Twelve years of global observations of formaldehyde in the troposphere using GOME and SCIAMACHY sensors

This work presents global tropospheric formaldehyde columns retrieved from near-UV radiance measurements performed by the GOME instrument onboard ERS-2 since 1995, and by SCIAMACHY, in operation on ENVISAT since the end of 2002. A special effort has been made to ensure the coherence and quality of the CH<sub>2</sub>O dataset covering the period 1996–2007. Optimised DOAS settings are proposed in order to reduce the impact of two important sources of error in the derivation of slant columns, namely, the polarisation anomaly affecting the SCIAMACHY spectra around 350 nm, and a major absorption band of the O<sub>4</sub> collision complex centred near 360 nm. The air mass factors are determined from scattering weights generated using radiative transfer calculations taking into account the cloud fraction, the cloud height and the ground albedo. Vertical profile shapes of CH<sub>2</sub>O are provided by the global CTM IMAGES based on an up-to-date representation of emissions, atmospheric transport and photochemistry. A comprehensive error analysis is presented. This includes errors on the slant columns retrieval and errors on the air mass factors which are mainly due to uncertainties in the a priori profile and in the cloud properties. The major features of the retrieved formaldehyde column distribution are discussed and compared with previous CH<sub>2</sub>O datasets over the major emission regions

Evaluating the performance of pyrogenic and biogenic emission inventories against one decade of space-based formaldehyde columns

A new one-decade (1997–2006) dataset of formaldehyde (HCHO) columns retrieved from GOME and SCIAMACHY is compared with HCHO columns simulated by an updated version of the IMAGES global chemical transport model. This model version includes an optimized chemical scheme with respect to HCHO production, where the short-term and final HCHO yields from pyrogenically emitted non-methane volatile organic compounds (NMVOCs) are estimated from the Master Chemical Mechanism (MCM) and an explicit speciation profile of pyrogenic emissions. The model is driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, whereas biogenic emissions are provided either by the Global Emissions Inventory Activity (GEIA), or by a newly developed inventory based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) algorithms driven by meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). The comparisons focus on tropical ecosystems, North America and China, which experience strong biogenic and biomass burning NMVOC emissions reflected in the enhanced measured HCHO columns. These comparisons aim at testing the ability of the model to reproduce the observed features of the HCHO distribution on the global scale and at providing a first assessment of the performance of the current emission inventories. The high correlation coefficients (<i>r</i>>0.7) between the observed and simulated columns over most regions indicate a good consistency between the model, the implemented inventories and the HCHO dataset. The use of the MEGAN-ECMWF inventory improves the model/data agreement in almost all regions, but biases persist over parts of Africa and Australia. Although neither GFED version is consistent with the data over all regions, a better agreement is achieved over Indonesia and Southern Africa when GFEDv2 is used, but GFEDv1 succeeds better in getting the correct seasonal patterns and intensities of the fire episodes over the Amazon basin, as reflected in the significantly higher correlations calculated in this region. Although the uncertainties in the HCHO retrievals, especially over fire scenes, can be quite large, this study provides a first assessment about whether the improved methodologies and input data implemented in GFEDv2 and MEGAN-ECMWF lead to better results in the comparisons of modelled with observed HCHO column measurements

