Model studies of the meteorology and chemical composition of the troposphere over the North Atlantic during August 18-30, 1993

A mesoscale chemistry transport model driven by meteorological data from a numerical weather prediction model is used to calculate ozone, carbon monoxide, oxides of nitrogen, and other chemical species over the North Atlantic for a 13-days period (August 18-30, 1993). The model has a circumpolar grid so that the boundary condition problems are minimized, and the influence of North American emissions on the chemical composition of the troposphere over the North Atlantic and Europe is calculated. During the first part of the period there is a zonal flow across the North Atlantic in the free troposphere; later, there is a strong north-south as well as vertical component in the advection field. The variability in the concentrations of ozone in the free troposphere is mainly caused by dynamical processes, while the chemical modification is small over an integration time of less than two weeks. A continental plume off the North American continent extending 2000 km or more into the North Atlantic is identified toward the end of the calculation period. There is then a maximum in the concentration of ozone around 1 km above the sea surface, with a much lower concentration in the marine boundary layer close to the ocean surface. Measurements from the U.K. Meteorological Office Hercules C-130 in the free troposphere off the Atlantic Provinces, across the Atlantic Ocean, and around the Azores together with ozone soundings from the Azores, Bermuda, and Iceland were used for model comparison. The calculations indicate that in the free troposphere the initial conditions as well as the upper boundary conditions are important for ozone distribution. In the upper troposphere the net change in the chemical formation rate of ozone due to a change in the NOx concentration is quite independent of the absolute value of the ozone concentration itself and, consequently, the choice of boundary conditions for ozone is not so important in this context, In the lower troposphere the change in the net chemical formation rate of ozone, which follows from a change in the concentration of NOx, shows a marked dependence on the concentration of ozone

Calibration of TCCON column-averaged CO2: the first aircraft campaign over European TCCON sites

The Total Carbon Column Observing Network (TCCON) is a ground-based network of Fourier Transform Spectrometer (FTS) sites around the globe, where the column abundances of CO2, CH4, N2O, CO and O2 are measured. CO2 is constrained with a precision better than 0.25% (1-σ). To achieve a similarly high accuracy, calibration to World Meteorological Organization (WMO) standards is required. This paper introduces the first aircraft calibration campaign of five European TCCON sites and a mobile FTS instrument. A series of WMO standards in-situ profiles were obtained over European TCCON sites via aircraft and compared with retrievals of CO2 column amounts from the TCCON instruments. The results of the campaign show that the FTS measurements are consistently biased 1.1% ± 0.2% low with respect to WMO standards, in agreement with previous TCCON calibration campaigns. The standard a priori profile for the TCCON FTS retrievals is shown to not add a bias. The same calibration factor is generated using aircraft profiles as a priori and with the TCCON standard a priori. With a calibration to WMO standards, the highly precise TCCON CO2 measurements of total column concentrations provide a suitable database for the calibration and validation of nadir-viewing satellite

Calibration of TCCON column-averaged CO₂: the first aircraft campaign over European TCCON sites

The Total Carbon Column Observing Network (TCCON) is a ground-based network of Fourier Transform Spectrometer (FTS) sites around the globe, where the column abundances of CO₂, CH₄, N₂O, CO and O₂ are measured. CO₂ is constrained with a precision better than 0.25% (1-σ). To achieve a similarly high accuracy, calibration to World Meteorological Organization (WMO) standards is required. This paper introduces the first aircraft calibration campaign of five European TCCON sites and a mobile FTS instrument. A series of WMO standards in-situ profiles were obtained over European TCCON sites via aircraft and compared with retrievals of CO₂ column amounts from the TCCON instruments. The results of the campaign show that the FTS measurements are consistently biased 1.1% ± 0.2% low with respect to WMO standards, in agreement with previous TCCON calibration campaigns. The standard a priori profile for the TCCON FTS retrievals is shown to not add a bias. The same calibration factor is generated using aircraft profiles as a priori and with the TCCON standard a priori. With a calibration to WMO standards, the highly precise TCCON CO₂ measurements of total column concentrations provide a suitable database for the calibration and validation of nadir-viewing satellites

Retrieval and Validation of Carbon Dioxide, Methane, and Water Vapor for the Canary Islands IR-Laser Occultation Experiment

