Laurens Ganzeveld

Atmospheric oxidation capacity sustained by a tropical forest

Terrestrial vegetation, especially tropical rain forest, releases vast quantities of volatile organic compounds (VOCs) to the atmosphere, which are removed by oxidation reactions and deposition of reaction products. The oxidation is mainly initiated by hydroxyl radicals (OH), primarily formed through the photodissociation of ozone. Previously it was thought that, in unpolluted air, biogenic VOCs deplete OH and reduce the atmospheric oxidation capacity. Conversely, in polluted air VOC oxidation leads to noxious oxidant build-up by the catalytic action of nitrogen oxides (NOx = NO + NO2). Here we report aircraft measurements of atmospheric trace gases performed over the pristine Amazon forest. Our data reveal unexpectedly high OH concentrations. We propose that natural VOC oxidation, notably of isoprene, recycles OH efficiently in low-NOx air through reactions of organic peroxy radicals. Computations with an atmospheric chemistry model and the results of laboratory experiments suggest that an OH recycling efficiency of 40–80 per cent in isoprene oxidation may be able to explain the high OH levels we observed in the field. Although further laboratory studies are necessary to explore the chemical mechanism responsible for OH recycling in more detail, our results demonstrate that the biosphere maintains a remarkable balance with the atmospheric environment.

Recent Trends in Global Greenhouse Gas Emissions: Regional Trends 1970-2000 and Spatial Distribution of Key Sources in 2000

Abstract In 2004, the Joint Research Centre (JRC) of the European Commission, the Netherlands Environmental Assessment Agency (MNP) and the Max Plank Institute for Chemistry (MPIC) started a project to create fast (bi-)annual updates of the EDGAR global emission inventory system, based on the more detailed previous version 3.2. Here, the key features of the Emission Database for Global Atmospheric Research, EDGAR 3 are first summarized, and then the compilation of recent global trends having a major influence on variables and the new ‘Fast Track’ approach to estimate recent emissions of greenhouse gases and air pollutants in 2000 at a country-specific level are described. Also provided is an overview of the approaches and data sources used for this EDGAR 3.2 Fast Track 2000 dataset, the different source sectors and the accuracies achieved, with a focus on anthropogenic sources of methane and nitrous oxide. Results of global emission trends for four air pollutants are also briefly addressed. Results for various sources and greenhouse gases at regional and national scales and on 1×1 degree grid have been made available on the EDGAR website.

Dry deposition parameterization in a chemistry general circulation model and its influence on the distribution of reactive trace gases

A dry deposition scheme has been developed for the chemistry general circulation model to improve the description of the removal of chemically reactive trace gases at the earths surface. The chemistry scheme simulates background CH 4 -CO-NO x -HO x photochemistry and calculates concentrations of, for example, HNO 3 , NO x , and O 3 . A resistance analog is used to parameterize the dry deposition velocity for these gases. The aerodynamic resistance is calculated from the model boundary layer stability, wind speed, and surface roughness, and a quasi-laminar boundary layer resistance is incorporated. The stomatal resistance is explicitly calculated and combined with representative cuticle and mesophyll resistances for each trace gas. The new scheme contributes to internal consistency in the model, in particular with respect to diurnal and seasonal cycles in both the chemistry and the planetary boundary layer processes and surface characteristics that control dry deposition. Evaluation of the model indicates satisfactory agreement between calculated and observed deposition velocities. Comparison of the results with model simulations in which the deposition velocity was kept constant indicates significant relative differences in deposition fluxes and surface layer trace gas concentrations up to about ±35%. Shortcomings are discussed, for example, violation of the constant flux approach for the surface layer, the lacking canopy description, and effects of surface water layers.

A dry deposition parameterization for sulfur oxides in a chemistry and general circulation model

A dry deposition scheme, originally developed to calculate the deposition velocities for the trace gases O3, NO2, NO, and HNO3 in the chemistry and general circulation European Centre Hamburg Model (ECHAM), is extended to sulfur dioxide (SO2) and sulfate (SO42−). In order to reduce some of the shortcomings of the previous model version a local surface roughness and a more realistic leaf area index (LAI), derived from a high-resolution ecosystem database are introduced. The current model calculates the deposition velocities from the aerodynamic resistance, a quasi-laminary boundary layer resistance and a surface resistance of the surface cover, e.g., snow/ice, bare soil, vegetation, wetted surfaces, and ocean. The SO2 deposition velocity over vegetated surfaces is calculated as a function of the vegetation activity, the canopy wetness, turbulent transport through the canopy to the soil, and uptake by the soil. The soil resistance is explicitly calculated from the relative humidity and the soil pH, derived from a high-resolution global soil pH database. The snow/ice resistance of SO2 is a function of temperature. The SO2 deposition velocity over the oceans is controlled by turbulence. The sulfate deposition velocity is calculated considering diffusion, impaction, and sedimentation. Over sea surfaces the effect of bubble bursting, causing the breakdown of the quasi-laminary boundary layer, scavenging of the sulfate aerosol by sea spray, and aerosol growth due to high local relative humidities are considered. An integrated sulfate deposition velocity is calculated, applying a unimodal mass size distribution over land and a bimodal mass size distribution over sea. The calculated sulfate deposition velocity is about an order of magnitude larger than that based on a monodisperse aerosol, which is often applied in chemistry-transport models. Incorporation of the new dry deposition scheme in the ECHAM model yields significant relative differences (up to ∼50%) in mass flux densities and surface layer concentrations compared to those calculated with a simple, constant dry deposition scheme.

