scholarly journals Comparing three vegetation monoterpene emission models to measured gas concentrations with a model of meteorology, air chemistry and chemical transport

2013 ◽  
Vol 10 (11) ◽  
pp. 18563-18611
Author(s):  
S. Smolander ◽  
Q. He ◽  
D. Mogensen ◽  
L. Zhou ◽  
J. Bäck ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Coniferous Forest ◽  
Chemical Species ◽  
Field Measurements ◽  
Global Scale ◽  
Aerosol Formation ◽  
Seasonal And Diurnal Variations ◽  
Air Chemistry ◽  
Emission Models

Abstract. Biogenic volatile organic compounds (BVOCs) are essential in atmospheric chemistry because of their chemical reactions that produce and destroy tropospheric ozone, their effects on aerosol formation and growth, and their potential influence on global warming. As one of the important BVOC groups, monoterpenes have been a focus of scientific attention in atmospheric research. Detailed regional measurements and model estimates are needed to study emission potential and the monoterpene budget on a global scale. Since the use of empirical measurements for upscaling is limited by many physical and biological factors such as genetic variation, temperature and light, water availability, seasonal changes, and environmental stresses, comprehensive inventories over larger areas are difficult to obtain. We applied the boundary layer-chemistry-transport model SOSA to investigate Scots pine (Pinus sylvestris) monoterpene emissions in a boreal coniferous forest at the SMEAR II site, Southern Finland. SOSA was applied to simulate monoterpene emissions with three different emission modules: the semi-empirical G95, MEGAN 2.04 with improved descriptions of temperature and light responses and including also carbonyl emissions, and a process-based model SIM-BIM. For the first time, the emission models included seasonal and diurnal variations in both quantity and chemical species of emitted monoterpenes, based on parameterizations obtained from field measurements. Results indicate that modelling and observations agreed reasonably well, and that the model can be used for investigating regional air chemistry questions related to monoterpenes. The predominant modelled monoterpene concentrations, α-pinene and Δ3-carene, are consistent with observations.

scholarly journals Comparing three vegetation monoterpene emission models to measured gas concentrations with a model of meteorology, air chemistry and chemical transport

2014 ◽  
Vol 11 (19) ◽  
pp. 5425-5443 ◽  
Author(s):  
S. Smolander ◽  
Q. He ◽  
D. Mogensen ◽  
L. Zhou ◽  
J. Bäck ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Coniferous Forest ◽  
Chemical Species ◽  
Field Measurements ◽  
Global Scale ◽  
Aerosol Formation ◽  
Seasonal And Diurnal Variations ◽  
Air Chemistry ◽  
Emission Models

Abstract. Biogenic volatile organic compounds (BVOCs) are essential in atmospheric chemistry because of their chemical reactions that produce and destroy tropospheric ozone, their effects on aerosol formation and growth, and their potential influence on global warming. As one of the important BVOC groups, monoterpenes have been a focus of scientific attention in atmospheric research. Detailed regional measurements and model estimates are needed to study emission potential and the monoterpene budget on a global scale. Since the use of empirical measurements for upscaling is limited by many physical and biological factors, such as genetic variation, temperature and light, water availability, seasonal changes, and environmental stresses, comprehensive inventories over larger areas are difficult to obtain. We applied the boundary-layer–chemistry-transport model SOSA (model to Simulate the concentrations of Organic vapours and Sulphuric Acid) to investigate Scots pine (Pinus sylvestris) monoterpene emissions in a boreal coniferous forest at the SMEAR (Station for Measuring forest Ecosystem–Atmosphere Relations) II site, southern Finland. SOSA was applied to simulate monoterpene emissions with three different emission modules: the semiempirical G95, MEGAN (Model of Emissions of Gases and Aerosols from Nature) 2.04 with improved descriptions of temperature and light responses and including also carbonyl emissions, and a process-based model SIM–BIM (Seasonal Isoprenoid synthase Model – Biochemical Isoprenoid biosynthesis Model). For the first time, the emission models included seasonal and diurnal variations in both quantity and chemical species of emitted monoterpenes, based on parameterizations obtained from field measurements. Results indicate that modelling and observations agreed reasonably well and that the model can be used for investigating regional air chemistry questions related to monoterpenes. The predominant modelled monoterpene concentrations, α-pinene and Δ3-carene, are consistent with observations.

