Atmospheric transport and chemistry of trace gases in LMDz5B: evaluation and implications for inverse modelling

Representation of atmospheric transport is a major source of error in the estimation of greenhouse gas sources and sinks by inverse modelling. Here we assess the impact on trace gas mole fractions of the new physical parameterizations recently implemented in the atmospheric global climate model LMDz to improve vertical diffusion, mesoscale mixing by thermal plumes in the planetary boundary layer (PBL), and deep convection in the troposphere. At the same time, the horizontal and vertical resolution of the model used in the inverse system has been increased. The aim of this paper is to evaluate the impact of these developments on the representation of trace gas transport and chemistry, and to anticipate the implications for inversions of greenhouse gas emissions using such an updated model. Comparison of a one-dimensional version of LMDz with large eddy simulations shows that the thermal scheme simulates shallow convective tracer transport in the PBL over land very efficiently, and much better than previous versions of the model. This result is confirmed in three-dimensional simulations, by a much improved reproduction of the radon-222 diurnal cycle. However, the enhanced dynamics of tracer concentrations induces a stronger sensitivity of the new LMDz configuration to external meteorological forcings. At larger scales, the inter-hemispheric exchange is slightly slower when using the new version of the model, bringing them closer to observations. The increase in the vertical resolution (from 19 to 39 layers) significantly improves the representation of stratosphere/troposphere exchange. Furthermore, changes in atmospheric thermodynamic variables, such as temperature, due to changes in the PBL mixing modify chemical reaction rates, which perturb chemical equilibriums of reactive trace gases. One implication of LMDz model developments for future inversions of greenhouse gas emissions is the ability of the updated system to assimilate a larger amount of high-frequency data sampled at high-variability stations. Others implications are discussed at the end of the paper

Sea-air CO2 fluxes in the Indian Ocean between 1990 and 2009

The Indian Ocean (44 S-30 N) plays an important role in the global carbon cycle, yet it remains one of the most poorly sampled ocean regions. Several approaches have been used to estimate net sea-air CO2 fluxes in this region: interpolated observations, ocean biogeochemical models, atmospheric and ocean inversions. As part of the RECCAP (REgional Carbon Cycle Assessment and Processes) project, we combine these different approaches to quantify and assess the magnitude and variability in Indian Ocean sea-air CO2 fluxes between 1990 and 2009. Using all of the models and inversions, the median annual mean sea-air CO2 uptake of −0.37 ± 0.06 PgC yr -1 is consistent with the −0.24 ± 0.12 PgC yr -1 calculated from observations. The fluxes from the southern Indian Ocean (18-44 S; -0.43 ± 0.07 PgC yr-1 are similar in magnitude to the annual uptake for the entire Indian Ocean. All models capture the observed pattern of fluxes in the Indian Ocean with the following exceptions: underestimation of upwelling fluxes in the northwestern region (off Oman and Somalia), overestimation in the northeastern region (Bay of Bengal) and underestimation of the CO2 sink in the subtropical convergence zone. These differences were mainly driven by lack of atmospheric CO2 data in atmospheric inversions, and poor simulation of monsoonal currents and freshwater discharge in ocean biogeochemical models. Overall, the models and inversions do capture the phase of the observed seasonality for the entire Indian Ocean but overestimate the magnitude. The predicted sea-air CO 2 fluxes by ocean biogeochemical models (OBGMs) respond to seasonal variability with strong phase lags with reference to climatological CO 2 flux, whereas the atmospheric inversions predicted an order of magnitude higher seasonal flux than OBGMs. The simulated interannual variability by the OBGMs is weaker than that found by atmospheric inversions. Prediction of such weak interannual variability in CO2 fluxes by atmospheric inversions was mainly caused by a lack of atmospheric data in the Indian Ocean. The OBGM models suggest a small strengthening of the sink over the period 1990-2009 of -0.01 PgC decade-1. This is inconsistent with the observations in the southwestern Indian Ocean that shows the growth rate of oceanic pCO 2 was faster than the observed atmospheric CO2 growth, a finding attributed to the trend of the Southern Annular Mode (SAM) during the 1990s

A new estimation of the recent tropospheric molecular hydrogen budget using atmospheric observations and variational inversion

This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and European surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, then deposition velocity and surface emissions and finally, deposition velocity, biomass burning, anthropogenic and N2 fixation-related emissions were simultaneously inverted in several scenarios. These scenarios have focused on the sensibility of the soil uptake value to different spatio-temporal distributions. The range of variations of these diverse inversion sets generate an estimate of the uncertainty for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between −8 and +8 Tg yr−1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on bottom-up and top-down estimations. Our estimate of global H2 soil uptake is −59±9 Tg yr−1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions within the range of their respective uncertainties. Additional constraints, such as isotopic measurements would be needed to infer a more robust partition of H2 sources and sinks

