 July and 17 August 2006, above an area between 4° N and 18° N and 3° W and 4° E, encompassing ocean, mosaic forest, and the Sahel desert. High time resolution observations of counts at mass to charge (m/z) ratios of 42, 59, 69, 71, and 79 were used to calculate mixing ratios of acetonitrile, acetone, isoprene, the sum of methyl vinyl ketone and methacrolein, and benzene, respectively using laboratory-derived humidity-dependent calibration factors. Strong spatial associations between vegetation and isoprene and its oxidation products were observed in the boundary layer, consistent with biogenic emissions followed by rapid atmospheric oxidation. Acetonitrile, benzene, and acetone were all enhanced in airmasses which had been heavily influenced by biomass burning. Benzene and acetone were also elevated in airmasses with urban influence from cities such as Lagos, Cotonou, and Niamey. The observations provide evidence that both deep convection and mixing associated with fair-weather cumulus were responsible for vertical redistribution of VOCs emitted from the surface. Profiles over the ocean showed a depletion of acetone in the marine boundary layer, but no significant decrease for acetonitrile.


2015 ◽  
Vol 15 (11) ◽  
pp. 6467-6486 ◽  
Author(s):  
W. Frey ◽  
R. Schofield ◽  
P. Hoor ◽  
D. Kunkel ◽  
F. Ravegnani ◽  
...  

Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 campaign in connection with a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For example, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere, but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.


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