Isoprene emissions over Asia 1979–2012: impact of climate and land-use changes

Due to the scarcity of observational constraints and the rapidly changing environment in East and Southeast Asia, isoprene emissions predicted by models are expected to bear substantial uncertainties. The aim of this study is to improve upon the existing bottom-up estimates, and to investigate the temporal evolution of the fluxes in Asia over 1979-2012. To this purpose, we calculate the hourly emissions at 0.5& deg; & times;0.5 & deg; resolution using the MEGAN-MOHYCAN model driven by ECMWF ERA-Interim climatology. In order to remedy for known biases identified in previous studies, and to improve the simulation of interannual variability and trends in emissions, this study incorporates (i) changes in land use, including the rapid expansion of oil palms, (ii) meteorological variability according to ERA-Interim, (iii) long-term changes in solar radiation (dimming/brightening) constrained by surface network radiation measurements, and (iv) recent experimental evidence that South Asian tropical forests are much weaker isoprene emitters than previously assumed, and on the other hand, that oil palms have a strong isoprene emission capacity. These effects lead to a significant lowering (factor of 2) in the total isoprene fluxes over the studied domain, and to emission reductions reaching a factor of 3.5 in Southeast Asia. The bottom-up annual isoprene emissions for 2005 are estimated at 7.0, 4.8, 8.3, and 2.9 Tg in China, India, Indonesia and Malaysia, respectively. The isoprene flux anomaly over the whole domain and studied period is found to be strongly correlated with the Oceanic Niño Index ( Combining double low line 0.73), with positive (negative) anomalies related to El Niño (La Niña) years. Changes in temperature and solar radiation are the major drivers of the interannual variability and trends in the emissions, except over semi-arid areas such as northwestern China, Pakistan and Kazakhstan, where soil moisture is by far the main cause of interannual emission changes. In our base simulation, annual positive flux trends of 0.2% and 0.52% throughout the entire period are found in Asia and China, respectively, related to a positive trend in temperature and solar radiation. The impact of oil palm expansion in Indonesia and Malaysia is to enhance the trends over that region, e.g., from 1.17% to 1.5% in 1979-2005 in Malaysia. A negative emission trend is derived in India (ĝ'0.4%), owing to the negative trend in solar radiation data associated with the strong dimming effect likely due to increasing aerosol loadings. The bottom-up emissions are compared to field campaign measurements in Borneo and South China and further evaluated against top-down isoprene emission estimates constrained by GOME-2/MetOp-A formaldehyde columns through 2007-2012. The satellite-based estimates appear to support our assumptions, and confirm the lower emission rate in tropical forests of Indonesia and Malaysia. Additional flux measurements are clearly needed to characterize the spatial variability of emission factors better. Finally, a decreasing trend in the inferred top-down Chinese emissions since 2007 is in line with recorded cooling in China after that year, thus suggesting that the satellite HCHO columns are able to capture climate-induced changes in emissions. © 2014 Author(s)

Global emissions of non-methane hydrocarbons deduced from SCIAMACHY formaldehyde columns through 2003-2006

Formaldehyde columns retrieved from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography/Chemistry (SCIAMACHY) instrument onboard ENVISAT satellite through 2003 to 2006 are used as top-down constraints to derive updated global biogenic and biomass burning flux estimates for the non-methane volatile organic compounds (NMVOCs) precursors of formaldehyde. Our interest is centered over regions experiencing strong emissions, and hence exhibiting a high signal-to-noise ratio and lower measurement uncertainties. The formaldehyde dataset used in this study has been recently made available to the community and complements the long record of formaldehyde measurements from the Global Ozone Monitoring Experiment (GOME). We use the IMAGESv2 global chemistry-transport model driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, and from the newly developed MEGAN-ECMWF isoprene emission database. The adjoint of the model is implemented in a grid-based framework within which emission fluxes are derived at the model resolution, together with a differentiation of the sources in a grid cell. Two inversion studies are conducted using either the GFEDv1 or GFEDv2 as a priori for the pyrogenic fluxes. Although on the global scale the inferred emissions from the two categories exhibit only weak deviations from the corresponding a priori estimates, the regional updates often present large departures from their a priori values. The posterior isoprene emissions over North America, amounting to about 34 Tg C/yr, are estimated to be on average by 25% lower than the a priori over 2003–2006, whereas a strong increase (55%) is deduced over the south African continent, the optimized emission being estimated at 57 Tg C/yr. Over Indonesia the biogenic emissions appear to be overestimated by 20–30%, whereas over Indochina and the Amazon basin during the wet season the a priori inventory captures both the seasonality and the magnitude of the observed columns. Although neither biomass burning inventory seems to be consistent with the data over all regions, pyrogenic estimates inferred from the two inversions are reasonably similar, despite their a priori deviations. A number of sensitivity experiments are conducted in order to assess the impact of uncertainties related to the inversion setup and the chemical mechanism. Whereas changes in the background error covariance matrix have only a limited impact on the posterior fluxes, the use of an alternative isoprene mechanism characterized by lower HCHO yields (the GEOS-Chem mechanism) increases the posterior isoprene source estimate by 11% over northern America, and by up to 40% in tropical regions