Analysis of the potential of near-ground measurements of CO2 and CH4 in London, UK, for the monitoring of city-scale emissions using an atmospheric transport model

Carbon dioxide (CO2) and methane (CH4) mole fractions were measured at four near-ground sites located in and around London during the summer of 2012 with a view to investigating the potential of assimilating such measurements in an atmospheric inversion system for the monitoring of the CO2 and CH4 emissions in the London area. These data were analysed and compared with simulations using a modelling framework suited to building an inversion system: a 2 km horizontal resolution south of England configuration of the transport model CHIMERE driven by European Centre for Medium-Range Weather Forecasts (ECMWF) meteorological forcing, coupled to a 1 km horizontal resolution emission inventory (the UK National Atmospheric Emission Inventory). First comparisons reveal that local sources, which cannot be represented in the model at a 2 km resolution, have a large impact on measurements. We evaluate methods to filter out the impact of some of the other critical sources of discrepancies between the measurements and the model simulation except that of the errors in the emission inventory, which we attempt to isolate. Such a separation of the impact of errors in the emission inventory should make it easier to identify the corrections that should be applied to the inventory. Analysis is supported by observations from meteorological sites around the city and a 3-week period of atmospheric mixing layer height estimations from lidar measurements. The difficulties of modelling the mixing layer depth and thus CO2 and CH4 concentrations during the night, morning and late afternoon lead to focusing on the afternoon period for all further analyses. The discrepancies between observations and model simulations are high for both CO2 and CH4 (i.e. their root mean square (RMS) is between 8 and 12 parts per million (ppm) for CO2 and between 30 and 55 parts per billion (ppb) for CH4 at a given site). By analysing the gradients between the urban sites and a suburban or rural reference site, we are able to decrease the impact of uncertainties in the fluxes and transport outside the London area and in the model domain boundary conditions. We are thus able to better focus attention on the signature of London urban CO2 and CH4 emissions in the atmospheric CO2 and CH4 concentrations. This considerably improves the statistical agreement between the model and observations for CO2 (with model–data RMS discrepancies that are between 3 and 7 ppm) and to a lesser degree for CH4 (with model–data RMS discrepancies that are between 29 and 38 ppb). Between one of the urban sites and either the rural or suburban reference site, selecting the gradients during periods wherein the reference site is upwind of the urban site further decreases the statistics of the discrepancies in general, though not systematically. In a further attempt to focus on the signature of the city anthropogenic emission in the mole fraction measurements, we use a theoretical ratio of gradients of carbon monoxide (CO) to gradients of CO2 from fossil fuel emissions in the London area to diagnose observation-based fossil fuel CO2 gradients, and compare them with the fossil fuel CO2 gradients simulated with CHIMERE. This estimate increases the consistency between the model and the measurements when considering only one of the two urban sites, even though the two sites are relatively close to each other within the city. While this study evaluates and highlights the merit of different approaches for increasing the consistency between the mesoscale model and the near-ground data, and while it manages to decrease the random component of the analysed model–data discrepancies to an extent that should not be prohibitive to extracting the signal from the London urban emissions, large biases, the sign of which depends on the measurement sites, remain in the final model–data discrepancies. Such biases are likely related to local emissions to which the urban near-ground sites are highly sensitive. This questions our current ability to exploit urban near-ground data for the atmospheric inversion of city emissions based on models at spatial resolution coarser than 2 km. Several measurement and modelling concepts are discussed to overcome this challenge

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

Mesoscale modelling of the CO2 interactions between the surface and the atmosphere applied to the April 2007 CERES field experiment

This paper describes a numerical interpretation of the April 2007, CarboEurope Regional Experiment Strategy (CERES) campaign, devoted to the study of the CO2 cycle at the regional scale. Four consecutive clear sky days with intensive observations of CO2 concentration, fluxes at the surface and in the boundary layer have been simulated with the Meso-NH mesoscale model, coupled to ISBA-A-gs land surface model. The main result of this paper is to show how aircraft observations of CO2 concentration have been used to identify surface model errors and to calibrate the CO2 driving component of the surface model. In fact, the comparisons between modelled and observed CO2 concentrations within the Atmospheric Boundary Layer (ABL) allow to calibrate and correct not only the parameterization of respired CO2 fluxes by the ecosystem but also the Leaf Area Index (LAI) of the dominating land cover. After this calibration, the paper describes systematic comparisons of the model outputs with numerous data collected during the CERES campaign, in April 2007. For instance, the originality of this paper is the spatial integration of the comparisons. In fact, the aircraft observations of CO2 concentration and fluxes and energy fluxes are used for the model validation from the local to the regional scale. As a conclusion, the CO2 budgeting approach from the mesoscale model shows that the winter croplands are assimilating more CO2 than the pine forest, at this stage of the year and this case study

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