ALBERT

Description: We estimated CO2, CH4, CO and N2O emission fluxes over the British Isles and Western Europe using atmospheric radon observations and concentrations recorded at the Mace Head Atmospheric Research Station between 1996 and 2005. We classified hourly concentration data into either long-range European or regional sources from Ireland and UK, by using local wind speed data in conjunction with 222Rn and 212Pb threshold criteria. This leads to the selection of about 7% of the total data for both sectors. We then used continuous 222Rn measurements and assumptions on the surface emissions of 222Rn to deduce the unknown fluxes of CO2, CH4, CO and N2O. Our results have been compared to the UNFCCC, EMEP and EDGAR statistical inventories and to inversion results for CH4. For Western Europe, we found yearly mean fluxes of 4.1±1.5 106 kg CO2 km−2 yr−1 , 11.9±2.0 103 kg CH4 km−2 yr−1, 12.8±4.2 103 kg CO km−2 yr−1 and 520.2±129.2 kg N2O km−2 yr−1, respectively, for CO2, CH4, CO and N2O over the period 1996–2005. The method based upon 222Rn to infer emissions has many sources of systematic errors, in particular its poorly known and variable footprint, uncertainties in 222Rn soil fluxes and in atmospheric mixing of air masses with background air. However, these biases are likely to remain constant in the long-term, which makes the method quite efficient to detect trends in fluxes. Over the last ten years period, the decrease of the anthropogenic CH4, CO and N2O emissions in Europe estimated by inventories (respectively −30%, −35% and −23%) is confirmed by the Mace Head data within 2%. Therefore, the 222Rn method provides an independent way of verification of changes in national emissions derived from inventories. Using European-wide estimates of the CO/CO2 emission ratio, we also found that it is possible to separate the fossil fuel CO2 emissions contribution from the one of total CO2 fluxes. The fossil fuel CO2 emissions and their trends derived in that manner agree very well with inventories.

Description: Three years of greenhouse gases measurements, obtained using a gas chromatograph (GC) system located at the Puy de Dôme station at 1465 m a.s.l. in Central France are presented. The GC system was installed in 2010 at Puy de Dôme and was designed for automatic and accurate semi-continuous measurements of atmospheric carbon dioxide, methane, nitrous oxide and sulfur hexafluoride mole fractions. We present in detail the instrumental set up and the calibration strategy, which together allow the GC to reach repeatabilities of 0.1 μmol mol−1, 1.2, 0.3 nmol mol−1 and 0.06 pmol mol−1 for CO2, CH4, N2O and SF6, respectively. Comparisons of the atmospheric time series with those obtained using other instruments shown that the GC system meets the World Meteorological Organization recommendations. The analysis of the three-year atmospheric time series revealed how the planetary boundary layer height drives the mole fractions observed at a mountain site such as Puy de Dôme where air masses alternate between the planetary boundary layer and the free troposphere. Accurate long-lived greenhouse gases measurements collocated with 222Rn measurements as an atmospheric tracer, allowed us to determine the CO2, CH4 and N2O emissions in the catchment area of the station. The derived CO2 surface flux revealed a clear seasonal cycle with net uptake by plant assimilation in the spring and net emission caused by the biosphere and burning of fossil fuel during the remainder of the year. We calculated a mean annual CO2 flux of 1150 t(CO2) km−2. The derived CH4 and N2O emissions in the station catchment area were 5.6 t(CH4) km−2 yr−1 and 1.5 t(N2O) km−2 yr−1, respectively. Our derived annual CH4 flux is in agreement with the national French inventory, whereas our derived N2O flux is five times larger than the same inventory.

Description: This study presents two methods for estimating methane emissions from a waste water treatment plant (WWTP) along with results from a measurement campaign at a WWTP in Valence, France. These methods, chamber measurements and tracer release, rely on Fourier Transform Infrared (FTIR) spectroscopy and Cavity Ring Down Spectroscopy (CRDS) instruments. We show that the tracer release method is suitable to quantify facility- and some process-scale emissions, while the chamber measurements, provide insight into individual process emissions. Uncertainties for the two methods are described and discussed. Applying the methods to CH4 emissions of the WWTP, we confirm that the open basins are not a major source of CH4 on the WWTP (about 10% of the total emissions), but that the pretreatment and sludge treatment are the main emitters. Overall, the waste water treatment plant represents a small part (about 1.5%) of the methane emissions of the city of Valence and its surroundings, which is lower than the national inventories.

Description: This study compares actual evapotranspiration (ETa) measurements by a set of six weighable lysimeters, ETa estimates obtained with the eddy covariance (EC) method, and evapotranspiration calculated with the full-form Penman–Monteith equation (ETPM) for the Rollesbroich site in the Eifel (western Germany). The comparison of ETa measured by EC (including correction of the energy balance deficit) and by lysimeters is rarely reported in the literature and allows more insight into the performance of both methods. An evaluation of ETa for the two methods for the year 2012 shows a good agreement with a total difference of 3.8% (19 mm) between the ETa estimates. The highest agreement and smallest relative differences (〈 8%) on a monthly basis between both methods are found in summer. ETa was close to ETPM, indicating that ET was energy limited and not limited by water availability. ETa differences between lysimeter and EC were mainly related to differences in grass height caused by harvest and the EC footprint. The lysimeter data were also used to estimate precipitation amounts in combination with a filter algorithm for the high-precision lysimeters recently introduced by Peters et al. (2014). The estimated precipitation amounts from the lysimeter data differ significantly from precipitation amounts recorded with a standard rain gauge at the Rollesbroich test site. For the complete year 2012 the lysimeter records show a 16 % higher precipitation amount than the tipping bucket. After a correction of the tipping bucket measurements by the method of Richter (1995) this amount was reduced to 3%. With the help of an on-site camera the precipitation measurements of the lysimeters were analyzed in more detail. It was found that the lysimeters record more precipitation than the tipping bucket, in part related to the detection of rime and dew, which contribute 17% to the yearly difference between both methods. In addition, fog and drizzle explain an additional 5.5% of the total difference. Larger differences are also recorded for snow and sleet situations. During snowfall, the tipping bucket device underestimated precipitation severely, and these situations contributed also 7.9% to the total difference. However, 36% of the total yearly difference was associated with snow cover without apparent snowfall, and under these conditions snow bridges and snow drift seem to explain the strong overestimation of precipitation by the lysimeter. The remaining precipitation difference (about 33%) could not be explained and did not show a clear relation to wind speed. The variation of the individual lysimeters devices compared to the lysimeter mean are small, showing variations up to 3% for precipitation and 8% for evapotranspiration.

