Abstract. Spectroscopic measurements of atmospheric N2O and CH4 mole fractions were made on board the FAAM (Facility for Airborne Atmospheric Measurements) large atmospheric research aircraft. We present details of the mid-infrared quantum cascade laser absorption spectrometer (QCLAS, Aerodyne Research Inc., USA) employed, including its configuration for airborne sampling, and evaluate its performance over 17 flights conducted during summer 2014. Two different methods of correcting for the influence of water vapour on the spectroscopic retrievals are compared and evaluated. A new in-flight calibration procedure to account for the observed sensitivity of the instrument to ambient pressure changes is described, and its impact on instrument performance is assessed. Test flight data linking this sensitivity to changes in cabin pressure are presented. Total 1σ uncertainties of 2.47 ppb for CH4 and 0.54 ppb for N2O are derived. We report a mean difference in 1 Hz CH4 mole fraction of 2.05 ppb (1σ = 5.85 ppb) between in-flight measurements made using the QCLAS and simultaneous measurements using a previously characterised Fast Greenhouse Gas Analyser (FGGA, Los Gatos Research, USA). Finally, a potential case study for the estimation of a regional N2O flux using a mass balance technique is identified, and the method for calculating such an estimate is outlined.
We have conducted an observing system simulation experiment for the Tropospheric Emission Spectrometer (TES) satellite instrument to determine the potential of nadir retrievals of carbon monoxide (CO) from this instrument to constrain estimates of continental sources of CO. We use the GEOS‐CHEM global chemical transport model to produce a pseudoatmosphere in which the relationship between sources and concentrations of CO is known. Linear profile retrievals of CO are calculated by sampling this pseudoatmosphere along the orbit of TES. These retrievals are used as pseudo‐observations with a maximum a posteriori inverse algorithm to estimate the CO sources from the different continents. This algorithm accounts for the finite vertical resolution of the retrieval, instrument errors, and representation and transport errors in the GEOS‐CHEM simulation of CO. The structure of the transport error is estimated using the statistics of the difference between paired GEOS‐CHEM forecasts of CO, and this structure is then scaled to match the model error in the GEOS‐CHEM simulation of aircraft observations of Asian outflow over the NW Pacific. We show that with proper characterization of observation errors just 2 weeks of observations from TES have the potential to constrain estimates of continental sources of CO to within 10%.
Aircraft observations of Asian outflow from the Transport and Chemical Evolution Over the Pacific (TRACE‐P) aircraft mission over the NW Pacific (March and April 2001) show large CH 4 enhancements relative to background, as well as strong CH 4 ‐C 2 H 6 ‐CO correlations that provide signatures of regional sources. We apply a global chemical transport model simulation of the CH 4 ‐C 2 H 6 ‐CO system for the TRACE‐P period to interpret these observations in terms of CH 4 sources and to explore in particular the unique constraints from the CH 4 ‐C 2 H 6 ‐CO correlations. We use as a priori a global CH 4 source inventory constrained with National Oceanic and Atmospheric Administration (NOAA) Climate Monitoring and Diagnostics Laboratory (CMDL) surface observations [ Wang et al. , 2004 ]. We find that the observed CH 4 concentration enhancements and CH 4 ‐C 2 H 6 ‐CO correlations in Asian outflow in TRACE‐P are determined mainly by anthropogenic emissions from China and Eurasia (defined here as Europe and eastern Russia), with only little contribution from tropical sources (wetlands and biomass burning). The a priori inventory overestimates the observed CH 4 enhancements and shows regionally variable biases for the CH 4 /C 2 H 6 slope. The CH 4 /CO slopes are simulated without significant bias. Matching both the observed CH 4 enhancements and the CH 4 ‐C 2 H 6 ‐CO slopes in Asian outflow requires increasing the east Asian anthropogenic source of CH 4 , and decreasing the Eurasian anthropogenic source, by at least 30% for both. The need to increase the east Asian source is driven by the underestimate of the CH 4 /C 2 H 6 slope in boundary layer Chinese outflow. The Streets et al. [2003] anthropogenic emission inventory for east Asia fits this constraint by increasing CH 4 emissions from that region by 40% relative to the a priori, largely because of higher livestock and landfill source estimates. Eurasian sources (mostly European) then need to be reduced by 30–50% from the a priori value of 68 Tg yr −1 . The decrease of European sources could result in part from recent mitigation of emissions from coal mining and landfills.