Impact of future land use and land cover changes on atmospheric chemistry-climate interactions

annual soil NO emissions by ∼1.2 TgN yr −1 (9%), whereas isoprene emissions decrease by ∼50 TgC yr −1 (−12%). The analysis shows increases in simulated boundary layer ozone mixing ratios up to ∼9 ppbv and more than a doubling in hydroxyl radical concentrations over deforested areas in Africa. Small changes in global atmosphere‐biosphere fluxes of NOx and ozone point to compensating effects. Decreases in soil NO emissions in deforested regions are counteracted by a larger canopy release of NOx caused by reduced foliage uptake. Despite this decrease in foliage uptake, the ozone deposition flux does not decrease since surface layer mixing ratios increase because of a reduced oxidation of isoprene by ozone. Our study indicates that the simulated impact of land cover and land use changes on atmospheric chemistry depends on a consistent representation of emissions, deposition, and canopy interactions and their dependence on meteorological, hydrological, and biological drivers to account for these compensating effects. It results in negligible changes in the atmospheric oxidizing capacity and, consequently, in the lifetime of methane. Conversely, we expect a pronounced increase in oxidizing capacity as a consequence of anthropogenic emission increases. Citation: Ganzeveld, L., L. Bouwman, E. Stehfest, D. P. van Vuuren, B. Eickhout, and J. Lelieveld (2010), Impact of future land use and land cover changes on atmospheric chemistry‐climate interactions, J. Geophys. Res., 115, D23301,

Atmosphere-ocean ozone exchange: A global modeling study of biogeochemical, atmospheric, and waterside turbulence dependencies

Received 9 July 2008; revised 12 June 2009; accepted 17 July 2009; published 7 November 2009. [1] The significance of the removal of tropospheric ozone by the oceans, covering 2/3 of the Earth’s surface, has only been addressed in a few studies involving water tank, aircraft, and tower flux measurements. On the basis of results from these few observations of the ozone dry deposition velocity (VdO3), atmospheric chemistry models generally apply an empirical, constant ocean uptake rate of 0.05 cm s 1 . This value is substantially smaller than the atmospheric turbulent transport velocity for ozone. On the other hand, the uptake is higher than expected from the solubility of ozone in clean water alone, suggesting that there is an enhancement in oceanic ozone uptake, e.g., through a chemical destruction mechanism. We present an evaluation of a global-scale analysis with a new mechanistic representation of atmosphere-ocean ozone exchange. The applied atmosphere chemistry-climate model includes not only atmospheric but also waterside turbulence and the role of waterside chemical loss processes as a function of oceanic biogeochemistry. The simulations suggest a larger role of biogeochemistry in tropical and subtropical ozone oceanic uptake with a relative small temporal variability, whereas in midlatitude and high-latitude regions, highly variable ozone uptake rates are expected because of the stronger influence of waterside turbulence. Despite a relatively large range in the explicitly calculated ocean uptake rate, there is a surprisingly small sensitivity of simulated Marine Boundary Layer ozone concentrations compared to the sensitivity for the commonly applied constant ocean uptake approach. This small sensitivity points at compensating effects through inclusion of the process-based ocean uptake mechanisms to consider variability in oceanic O3 deposition consistent with that in atmospheric and oceanic physical, chemical, and biological processes.

A comprehensive view on climate change: Coupling of earth system and integrated assessment models

There are several reasons to strengthen the cooperation between the integrated assessment (IA) and earth system (ES) modeling teams in order to better understand the joint development of environmental and human systems. This cooperation can take many different forms, ranging from information exchange between research communities to fully coupled modeling approaches. Here, we discuss the strengths and weaknesses of different approaches and try to establish some guidelines for their applicability, based mainly on the type of interaction between the model components (including the role of feedback), possibilities for simplification and the importance of uncertainty. We also discuss several important areas of joint IA‐ES research, such as land use/land cover dynamics and the interaction between climate change and air pollution, and indicate the type of collaboration that seems to be most appropriate in each case. We find that full coupling of IA‐ES models might not always be the most desirable form of cooperation, since in some cases the direct feedbacks between IA and ES may be too weak or subject to considerable process or scenario uncertainty. However, when local processes are important, it could be important to consider full integration. By encouraging cooperation between the IA and ES communities in the future more consistent insights can be developed.