scholarly journals Seasonal variability of tropical wetland CH<sub>4</sub> emissions: the role of the methanogen-available carbon pool

2012 ◽  
Vol 9 (8) ◽  
pp. 2821-2830 ◽  
Author(s):  
A. A. Bloom ◽  
P. I. Palmer ◽  
A. Fraser ◽  
D. S. Reay
Keyword(s):  
Atmospheric Chemistry ◽  
Seasonal Variability ◽  
Transport Model ◽  
Global Scale ◽  
Plant Litter ◽  
Carbon Pool ◽  
Spatial And Temporal Variability ◽  
Ch4 Emissions ◽  
Available Carbon

Abstract. We develop a dynamic methanogen-available carbon model (DMCM) to quantify the role of the methanogen-available carbon pool in determining the spatial and temporal variability of tropical wetland CH4 emissions over seasonal timescales. We fit DMCM parameters to satellite observations of CH4 columns from SCIAMACHY CH4 and equivalent water height (EWH) from GRACE. Over the Amazon River basin we found substantial seasonal variability of this carbon pool (coefficient of variation = 28 ± 22%) and a rapid decay constant (φ = 0.017 day−1), in agreement with available laboratory measurements, suggesting that plant litter is likely the prominent methanogen carbon source over this region. Using the DMCM we derived global CH4 emissions for 2003–2009, and determined the resulting seasonal variability of atmospheric CH4 on a global scale using the GEOS-Chem atmospheric chemistry and transport model. First, we estimated that tropical emissions amounted to 111.1 Tg CH4 yr−1, of which 24% was emitted from Amazon wetlands. We estimated that annual tropical wetland emissions increased by 3.4 Tg CH4 yr−1 between 2003 and 2009. Second, we found that the model was able to reproduce the observed seasonal lag of CH4 concentrations peaking 1–3 months before peak EWH values. We also found that our estimates of CH4 emissions substantially improved the comparison between the model and observed CH4 surface concentrations (r = 0.9). We anticipate that these new insights from the DMCM represent a fundamental step in parameterising tropical wetland CH4 emissions and quantifying the seasonal variability and future trends of tropical CH4 emissions.

scholarly journals Impact of transport model errors on the global and regional methane emissions estimated by inverse modelling

2013 ◽  
Vol 13 (19) ◽  
pp. 9917-9937 ◽  
Author(s):  
R. Locatelli ◽  
P. Bousquet ◽  
F. Chevallier ◽  
A. Fortems-Cheney ◽  
S. Szopa ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Initial Conditions ◽  
Spatial Scales ◽  
Global Scale ◽  
Methane Emissions ◽  
Inverse Modelling ◽  
Model Errors ◽  
Inverse Systems ◽  
The Impact

Abstract. A modelling experiment has been conceived to assess the impact of transport model errors on methane emissions estimated in an atmospheric inversion system. Synthetic methane observations, obtained from 10 different model outputs from the international TransCom-CH4 model inter-comparison exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the three-component PYVAR-LMDZ-SACS (PYthon VARiational-Laboratoire de Météorologie Dynamique model with Zooming capability-Simplified Atmospheric Chemistry System) inversion system to produce 10 different methane emission estimates at the global scale for the year 2005. The same methane sinks, emissions and initial conditions have been applied to produce the 10 synthetic observation datasets. The same inversion set-up (statistical errors, prior emissions, inverse procedure) is then applied to derive flux estimates by inverse modelling. Consequently, only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg yr−1 at the global scale, representing 5% of total methane emissions. At continental and annual scales, transport model errors are proportionally larger than at the global scale, with errors ranging from 36 Tg yr−1 in North America to 7 Tg yr−1 in Boreal Eurasia (from 23 to 48%, respectively). At the model grid-scale, the spread of inverse estimates can reach 150% of the prior flux. Therefore, transport model errors contribute significantly to overall uncertainties in emission estimates by inverse modelling, especially when small spatial scales are examined. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher horizontal resolution in transport models. The large differences found between methane flux estimates inferred in these different configurations highly question the consistency of transport model errors in current inverse systems. Future inversions should include more accurately prescribed observation covariances matrices in order to limit the impact of transport model errors on estimated methane fluxes.

scholarly journals Rapid formation of isoprene photo-oxidation products observed in Amazonia

