ALBERT

Description: We use isoprene and related field measurements from three different ocean data sets together with remotely sensed satellite data to model global marine isoprene emissions. We show that using monthly mean satellite-derived chl a concentrations to parameterize isoprene with a constant chl a normalized isoprene production rate underpredicts the measured oceanic isoprene concentration by a mean factor of 19 ± 12. Improving the model by using phytoplankton functional type dependent production values and by decreasing the bacterial degradation rate of isoprene in the water column results in only a slight underestimation (factor 1.7 ± 1.2). We calculate global isoprene emissions of 0.21 Tg C for 2014 using this improved model, which is twice the value calculated using the original model. Nonetheless, the sea-to-air fluxes have to be at least 1 order of magnitude higher to account for measured atmospheric isoprene mixing ratios. These findings suggest that there is at least one missing oceanic source of isoprene and, possibly, other unknown factors in the ocean or atmosphere influencing the atmospheric values. The discrepancy between calculated fluxes and atmospheric observations must be reconciled in order to fully understand the importance of marine-derived isoprene as a precursor to remote marine boundary layer particle formation.

Description: The main field activities of the Coordinated Airborne Studies in the Tropics (CAST) campaign took place in the west Pacific during January–February 2014. The field campaign was based in Guam (13.5°N, 144.8°E), using the U.K. Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 atmospheric research aircraft, and was coordinated with the Airborne Tropical Tropopause Experiment (ATTREX) project with an unmanned Global Hawk and the Convective Transport of Active Species in the Tropics (CONTRAST) campaign with a Gulfstream V aircraft. Together, the three aircraft were able to make detailed measurements of atmospheric structure and composition from the ocean surface to 20 km. These measurements are providing new information about the processes influencing halogen and ozone levels in the tropical west Pacific, as well as the importance of trace-gas transport in convection for the upper troposphere and stratosphere. The FAAM aircraft made a total of 25 flights in the region between 1°S and 14°N and 130° and 155°E. It was used to sample at altitudes below 8 km, with much of the time spent in the marine boundary layer. It measured a range of chemical species and sampled extensively within the region of main inflow into the strong west Pacific convection. The CAST team also made ground-based measurements of a number of species (including daily ozonesondes) at the Atmospheric Radiation Measurement Program site on Manus Island, Papua New Guinea (2.1°S, 147.4°E). This article presents an overview of the CAST project, focusing on the design and operation of the west Pacific experiment. It additionally discusses some new developments in CAST, including flights of new instruments on board the Global Hawk in February–March 2015.

Description: We have developed an ensemble Kalman Filter (EnKF) to estimate 8-day regional surface fluxes of CO2 from space-borne CO2 dry-air mole fraction observations (XCO2

Description: We use the GEOS-Chem chemistry transport model to interpret variability of CO2 columns and associated column-averaged volume mixing ratios (CVMRs) observed by the SCIAMACHY satellite instrument during the 2003 North American growing season, accounting for the instrument averaging kernel. Model and observed columns, largely determined by surface topography, averaged on a 2°×2.5° grid, are in excellent agreement (model bias=3%, r〉0.9), as expected. Model and observed CVMRs, determined by scaling column CO2 by surface pressure data, are on average within 3% but are only weakly correlated, reflecting a large positive model bias (10–15 ppmv) at 50–70° N during midsummer at the peak of biospheric uptake. GEOS-Chem generally reproduces the magnitude and seasonal cycle of observed CO2 surface VMRs across North America. During midsummer we find that model CVMRs and surface VMRs converge, reflecting the instrument vertical sensitivity and the strong influence of the land biosphere on lower tropospheric CO2 columns. We use model tagged tracers to show that local fluxes largely determine CVMR variability over North America, with the largest individual CVMR contributions (1.1%) from the land biosphere. Fuel sources are relatively constant while biomass burning make a significant contribution only during midsummer. We also show that non-local sources contribute significantly to total CVMRs over North America, with the boreal Asian land biosphere contributing close to 1% in midsummer at high latitudes. We used the monthly-mean Jacobian matrix for North America to illustrate that: 1) North American CVMRs represent a superposition of many weak flux signatures, but differences in flux distributions should permit independent flux estimation; and 2) the atmospheric e-folding lifetimes for many of these flux signatures are 3–4 months, beyond which time they are too well-mixed to interpret.