Atmosphere‐ocean ozone fluxes during the TexAQS 2006, STRATUS 2006, GOMECC 2007, GasEx 2008, and AMMA 2008 cruises

A ship-based eddy covariance ozone flux system was deployed to investigate the magnitude and variability of ozone surface fluxes over the open ocean. The flux experiments were conducted on five cruises on board the NOAA research vessel Ronald Brown during 2006-2008. The cruises covered the Gulf of Mexico, the southern as well as northern Atlantic, the Southern Ocean, and the persistent stratus cloud region off Chile in the eastern Pacific Ocean. These experiments resulted in the first ship-borne open-ocean ozone flux measurement records. The median of 10 min oceanic ozone deposition velocity (v(d)) results from a combined similar to 1700 h of observations ranged from 0.009 to 0.034 cm s(-1). For the Gulf of Mexico cruise (Texas Air Quality Study (TexAQS)) the median v(d) (interquartile range) was 0.034 (0.009-0.065) cm s(-1) (total number of 10 min measurement intervals, N-f = 1953). For the STRATUS cruise off the Chilean coast, the median v(d) was 0.009 (0.004-0.037) cm s(-1) (N-f = 1336). For the cruise from the Gulf of Mexico and up the eastern U. S. coast (Gulf of Mexico and East Coast Carbon cruise (GOMECC)) a combined value of 0.018 (0.006-0.045) cm s(-1) (N-f = 1784) was obtained (from 0.019 (-0.014-0.043) cm s(-1), N-f = 663 in the Gulf of Mexico, and 0.018 (-0.004-0.045) cm s(-1), N-f = 1121 in the North Atlantic region). The Southern Ocean Gas Exchange Experiment (GasEx) and African Monsoon Multidisciplinary Analysis (AMMA), the Southern Ocean and northeastern Atlantic cruises, respectively, resulted in median ozone v(d) of 0.009 (-0.005-0.026) cm s(-1) (N-f = 2745) and 0.020 (-0.003-0.044) cms(-1) (N-f = 1147). These directly measured ozone deposition values are at the lower end of previously reported data in the literature (0.01-0.12 cm s(-1)) for ocean water. Data illustrate a positive correlation (increase) of the oceanic ozone uptake rate with wind speed, albeit the behavior of the relationship appears to differ during these cruises. The encountered wide range of meteorological and ocean biogeochemical conditions is used to investigate fundamental drivers of oceanic O-3 deposition and for the evaluation of a recently developed global oceanic O-3 deposition modeling system.

Global reactive nitrogen deposition from lightning NOx

We present results of the deposition of nitrogen compounds formed from lightning (LNO x ) using the global chemical transport Model of Atmospheric Transport and Chemistry?Max Planck Institute for Chemistry version. The model indicates an approximately equal deposition of LNO x in both terrestrial and oceanic ecosystems, primarily in the tropics and midlatitudes open ocean, despite much higher intensities of lightning flashes above landmasses. The highest values of deposition are due to wet convective deposition, with highest values concentrated in the tropical continents. Nonconvective wet deposition, associated with large-scale weather patterns, occurs over large areas of the ocean amid lower values per square meter, manifesting the long-range transport of NO y , including long-lived species such as HNO3 at high altitudes and PAN. Dry deposition is concentrated primarily above landmasses, yet oceanic deposition over wide areas is still observed. Combined together, the total LNO x deposition exhibits maximal influx values over land, whereas oceanic deposition over wider areas renders the integrated deposition over both ecosystems almost identical. Peaks of terrestrial deposition values (located in Africa, South America, and Asia) show seasonal variability by meridionally penetrating the northern or southern midlatitude following the corresponding summer hemisphere, in accordance with the migration of LNO x production sites. On land, wet and dry deposition rates are more or less equal with a small bias toward wet deposition, whereas above the ocean, wet deposition is markedly higher because of a small water uptake efficiency and relatively small surface roughness. Further work of modeling additional species and obtaining more information on different compounds is required

On the Segregation of Chemical Species in a Clear Boundary Layer Over Heterogeneous Surface Conditions

The chemical segregation of isoprene has been investigated over heterogeneous surface conditions, and first results are presented and analysed.