The first ground-based experiment to prove the concept of a novel space-based observation technique for microwave and infrared-laser occultation between low-Earthorbit satellites was performed in the Canary Islands between La Palma and Tenerife. For two nights from 21 to 22 July 2011 the experiment delivered the infrared-laser differential transmission principle for the measurement of greenhouse gases (GHGs) in the free atmosphere. Such global and long-term stable measurements of GHGs, accompanied also by measurements of thermodynamic parameters and line-of-sight wind in a self-calibrating way, have become very important for climate change monitoring. The experiment delivered promising initial data for demonstrating the new observation concept by retrieving volume mixing ratios of GHGs along a ~ 144 km signal path at altitudes of ~ 2.4 km. Here, we present a detailed analysis of the measurements, following a recent publication that introduced the experiment\u27s technical setup and first results for an example retrieval of CO2. We present the observational and validation data sets, the latter simultaneously measured at the transmitter and receiver sites; the measurement data handling; and the differential transmission retrieval procedure. We also determine the individual and combined uncertainties influencing the results and present the retrieval results for 12CO2, 13CO2, C18OO, H2O and CH4. The new method is found to have a reliable basis for monitoring of greenhouse gases such as CO2, CH4, and H2O in the free atmosphere

The CO2 record at the Amazon Tall Tower Observatory : A new opportunity to study processes on seasonal and inter-annual scales

High-quality atmospheric CO2 measurements are sparse in Amazonia, but can provide critical insights into the spatial and temporal variability of sources and sinks of CO2. In this study, we present the first 6 years (2014-2019) of continuous, high-precision measurements of atmospheric CO2 at the Amazon Tall Tower Observatory (ATTO, 2.1 degrees S, 58.9 degrees W). After subtracting the simulated background concentrations from our observational record, we define a CO2 regional signal (Delta CO2obs) that has a marked seasonal cycle with an amplitude of about 4 ppm. At both seasonal and inter-annual scales, we find differences in phase between Delta CO2obs and the local eddy covariance net ecosystem exchange (EC-NEE), which is interpreted as an indicator of a decoupling between local and non-local drivers of Delta CO2obs. In addition, we present how the 2015-2016 El Nino-induced drought was captured by our atmospheric record as a positive 2 sigma anomaly in both the wet and dry season of 2016. Furthermore, we analyzed the observed seasonal cycle and inter-annual variability of Delta CO2obs together with net ecosystem exchange (NEE) using a suite of modeled flux products representing biospheric and aquatic CO2 exchange. We use both non-optimized and optimized (i.e., resulting from atmospheric inverse modeling) NEE fluxes as input in an atmospheric transport model (STILT). The observed shape and amplitude of the seasonal cycle was captured neither by the simulations using the optimized fluxes nor by those using the diagnostic Vegetation and Photosynthesis Respiration Model (VPRM). We show that including the contribution of CO2 from river evasion improves the simulated shape (not the magnitude) of the seasonal cycle when using a data-driven non-optimized NEE product (FLUXCOM). The simulated contribution from river evasion was found to be 25% of the seasonal cycle amplitude. Our study demonstrates the importance of the ATTO record to better understand the Amazon carbon cycle at various spatial and temporal scales.Peer reviewe

Calibration of column-averaged CH4 over European TCCON FTS sites with airborne in-situ measurements

In September/October 2009, six European groundbased Fourier Transform Spectrometers (FTS) of the Total Carbon Column Observation Network (TCCON) were calibrated for the first time using aircraft measurements. The campaign was part of the Infrastructure for Measurement of the European Carbon Cycle (IMECC) project. During this campaign, altitude profiles of several trace gases and meteorological parameters were taken close to the FTS sites (typically within 1–2 km distance for flight altitudes below 5000 m). Profiles of CO2, CH4, CO and H2O were measured continuously. N2O, H2, and SF6 were later derived from flask measurements. The aircraft data had a vertical coverage ranging from approximately 300 to 13 000 m, corresponding to ~80% of the total atmospheric column seen by the FTS. This study summarizes the calibration results for CH4. The resulting calibration factor of 0.978±0.002 (±1 σ) from the IMECC campaign agreed very well with the results that Wunch et al. (2010) had derived for TCCON instruments in North America, Australia, New Zealand, and Japan using similar methods. By combining our results with the data of Wunch et al. (2010), the uncertainty of the calibration factor could be reduced by a factor of three (compared to using only IMECC or only Wunch et al. (2010) data). A careful analysis of the calibration method used by Wunch et al. (2010) revealed that the incomplete vertical coverage of the aircraft profiles can lead to a bias in the calibration factor. This bias can be compensated with a new iterative approach that we developed. Using this improved method, we derived a significantly lower calibration factor of 0.974±0.002 (±1 σ). This corresponds to a correction of all TCCON CH4 measurements by roughly −7 ppb