2009 ◽  
Vol 9 (20) ◽  
pp. 7753-7767 ◽  
Author(s):  
T. Karl ◽  
A. Guenther ◽  
A. Turnipseed ◽  
G. Tyndall ◽  
P. Artaxo ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Global Climate ◽  
Field Measurements ◽  
Oxidative Capacity ◽  
Oxidation Products ◽  
Lower Atmosphere ◽  
Peroxy Radicals ◽  
Aerosol Formation ◽  
Photo Oxidation ◽  
Voc Oxidation

Abstract. Isoprene represents the single most important reactive hydrocarbon for atmospheric chemistry in the tropical atmosphere. It plays a central role in global and regional atmospheric chemistry and possible climate feedbacks. Photo-oxidation of primary hydrocarbons (e.g. isoprene) leads to the formation of oxygenated VOCs (OVOCs). The evolution of these intermediates affects the oxidative capacity of the atmosphere (by reacting with OH) and can contribute to secondary aerosol formation, a poorly understood process. An accurate and quantitative understanding of VOC oxidation processes is needed for model simulations of regional air quality and global climate. Based on field measurements conducted during the Amazonian Aerosol Characterization Experiment (AMAZE-08) we show that the production of certain OVOCs (e.g. hydroxyacetone) from isoprene photo-oxidation in the lower atmosphere is significantly underpredicted by standard chemistry schemes. Recently reported fast secondary production could explain 50% of the observed discrepancy with the remaining part possibly produced via a novel primary production channel, which has been proposed theoretically. The observations of OVOCs are also used to test a recently proposed HOx recycling mechanism via degradation of isoprene peroxy radicals. If generalized our observations suggest that prompt photochemical formation of OVOCs and other uncertainties in VOC oxidation schemes could result in uncertainties of modelled OH reactivity, potentially explaining a fraction of the missing OH sink over forests which has previously been largely attributed to a missing source of primary biogenic VOCs.

scholarly journals A review of operational, regional-scale, chemical weather forecasting models in Europe

2012 ◽  
Vol 12 (1) ◽  
pp. 1-87 ◽  
Author(s):  
J. Kukkonen ◽  
T. Olsson ◽  
D. M. Schultz ◽  
A. Baklanov ◽  
T. Klein ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Weather Forecasting ◽  
Numerical Models ◽  
Weather Prediction ◽  
Regional Scale ◽  
Chemical Species ◽  
Future Research ◽  
Physical Processes ◽  
Forecasting Models ◽  
Air Chemistry

Abstract. Numerical models that combine weather forecasting and atmospheric chemistry are here referred to as chemical weather forecasting models. Eighteen operational chemical weather forecasting models on regional and continental scales in Europe are described and compared in this article. Topics discussed in this article include how weather forecasting and atmospheric chemistry models are integrated into chemical weather forecasting systems, how physical processes are incorporated into the models through parameterization schemes, how the model architecture affects the predicted variables, and how air chemistry and aerosol processes are formulated. In addition, we discuss sensitivity analysis and evaluation of the models, user operational requirements, such as model availability and documentation, and output availability and dissemination. In this manner, this article allows for the evaluation of the relative strengths and weaknesses of the various modelling systems and modelling approaches. Finally, this article highlights the most prominent gaps of knowledge for chemical weather forecasting models and suggests potential priorities for future research directions, for the following selected focus areas: emission inventories, the integration of numerical weather prediction and atmospheric chemical transport models, boundary conditions and nesting of models, data assimilation of the various chemical species, improved understanding and parameterization of physical processes, better evaluation of models against data and the construction of model ensembles.

scholarly journals Current estimates of biogenic emissions from Eucalypts uncertain for Southeast Australia

2016 ◽  
Author(s):  
K. M. Emmerson ◽  
I. E. Galbally ◽  
A. B. Guenther ◽  
C. Paton-Walsh ◽  
E.-A. Guerette ◽  
...  
Keyword(s):  
Transport Model ◽  
Chemical Species ◽  
Field Measurements ◽  
Oxidation Products ◽  
Biogenic Emissions ◽  
Emission Rates ◽  
Chemical Transport Model ◽  
Southeast Australia ◽  
Unusual Position ◽  
Adult Trees