Abstract. Atmospheric inversion approaches are expected to play a critical role in future observation-based monitoring systems for surface fluxes of greenhouse gases (GHGs), pollutants and other trace gases. In the past decade, the research community has developed various inversion software, mainly using variational or ensemble Bayesian optimization methods, with various assumptions on uncertainty structures and prior information and with various atmospheric chemistry–transport models. Each of them can assimilate some or all of the available observation streams for its domain area of interest: flask samples, in situ measurements or satellite observations. Although referenced in peer-reviewed publications and usually accessible across the research community, most systems are not at the level of transparency, flexibility and accessibility needed to provide the scientific community and policy makers with a comprehensive and robust view of the uncertainties associated with the inverse estimation of GHG and reactive species fluxes. Furthermore, their development, usually carried out by individual research institutes, may in the future not keep pace with the increasing scientific needs and technical possibilities. We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is primarily a programming protocol to allow various inversion bricks to be exchanged among researchers. In practice, the ensemble of bricks makes a flexible, transparent and open-source Python-based tool to estimate the fluxes of various GHGs and reactive species both at the global and regional scales. It will allow for running different atmospheric transport models, different observation streams and different data assimilation approaches. This adaptability will allow for a comprehensive assessment of uncertainty in a fully consistent framework. We present here the main structure and functionalities of the system, and we demonstrate how it operates in a simple academic case.
Two cold front episodes were sampled during the two flights out of Yokota, Japan, during the Transport and Chemical Evolution Over the Pacific (TRACE‐P) experiment during March 2001. The data from these two flights are examined using a mesoscale three‐dimensional model. We show how these cyclonic systems have impacted the export of pollution out of the Asian continent. We contrast the relative role of convection and ascent in the warm conveyor belts associated with the cyclone during these two episodes. Although the necessary meteorological conditions for an efficient export of pollution are met during flight 13 (i.e., the occurrences of the warm conveyor belt near the source regions), no significant pollution is simulated in the mid‐Pacific in the lower and middle troposphere. The efficient ventilation of the WCB by convection near the coast, the advection by the anticyclonical flow above 700 hPa, and the downward motion associated with the Pacific high in the remote ocean significantly prevent any long‐range transport of undiluted pollution in the WCB. During flight 15 the conveyor belts have already moved to the remote ocean. The polluted plume is split by the rising air in the warm conveyor belt which transports CO‐poor air northward and by the oceanic convection which transports clean air masses upward. These mechanisms lead to the dilution of Asian pollution in WCB en route to North America and add to the episodic nature of the Asian outflow by fragmenting the pollution plume.
Abstract. GHOST is a novel, compact shortwave-infrared grating spectrometer, designed for remote sensing of tropospheric columns of greenhouse gases (GHGs) from an airborne platform. It observes solar radiation at medium to high spectral resolution (better than 0.3 nm), which has been reflected by the Earth's surface using similar methods to those used by polar-orbiting satellites such as the JAXA GOSAT mission, NASA's OCO-2, and the Copernicus Sentinel-5 Precursor. By using an original design comprising optical fibre inputs along with a single diffraction grating and detector array, GHOST is able to observe CO2 absorption bands centred around 1.61 and 2.06 µm (the same wavelength regions used by OCO-2 and GOSAT) whilst simultaneously measuring CH4 absorption at 1.65 µm (also observed by GOSAT) and CH4 and CO at 2.30 µm (observed by Sentinel-5P). With emissions expected to become more concentrated towards city sources as the global population residing in urban areas increases, there emerges a clear requirement to bridge the spatial scale gap between small-scale urban emission sources and global-scale GHG variations. In addition to the benefits achieved in spatial coverage through being able to remotely sense GHG tropospheric columns from an aircraft, the overlapping spectral ranges and comparable spectral resolutions mean that GHOST has unique potential for providing validation opportunities for these platforms, particularly over the ocean, where ground-based validation measurements are not available. In this paper we provide an overview of the GHOST instrument, calibration, and data processing, demonstrating the instrument's performance and suitability for GHG remote sensing. We also report on the first GHG observations made by GHOST during its maiden science flights on board the NASA Global Hawk unmanned aerial vehicle, which took place over the eastern Pacific Ocean in March 2015 as part of the CAST/ATTREX joint Global Hawk flight campaign.