Satellite-inferred European carbon sink larger than expected

Current knowledge about the European terrestrial biospheric carbon sink, from the Atlantic to the Urals, relies upon bottom-up inventory and surface flux inverse model estimates (e.g. 0.27±0.16 GtC a−1 for 2000–2005 (Schulze et al., 2009), 0.17±0.44 GtC a−1 for 2001–2007 (Peters et al., 2010), 0.45±0.40 GtC a−1 for 2010 (Chevallier et al., 2014), 0.40±0.42 GtC a−1 for 2001–2004 (Peylin et al., 2013)). Inverse models assimilate in situ CO2 atmospheric concentrations measured by surface-based air sampling networks. The intrinsic sparseness of these networks is one reason for the relatively large flux uncertainties (Peters et al., 2010; Bruhwiler et al., 2011). Satellite-based CO2 measurements have the potential to reduce these uncertainties (Miller et al., 2007; Chevallier et al., 2007). Global inversion experiments using independent models and independent GOSAT satellite data products consistently derived a considerably larger European sink (1.0–1.3 GtC a−1 for 09/2009–08/2010 (Basu et al., 2013), 1.2–1.8 GtC a−1 in 2010 (Chevallier et al., 2014)). However, these results have been considered unrealistic due to potential retrieval biases and/or transport errors (Chevallier et al., 2014) or have not been discussed at all (Basu et al., 2013; Takagi et al., 2014). Our analysis comprises a regional inversion approach using STILT (Gerbig et al., 2003; Lin et al., 2003) short-range (days) particle dispersion modelling, rendering it insensitive to large-scale retrieval biases and less sensitive to long-range transport errors. We show that the satellite-derived European terrestrial carbon sink is indeed much larger (1.02±0.30 GtC a−1 in 2010) than previously expected. This is qualitatively consistent among an ensemble of five different inversion set-ups and five independent satellite retrievals (BESD (Reuter et al., 2011) 2003–2010, ACOS (O’Dell et al., 2012) 2010, UoL-FP (Cogan et al., 2012) 2010, RemoTeC (Butz et al., 2011) 2010, and NIES (Yoshida et al., 2013) 2010) using data from two different instruments (SCIAMACHY (Bovensmann et al., 1999) and GOSAT (Kuze et al., 2009)). The difference to in situ based inversions (Peylin et al., 2013), whilst large with respect to the mean reported European carbon sink (0.4 GtC a−1 for 2001–2004), is similar in magnitude to the reported uncertainty (0.42 GtC a−1). The highest gain in information is obtained during the growing season when satellite observation conditions are advantageous, a priori uncertainties are largest, and the surface sink maximises; during the dormant season, the results are dominated by the a priori. Our results provide evidence that the current understanding of the European carbon sink has to be revisited

Inverse modelling of European CH4 emissions during 2006-2012 using different inverse models and reassessed atmospheric observations

We present inverse modelling (top down) estimates of European methane (CH4) emissions for 2006-2012 based on a new quality-controlled and harmonised in situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions.The inverse models infer total CH4 emissions of 26.8 (20.2-29.7) TgCH(4) yr(-1) (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006-2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom up, based on statistical data and emissions factors) amount to only 21.3 TgCH(4) yr(-1) (2006) to 18.8 TgCH(4) yr(-1) (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP), total wetland emissions of 4.3 (2.3-8.2) TgCH(4) yr(-1) from the EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Taking into account the wetland emissions from the WETCHIMP ensemble, the top-down estimates are broadly consistent with the sum of anthropogenic and natural bottom-up inventories. However, the contribution of natural sources and their regional distribution remain rather uncertain.Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. The estimated average regional biases range between -40 and 20% at the aircraft profile sites in France, Hungary and Poland.</p