Description: Emissions of biogenic volatile organic compounds (BVOC) are a chief uncertainty in calculating the burdens of important atmospheric compounds like tropospheric ozone or secondary organic aerosol, reflecting either imperfect chemical oxidation mechanisms or unreliable emission estimates, or both. To provide a starting point for a more systematic discussion we review here global isoprene and monoterpene emission estimates to-date. We note a surprisingly small variation in the predictions of global isoprene emission rate that is in stark contrast with our lack of process understanding and the small number of observations for model parameterisation and evaluation. Most of the models are based on similar emission algorithms, using fixed values for the emission capacity of various plant functional types. In some studies these values are very similar, but they differ substantially in others. The models differ also broadly with regard to their representation of net primary productivity, method of biome coverage determination and climate data. Their similarities with regard to the global isoprene emission rate would suggest that the dominant parameters driving the ultimate global estimate, and thus the dominant determinant of model sensitivity, are the specific emission algorithm and isoprene emission capacity. Contrary to isoprene, monoterpene estimates show significantly larger model-to-model variation although variation in terms of leaf algorithm, emission capacities, the way of model upscaling, vegetation cover or climatology used in terpene models are comparable to those used for isoprene. From our summary of published studies there appears to be no evidence that the terrestrial modelling community has been any more successful in "resolving unknowns" in the mechanisms that control global isoprene emissions, compared to global monoterpene emissions. Rather, the proliferation of common parameterization schemes within a large variety of model platforms lends the illusion of convergence towards a common estimate of global isoprene emissions. This convergence might be used to provide optimism that the community has reached the "relief phase", the phase when sufficient process understanding and data for evaluation allows for models to converge, when applying a recently proposed concept. We argue that there is no basis for this apparent "relief" phase. Rather, we urge modellers to be bolder in their analysis to draw attention to the fact that terrestrial emissions, particularly in the area of biome-specific emission capacities, are unknown rather than uncertain.

Description: We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.

Description: We use the GEOS-Chem global 3-D chemistry transport model to investigate the relative importance of chemical and physical processes that determine observed variability of hydrogen cyanide (HCN) in the troposphere and lower stratosphere. Consequently, we reconcile ground-based FTIR column measurements of HCN, which show annual and semi-annual variations, with recent space-borne measurements of HCN mixing ratio in the tropical lower stratosphere, which show a large two-year variation. We find that the observed column variability over the ground-based stations is determined by a superposition of HCN from several regional burning sources, with GEOS-Chem reproducing these column data with a positive bias of 5%. GEOS-Chem reproduces the observed tropical HCN variability from the Microwave Limb Sounder and the Atmospheric Chemistry Experiment satellite instruments with a negative bias of 7%. We show the tropical biomass burning emissions explain mostly the observed HCN variations in the upper troposphere and lower stratosphere (UTLS), with the remainder due to atmospheric transport and HCN chemistry. In the mid and upper stratosphere, atmospheric dynamics progressively exerts more influences on HCN variations. The extent of temporal overlap between African and other continental burning seasons is key in establishing the apparent bienniel cycle in the UTLS. Similar analysis of other, shorter-lived trace gases have not observed the transition between annual and bienniel cycles in the UTLS probably because the signal of inter-annual variations from surface emission has vanished before arriving at the lower stratosphere (LS), due to shorter atmospheric lifetimes.

Description: We use the GEOS-Chem chemistry transport model to interpret the sources and sinks of CO2 that determine variability of column-averaged volume mixing ratios (CVMRs), as observed by the SCIAMACHY satellite instrument, during the 2003 North American growing season. GEOS-Chem generally reproduces the magnitude and seasonal cycle of observed CO2 surface VMRs across North America and is quantitatively consistent with column VMRs in later years. However, it cannot reproduce the magnitude or variability of FSI-WFM-DOAS SCIAMACHY CVMRs. We use model tagged tracers to show that local fluxes largely determine CVMR variability over North America, with the largest individual CVMR contributions (1.1%) from the land biosphere. Fuel sources are relatively constant while biomass burning makes a significant contribution only during midsummer. We also show that non-local sources contribute significantly to total CVMRs over North America, with the boreal Asian land biosphere contributing close to 1% in midsummer at high latitudes. We used the monthly-mean Jacobian matrix for North America to illustrate that:~1) North American CVMRs represent a superposition of many weak flux signatures, but differences in flux distributions should permit independent flux estimation; and 2) the atmospheric e-folding lifetimes for many of these flux signatures are 3–4 months, beyond which time they are too well-mixed to interpret. These long lifetimes will improve the efficacy of observed CVMRs as surface CO2 flux constraints.

Description: Seasonally-resolved upper tropospheric profiles of formaldehyde (HCHO) observed by the ACE Fourier transform spectrometer (ACE-FTS) on a near-global scale are presented for the time period from March 2004 to November 2006. Large upper tropospheric HCHO mixing ratios (〉150 pptv) are observed during the growing season of the terrestrial biosphere in the Northern Hemisphere and during the biomass burning season in the Southern Hemisphere. The total errors estimated for the retrieved mixing ratios range from 30 to 40% in the upper troposphere and increase in the lower stratosphere. The sampled HCHO concentrations are in satisfactory agreement with previous aircraft and satellite observations with a negative bias (0.9). Both models underestimate the summer maximum over Europe and Russia and differences in the emissions used for North America result in a good reproduction of the summer maximum by GEOS-Chem but in an underestimate by LMDz-INCA. Globally, GEOS-Chem reproduces well the observations on average over one year but has some difficulties in reproducing the spatial variability of the observations. LMDz-INCA shows significant bias in the Southern Hemisphere, perhaps related to an underestimation of methane, but better reproduces the temporal and spatial variations. The differences between the models underline the large uncertainties that remain in the emissions of HCHO precursors.