Description: 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.

Description: We evaluate the capability of the global atmospheric transport model TM5 to simulate the boundary layer dynamics and associated variability of trace gases close to the surface, using radon (222Rn). Focusing on the European scale, we compare the boundary layer height (BLH) in the TM5 model with observations from the National Oceanic and Atmospheric Admnistration (NOAA) Integrated Global Radiosonde Archive (IGRA) and also with ceilometer and lidar (light detection and ranging) BLH retrievals at two stations. Furthermore, we compare TM5 simulations of 222Rn activity concentrations, using a novel, process-based 222Rn flux map over Europe (Karstens et al., 2015), with harmonised 222Rn measurements at 10 stations. The TM5 model reproduces relatively well the daytime BLH (within 10–20 % for most of the stations), except for coastal sites, for which differences are usually larger due to model representation errors. During night, however, TM5 overestimates the shallow nocturnal BLHs, especially for the very low observed BLHs (

Description: In recent decades, the central North Sea has been experiencing a general trend of decreasing dissolved oxygen (O2) levels during summer. To understand the potential causes driving lower O2, we investigated summertime turbulence and O2 dynamics in the thermocline and bottom boundary layer (BBL). The study focuses on coupling biogeochemical processes with physical transport processes to identify key drivers of the O2 and organic carbon turnover within the BBL. Combining our flux observations with an analytical process-oriented approach, we resolve the key drivers that ultimately determine the BBL O2 levels. We report substantial tidally-driven turbulent O2 fluxes from the thermocline into the otherwise isolated bottom water. This contribution to the local bottom water O2 and carbon budgets has been largely overlooked and might be a central factor maintaining relatively high O2 levels in the bottom water throughout the stratification period. With the current climate warming projections, we propose that higher water temperature and reduced turbulence could favour migrating algal species that could out-compete other species for light and nutrients, and shift the oxygen production zone higher up within the thermocline while maintaining similar organic carbon export to the bottom water. Due to the substantially lower turbulence levels in the central region of the thermocline as compared to the higher turbulence observed at the thermocline-BBL interface, such a shift in the production layer could lead to further isolation of the bottom water and promote the seasonal occurrence of lower O2 concentrations.

Description: The carbon (C) cycle in boreal regions is strongly influenced by fire, which converts biomass and detrital C mainly to gaseous forms (CO2 and smaller proportions of CO and CH4), and some 1–7% of mass to pyrogenic C (PyC). PyC is mainly produced as solid charred residues, including visually-defined charcoal, and a black carbon (BC) fraction chemically defined by its resistance to laboratory oxidation, plus much lower proportions of volatile soot and polycyclic aromatic hydrocarbons (PAHs). All PyC is characterized by fused aromatic rings, but varying in cluster sizes, and presence of other elements (N, O) and functional groups. There are several reasons for current interest in defining more precisely the role of PyC in the C cycle of boreal regions. First, PyC is resistant to decomposition, and therefore contributes to very stable C pools in soils and sediments. Second, it influences soil processes, mainly through its sorption properties and cation exchange capacity, and third, soot aerosols absorb solar radiation and may contribute to global warming. However, there are large gaps in the basic information needed to address these topics. While charcoal is commonly defined by visual criteria, analytical methods for BC are mainly based on various measures of oxidation resistance, or on yield of benzenepolycarboxylic acids. These methods are still being developed, and capture different fractions of the PyC "continuum". There are few quantitative reports of PyC production and stocks in boreal forests (essentially none for boreal peatlands), and results are difficult to compare due to varying experimental goals and methods, as well as inconsistent terminology. There are almost no direct field measurements of BC aerosol production from boreal wildfires, and little direct information on rates and mechanisms for PyC loss. Structural characterization of charred biomass and forest floor from wildfires generally indicates a low level of thermal alteration, with the bulk of the material having H/C ratios still 〉0.2, and small aromatic cluster sizes. For the more chemically-recalcitrant BC fraction, a variety of mainly circumstantial evidence suggests very slow decomposition, with turnover on a millennium timescale (5000–10 000 y), depending on environmental conditions and PyC properties, but the main limitation to PyC storage in soil is likely consumption by subsequent fires. Degraded, functionalized PyC is also incorporated into humified soil organic matter, and is transported to sediments in dissolved and particulate form. Boreal production is estimated as 7–17 Tg BC y−1 of solid residues and 2–2.5 Tg BC y−1 as aerosols. Primary research needs include basic field data on PyC production and stocks in boreal forests and peatlands, suitable to support C budget modeling, and development of standardized analytical methods and of improved approaches to assess the chemical recalcitrance of typical chars from boreal wildfires. To accomplish these goals effectively will require much greater emphasis on interdisciplinary cooperation.