Abstract. The biogenic emissions of isoprene and monoterpenes are one of the main drivers of atmospheric photochemistry, including oxidant and secondary organic aerosol production. In this paper, the emission rates of isoprene and monoterpenes from Australian vegetation are investigated for the first time using the Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGANv2.1), the CSIRO chemical transport model, and atmospheric observations of isoprene, monoterpenes and isoprene oxidation products (methacrolein and methyl-vinyl-ketone). Observations from four field campaigns during three different seasons are used, covering urban, coastal suburban and inland forest areas. The observed concentrations of isoprene and monoterpenes were of a broadly similar magnitude, which may indicate that southeast Australia holds an unusual position where neither chemical species dominates. The model results overestimate the observed atmospheric concentrations of isoprene (up to a factor of 6) and underestimate the monoterpene concentrations (up to a factor of 4). This may occur because the emission rates currently used in MEGANv2.1 for Australia are drawn mainly from young Eucalypt trees (< 7 years), which may emit more isoprene than adult trees. There is no single increase/decrease factor for the emissions which suits all seasons and conditions studied. There is a need for further field measurements of in-situ isoprene and monoterpene emission fluxes in Australia.

scholarly journals Simulating secondary organic aerosol from missing diesel-related intermediate-volatility organic compound emissions during the Clean Air for London (ClearfLo) campaign

2016 ◽  
Author(s):  
R. Ots ◽  
D. E. Young ◽  
M. Vieno ◽  
L. Xu ◽  
R. E. Dunmore ◽  
...  
Keyword(s):  
Organic Compound ◽  
Atmospheric Chemistry ◽  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Field Measurements ◽  
Organic Aerosol ◽  
Total Particulate Matter ◽  
Aerosol Mass ◽  
Clean Air ◽  
The Uk

Abstract. We present high-resolution atmospheric chemistry transport model (ACTM) simulations of secondary organic aerosol (SOA) formation over the UK for 2012. Our simulations include additional diesel-related intermediate volatility organic compound (IVOC) emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo) campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA) as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA) components derived from aerosol mass spectrometer (AMS) measurements also made during the ClearfLo campaign at three sites in the London area. Good hourly performance in comparison to the measurements was shown, giving confidence in the SOA prediction skill of the ACTM system used. According to the model simulations, diesel-related IVOCs can explain on average ~30% of the annual SOA in and around London. Furthermore, the 90-th percentile of modelled daily SOA concentrations for the whole year is 3.8 μg m−3 (more than 40% of which is produced from the missing diesel precursors), constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories) is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.

scholarly journals FTIR time-series of biomass burning products (HCN, C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, CH<sub>3</sub>OH, and HCOOH) at Reunion Island (21° S, 55° E) and comparisons with model data

2012 ◽  
Vol 12 (21) ◽  
pp. 10367-10385 ◽  
Author(s):  
C. Vigouroux ◽  
T. Stavrakou ◽  
C. Whaley ◽  
B. Dils ◽  
V. Duflot ◽  
...  
Keyword(s):  
Time Series ◽  
Biomass Burning ◽  
Transport Model ◽  
Chemical Species ◽  
Global Scale ◽  
Reunion Island ◽  
Chemical Transport Model ◽  
Solar Absorption ◽  
Réunion Island ◽  
The Indian Ocean

Abstract. Reunion Island (21° S, 55° E), situated in the Indian Ocean at about 800 km east of Madagascar, is appropriately located to monitor the outflow of biomass burning pollution from Southern Africa and Madagascar, in the case of short-lived compounds, and from other Southern Hemispheric landmasses such as South America, in the case of longer-lived species. Ground-based Fourier transform infrared (FTIR) solar absorption observations are sensitive to a large number of biomass burning products. We present in this work the FTIR retrieval strategies, suitable for very humid sites such as Reunion Island, for hydrogen cyanide (HCN), ethane (C2H6), acetylene (C2H2), methanol (CH3OH), and formic acid (HCOOH). We provide their total columns time-series obtained from the measurements during August–October 2004, May–October 2007, and May 2009–December 2010. We show that biomass burning explains a large part of the observed seasonal and interannual variability of the chemical species. The correlations between the daily mean total columns of each of the species and those of CO, also measured with our FTIR spectrometer at Reunion Island, are very good from August to November (R &amp;geq; 0.86). This allows us to derive, for that period, the following enhancement ratios with respect to CO: 0.0047, 0.0078, 0.0020, 0.012, and 0.0046 for HCN, C2H6, C2H2, CH3OH, and HCOOH, respectively. The HCN ground-based data are compared to the chemical transport model GEOS-Chem, while the data for the other species are compared to the IMAGESv2 model. We show that using the HCN/CO ratio derived from our measurements (0.0047) in GEOS-Chem reduces the underestimation of the modeled HCN columns compared with the FTIR measurements. The comparisons between IMAGESv2 and the long-lived species C2H6 and C2H2 indicate that the biomass burning emissions used in the model (from the GFED3 inventory) are probably underestimated in the late September–October period for all years of measurements, and especially in 2004. The comparisons with the short-lived species, CH3OH and HCOOH, with lifetimes of around 5 days, suggest that the emission underestimation in late September–October 2004, occurs more specifically in the Southeastern Africa-Madagascar region. The very good correlation of CH3OH and HCOOH with CO suggests that, despite the dominance of the biogenic source of these compounds on the global scale, biomass burning is their major source at Reunion Island between August and November.