Abstract. We use the GEOS-Chem global 3-D atmospheric chemistry transport model to interpret atmospheric observations of bromoform (CHBr3) and dibromomethane (CH2Br2) collected during the CAST and CONTRAST aircraft measurement campaigns over the western Pacific, January–February 2014. We use a new linearized, tagged version of CHBr3 and CH2Br2, allowing us to study the influence of emissions from specific geographical regions on observed atmospheric variations. The model describes 32 %–37 % of CHBr3 and 15 %–45 % of CH2Br2 observed variability during CAST and CONTRAST, reflecting model errors in vertical transport. The model has a mean positive bias of 30 % that is larger near the surface, reflecting errors in the poorly constrained prior emission estimates. We find using the model that observed variability of CHBr3 and CH2Br2 is driven by open ocean emissions where there is deep convection. Atmospheric variability above 6 km includes a significant contribution from coastal oceans, but it is still dominated by emissions from the open ocean and by older air masses that originate upwind. In the absence of reliable ocean emission estimates, we use a new physical age-of-air simulation to determine the relative abundance of halogens delivered by CHBr3 and CH2Br2 to the tropical transition layer (TTL). We find that 76 % (92 %) of air masses that originate from the ocean reach the TTL within two (three) atmospheric e-folding lifetimes of CHBr3 and almost all of them reach the TTL within one e-folding lifetime of CH2Br2. Over the duration of CAST and CONTRAST, and over our study region, oceans delivered a mean (range) CHBr3 and CH2Br2 mole fraction of 0.46 (0.13–0.72) and 0.88 (0.71–1.01) pptv, respectively, to the TTL, and a mean (range) Bry mole fraction of 3.14 (1.81–4.18) pptv from source gases to the upper troposphere.
An objective method, employing HYSPLIT back-trajectories and Moderate Resolution Imaging Spectroradiometer (MODIS) fire observations, is developed to estimate ozone enhancement in air transported from regions of active forest fires at 18 ozone sounding sites located across North America. The Differential Back Trajectory (DBT) method compares mean differences between ozone concentrations associated with fire-affected and fire-unaffected parcels. It is applied to more than 1100 ozonesonde profiles collected from these sites during the summer months June to August 2006, 2008, 2010 and 2011. Layers of high ozone associated with low humidity were first removed from the ozonesonde profiles to minimize the potential effects of stratospheric intrusions on the calculations. No significant influence on average ozone levels by North American fires was found for stations located at Arctic latitudes. The ozone enhancement for stations nearer large fires, such as Trinidad Head and Bratt's Lake, was up to 4.8% of the TTOC (Total Tropospheric Ozone Column). Fire ozone accounted for up to 8.3% of TTOC at downwind sites such as Yarmouth, Sable Island, Narragansett, and Walsingham. The results are consistent with other studies that have reported an increase in ozone production with the age of the smoke plume.
Abstract. We use the GEOS-Chem atmospheric chemistry transport model to interpret aircraft measurements of carbon monoxide (CO) in biomass burning outflow taken during the 2011 BORTAS-B campaign over eastern Canada. The model has some skill reproducing the observed variability (r = 0.45) but has a negative bias for observations below 100 ppb and a positive bias above 300 ppb. We find that observed CO variations are largely due to NW North American biomass burning, as expected, with smaller and less variable contributions from fossil fuel combustion from eastern Asia and NE North America. To help interpret observed variations of CO we develop an Eulerian effective age of emissions (A) metric, accounting for mixing and chemical decay, which we apply to pyrogenic emissions of CO. We find that during BORTAS-B the age of emissions intercepted over Halifax, Nova Scotia is typically 4–11 days, and on occasion as young as two days. We show that A is typically 1–5 days older than the associated photochemical ages inferred from colocated measurements of different hydrocarbons. We find that the median difference between the age measures (Δτ) in plumes (CH3CN > 150 ppt) peaks at 3–5 days corresponding to a chemical retardation of 50%. We find a strong relationship in plumes between A and Δτ (r2 = 0.60), which is not evident outwith these plumes (r2 = 0.23). We argue that these observed relationships, together with a robust observed relationship between CO and black carbon aerosol during BORTAS-B (r2 > 0.7), form the basis of indirect evidence that aerosols co-emitted with gases during pyrolysis markedly slowed down the plume photochemistry during BORTAS-B with respect to photochemistry at the same latitude and altitude in clear skies.
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