Global isoprene emissions estimated using MEGAN, ECMWF analyses and a detailed canopy environment model

International audienceThe global emissions of isoprene are calculated at 0.5° resolution for each year between 1995 and 2006, based on the MEGAN (Model of Emissions of Gases and Aerosols from Nature) version 2 model (Guenther et al., 2006) and a detailed multi-layer canopy environment model for the calculation of leaf temperature and visible radiation fluxes. The calculation is driven by meteorological fields ? air temperature, cloud cover, downward solar irradiance, windspeed, volumetric soil moisture in 4 soil layers ? provided by analyses of the European Centre for Medium-Range Weather Forecasts (ECMWF). The estimated annual global isoprene emission ranges between 374 Tg (in 1996) and 449 Tg (in 1998 and 2005), for an average of ca. 410 Tg/year over the whole period, i.e. about 30% less than the standard MEGAN estimate (Guenther et al., 2006). This difference is due, to a large extent, to the impact of the soil moisture stress factor, which is found here to decrease the global emissions by more than 20%. In qualitative agreement with past studies, high annual emissions are found to be generally associated with El Niño events. The emission inventory is evaluated against flux measurement campaigns at Harvard forest (Massachussets) and Tapajós in Amazonia, showing that the model can capture quite well the short-term variability of emissions, but that it fails to reproduce the observed seasonal variation at the tropical rainforest site, with largely overestimated wet season fluxes. The comparison of the HCHO vertical columns calculated by a chemistry and transport model (CTM) with HCHO distributions retrieved from space provides useful insights on tropical isoprene emissions. For example, the relatively low emissions calculated over Western Amazonia (compared to the corresponding estimates in the inventory of Guenther et al., 1995) are validated by the excellent agreement found between the CTM and HCHO data over this region. The parameterized impact of the soil moisture stress on isoprene emissions is found to reduce the model/data bias over Australia, but it leads to underestimated emissions near the end of the dry season over subtropical Africa

Ozone anomalies in the free troposphere during the COVID-19 pandemic

Using the CAM-chem Model, we simulate the response of chemical species in the free troposphere to scenarios of primary pollutant emission reductions during the COVID-19 pandemic. Zonally averaged ozone in the free troposphere during Northern Hemisphere spring and summer is found to be 5%-15% lower than 19-yr climatological values, in good agreement with observations. About one third of this anomaly is attributed to the reduction scenario of air traffic during the pandemic, another third to the reduction scenario of surface emissions, the remainder to 2020 meteorological conditions, including the exceptional springtime Arctic stratospheric ozone depletion. For the combined emission reductions, the overall COVID-19 reduction in northern hemisphere tropospheric ozone in June is less than 5 ppb below 400 hPa, but reaches 8 ppb at 250 hPa. In the Southern Hemisphere, COVID-19 related ozone reductions by 4%-6% were masked by comparable ozone increases due to other changes in 2020

Coastal New England pilot study to determine fossil and biogenic formaldehyde source contributions using radiocarbon

Author Posting. © American Geophysical Union, 2010. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research 115 (2010): D10301, doi:10.1029/2009JD012810.Compound specific radiocarbon analyses of atmospheric formaldehyde are reported as fraction modern (Fm) for a limited number of winter and summer air samples collected in coastal southern New England in 2007. The 11 of 13 samples with Fm 0.2 (max ∼ 0.35) were collected on days with strong northwesterly flow and the least urban impact. The Fm data were combined with VOC observations from the Rhode Island Department of Environmental Management, estimates of oxygenated VOC (OVOC), and back trajectories to interpret the relative contributions of biogenic and fossil carbon sources. It is argued that CH2O sources were dominated by pollutant VOCs and OVOCs from upwind coastal cities as opposed to more local biogenic VOCs at the times of sample collection.This research was supported by a graduate student internship program at WHOI National Ocean Sciences Accelerator Mass Spectrometry Facility (NSF OCE‐9807266) and by NASA project NNG04GB38G