scholarly journals The influence of megacities on global atmospheric chemistry: a modelling study

2009 ◽  
Vol 6 (3) ◽  
pp. 219 ◽  
Author(s):  
Timothy M. Butler ◽  
Mark G. Lawrence
Keyword(s):  
Atmospheric Chemistry ◽  
Urban Areas ◽  
Radiative Forcing ◽  
Transport Model ◽  
Spatial Scales ◽  
Global Scale ◽  
Reactive Nitrogen ◽  
Grid Cells ◽  
Chemical Transport Model ◽  
Future Scenario

Environmental context. Over half of the population of the world now live in urban areas, and the number of so-called ‘megacities’, with populations of ~10 million or more, is growing at a tremendous rate. We show how these patterns of urbanisation have the potential to influence the atmospheric chemical environment on a global scale, particularly through the effects of emissions from megacities on the reactive nitrogen cycle. With the growing worldwide interest in the study of the effects of megacities at all spatial scales, such as current European Union projects MEGAPOLI and CityZen, our study represents the first of many future studies that examine the effects of megacities on atmospheric chemistry on the global scale. Abstract. We present the first study of the effects of megacities on global atmospheric chemistry using a global three-dimensional chemical transport model. The effects on air quality, radiative forcing and atmospheric oxidation capacity are disproportionately smaller than the proportion of anthropogenic emissions due to megacities. Disproportionately large effects of megacities are modelled for reactive nitrogen compounds, in particular PAN (peroxy acetyl nitrate), which has increased in abundance globally by 9% due to megacities under year 2000 conditions, with 23% of the Earth experiencing an increase of 10% or more. These influences decrease under two very different future emission scenarios. Under a low-emission future scenario, the influence of megacities is generally reduced, and under a high-emission future scenario, although the local influence of megacities is increased, the geographical extent of the influence becomes smaller. In our model, the individual grid cells that contain megacities respond to the megacity emissions differently depending on their latitude. Tropical megacity grid cells generally show increased ozone year-round, while northern extratropical megacities generally show reduced ozone year-round. Better parameterisation of the sub-grid effects of megacities is an important issue for future work.

scholarly journals The impact of ice uptake of nitric acid on atmospheric chemistry

2006 ◽  
Vol 6 (1) ◽  
pp. 225-235 ◽  
Author(s):  
R. von Kuhlmann ◽  
M. G. Lawrence
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Global Scale ◽  
Large Set ◽  
Model Match ◽  
Uptake Process ◽  
Significant Uptake ◽  
The Impact ◽  
Experimental And Theoretical Studies

Abstract. The potential impact of the uptake of HNO3 on ice on the distribution of NOy species, ozone and OH has been assessed using the global scale chemistry-transport model MATCH-MPIC. Assuming equilibrium uptake according to dissociative Langmuir theory results in significant reductions of gas phase HNO3. Comparison to a large set of observations provides support that significant uptake of HNO3 on ice is occurring, but the degree of the uptake cannot be inferred from this comparison alone. Sensitivity simulations show that the uncertainties in the total amount of ice formation in the atmosphere and the actual expression of the settling velocity of ice particles only result in small changes in our results. The largest uncertainty is likely to be linked to the actual theory describing the uptake process and the value of the initial uptake coefficient. The inclusion of non-methane hydrocarbon chemistry partially compensates for the absence of HNO3 uptake on ice when this is neglected in the model. The calculated overall effect on upper tropospheric ozone concentrations and the tropospheric methane lifetime are moderate to low. These results support a shift in the motivation for future experimental and theoretical studies of HNO3-ice interaction towards the role of HNO3 in hydrometeor surface physics.

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