Seasonality of isoprenoid emissions from a primary rainforest in central Amazonia

Tropical rainforests are an important source of isoprenoid and other volatile organic compound (VOC) emissions to the atmosphere. The seasonal variation of these compounds is however still poorly understood. In this study, vertical profiles of mixing ratios of isoprene, total monoterpenes and total sesquiterpenes, were measured within and above the canopy, in a primary rainforest in central Amazonia, using a proton transfer reaction – mass spectrometer (PTR-MS). Fluxes of these compounds from the canopy into the atmosphere were estimated from PTR-MS measurements by using an inverse Lagrangian transport model. Measurements were carried out continuously from September 2010 to January 2011, encompassing the dry and wet seasons. Mixing ratios were higher during the dry (isoprene – 2.68 ± 0.9 ppbv, total monoterpenes – 0.67 ± 0.3 ppbv; total sesquiterpenes – 0.09 ± 0.07 ppbv) than the wet season (isoprene – 1.66 ± 0.9 ppbv, total monoterpenes – 0.47 ± 0.2 ppbv; total sesquiterpenes – 0.03 ± 0.02 ppbv) for all compounds. Ambient air temperature and photosynthetically active radiation (PAR) behaved similarly. Daytime isoprene and total monoterpene mixing ratios were highest within the canopy, rather than near the ground or above the canopy. By comparison, daytime total sesquiterpene mixing ratios were highest near the ground. Daytime fluxes varied significantly between seasons for all compounds. The maximums for isoprene (2.53 ± 0.5 µmol m−2 h−1) and total monoterpenes (1.77 ± 0.05 µmol m−2 h−1) were observed in the late dry season, whereas the maximum for total sesquiterpenes was found during the dry-to-wet transition season (0.77 ± 0.1 µmol m−2 h−1). These flux estimates suggest that the canopy is the main source of isoprenoids emitted into the atmosphere for all seasons. However, uncertainties in turbulence parameterization near the ground could affect estimates of fluxes that come from the ground. Leaf phenology seemed to be an important driver of seasonal variation of isoprenoid emissions. Although remote sensing observations of changes in leaf area index were used to estimate leaf phenology, MEGAN 2.1 did not fully capture the behavior of seasonal emissions observed in this study. This could be a result of very local effects on the observed emissions, but also suggest that other parameters need to be better determined in biogenic volatile organic compound (BVOC) models. Our results support established findings that seasonality of isoprenoids are driven by seasonal changes in light, temperature and leaf phenology. However, they suggest that leaf phenology and its role on isoprenoid production and emission from tropical plant species needs to be better understood in order to develop mechanistic explanations for seasonal variation in emissions. This also may reduce the uncertainties of model estimates associated with the responses to environmental factors. Therefore, this study strongly encourages long-term measurements of isoprenoid emissions, environmental factors and leaf phenology from leaf to ecosystem scale, with the purpose of improving BVOC model approaches that can characterize seasonality of isoprenoid emissions from tropical rainforests

The AeroCom evaluation and intercomparison of organic aerosol in global models

This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately

Airborne observations reveal elevational gradient in tropical forest isoprene emissions

Isoprene dominates global non-methane volatile organic compound emissions, and impacts tropospheric chemistry by influencing oxidants and aerosols. Isoprene emission rates vary over several orders of magnitude for different plants, and characterizing this immense biological chemodiversity is a challenge for estimating isoprene emission from tropical forests. Here we present the isoprene emission estimates from aircraft eddy covariance measurements over the Amazonian forest. We report isoprene emission rates that are three times higher than satellite top-down estimates and 35% higher than model predictions. The results reveal strong correlations between observed isoprene emission rates and terrain elevations, which are confirmed by similar correlations between satellite-derived isoprene emissions and terrain elevations. We propose that the elevational gradient in the Amazonian forest isoprene emission capacity is determined by plant species distributions and can substantially explain isoprene emission variability in tropical forests, and use a model to demonstrate the resulting impacts on regional air quality