ALBERT

Description: Direct measurements of the net ecosystem exchange (NEE) of gaseous elemental mercury (Hg0) are important to improve our understanding of global Hg cycling and, ultimately, human and wildlife Hg exposure. The lack of long-term, ecosystem-scale measurements causes large uncertainties in Hg0 flux estimates. It currently remains unclear whether terrestrial ecosystems are net sinks or sources of atmospheric Hg0. Here, we show a detailed validation of direct Hg0 flux measurements based on the eddy covariance technique (Eddy Mercury) using a Lumex RA-915 AM mercury monitor. The flux detection limit derived from a zero-flux experiment in the laboratory was 0.22 ng m−2 h−1 (maximum) with a 50 % cutoff at 0.074 ng m−2 h−1. We present eddy covariance NEE measurements of Hg0 over a low-Hg soil (41–75 ng Hg g−1 in the topsoil, referring to a depth of 0–10 cm), conducted in summer 2018 at a managed grassland at the Swiss FluxNet site in Chamau, Switzerland (CH-Cha). The statistical estimate of the Hg0 flux detection limit under outdoor conditions at the site was 5.9 ng m−2 h−1 (50 % cutoff). We measured a net summertime emission over a period of 34 d with a median Hg0 flux of 2.5 ng m−2 h−1 (with a −0.6 to 7.4 ng m−2 h−1 range between the 25th and 75th percentiles). We observed a distinct diel cycle with higher median daytime fluxes (8.4 ng m−2 h−1) than nighttime fluxes (1.0 ng m−2 h−1). Drought stress during the measurement campaign in summer 2018 induced partial stomata closure of vegetation. Partial stomata closure led to a midday depression in CO2 uptake, which did not recover during the afternoon. The median CO2 flux was only 24 % of the median CO2 flux measured during the same period in the previous year (2017). We suggest that partial stomata closure also dampened Hg0 uptake by vegetation, resulting in a NEE of Hg0 that was dominated by soil emission. Finally, we provide suggestions to further improve the precision and handling of the “Eddy Mercury” system in order to assure its suitability for long-term NEE measurements of Hg0 over natural background surfaces with low soil Hg concentrations (

Description: The TGS 2600 was the first low-cost solid-state sensor that shows a response to ambient levels of CH4 (e.g., range ≈1.8–2.7 µmol mol−1). Here we present an empirical function to correct the TGS 2600 signal for temperature and (absolute) humidity effects and address the long-term reliability of two identical sensors deployed from 2012 to 2018. We assess the performance of the sensors at 30 min resolution and aggregated to weekly medians. Over the entire period the agreement between TGS-derived and reference CH4 mole fractions measured by a high-precision Los Gatos Research instrument was R2=0.42, with better results during summer (R2=0.65 in summer 2012). Using absolute instead of relative humidity for the correction of the TGS 2600 sensor signals reduced the typical deviation from the reference to less than ±0.1 µmol mol−1 over the full range of temperatures from −41 to 27 ∘C. At weekly resolution the two sensors showed a downward drift of signal voltages indicating that after 10–13 years a TGS 2600 may have reached its end of life. While the true trend in CH4 mole fractions measured by the high-quality reference instrument was 10.1 nmolmol-1yr-1 (2012–2018), part of the downward trend in sensor signal (ca. 40 %–60 %) may be due to the increase in CH4 mole fraction because the sensor voltage decreases with increasing CH4 mole fraction. Weekly median diel cycles tend to agree surprisingly well between the TGS 2600 and reference measurements during the snow-free season, but in winter the agreement is lower. We suggest developing separate functions for deducing CH4 mole fractions from TGS 2600 measurements under cold and warm conditions. We conclude that the TGS 2600 sensor can provide data of research-grade quality if it is adequately calibrated and placed in a suitable environment where cross-sensitivities to gases other than CH4 are of no concern.

Description: The effects of atmospheric nitrogen deposition (Ndep) on carbon (C) sequestration in forests have often been assessed by relating differences in productivity to spatial variations of Ndep across a large geographic domain. These correlations generally suffer from covariation of other confounding variables related to climate and other growth-limiting factors, as well as large uncertainties in total (dry + wet) reactive nitrogen (Nr) deposition. We propose a methodology for untangling the effects of Ndep from those of meteorological variables, soil water retention capacity and stand age, using a mechanistic forest growth model in combination with eddy covariance CO2 exchange fluxes from a Europe-wide network of 22 forest flux towers. Total Nr deposition rates were estimated from local measurements as far as possible. The forest data were compared with data from natural or semi-natural, non-woody vegetation sites. The response of forest net ecosystem productivity to nitrogen deposition (dNEP ∕ dNdep) was estimated after accounting for the effects on gross primary productivity (GPP) of the co-correlates by means of a meta-modelling standardization procedure, which resulted in a reduction by a factor of about 2 of the uncorrected, apparent dGPP ∕ dNdep value. This model-enhanced analysis of the C and Ndep flux observations at the scale of the European network suggests a mean overall dNEP ∕ dNdep response of forest lifetime C sequestration to Ndep of the order of 40–50 g C per g N, which is slightly larger but not significantly different from the range of estimates published in the most recent reviews. Importantly, patterns of gross primary and net ecosystem productivity versus Ndep were non-linear, with no further growth responses at high Ndep levels (Ndep 〉 2.5–3 g N m−2 yr−1) but accompanied by increasingly large ecosystem N losses by leaching and gaseous emissions. The reduced increase in productivity per unit N deposited at high Ndep levels implies that the forecast increased Nr emissions and increased Ndep levels in large areas of Asia may not positively impact the continent's forest CO2 sink. The large level of unexplained variability in observed carbon sequestration efficiency (CSE) across sites further adds to the uncertainty in the dC∕dN response.

Description: The impact of atmospheric reactive nitrogen (Nr) deposition on carbon (C) sequestration in soils and biomass of unfertilized, natural, semi-natural and forest ecosystems has been much debated. Many previous results of this dC∕dN response were based on changes in carbon stocks from periodical soil and ecosystem inventories, associated with estimates of Nr deposition obtained from large-scale chemical transport models. This study and a companion paper (Flechard et al., 2020) strive to reduce uncertainties of N effects on C sequestration by linking multi-annual gross and net ecosystem productivity estimates from 40 eddy covariance flux towers across Europe to local measurement-based estimates of dry and wet Nr deposition from a dedicated collocated monitoring network. To identify possible ecological drivers and processes affecting the interplay between C and Nr inputs and losses, these data were also combined with in situ flux measurements of NO, N2O and CH4 fluxes; soil NO3- leaching sampling; and results of soil incubation experiments for N and greenhouse gas (GHG) emissions, as well as surveys of available data from online databases and from the literature, together with forest ecosystem (BASFOR) modelling. Multi-year averages of net ecosystem productivity (NEP) in forests ranged from −70 to 826 g C m−2 yr−1 at total wet + dry inorganic Nr deposition rates (Ndep) of 0.3 to 4.3 g N m−2 yr−1 and from −4 to 361 g C m−2 yr−1 at Ndep rates of 0.1 to 3.1 g N m−2 yr−1 in short semi-natural vegetation (moorlands, wetlands and unfertilized extensively managed grasslands). The GHG budgets of the forests were strongly dominated by CO2 exchange, while CH4 and N2O exchange comprised a larger proportion of the GHG balance in short semi-natural vegetation. Uncertainties in elemental budgets were much larger for nitrogen than carbon, especially at sites with elevated Ndep where Nr leaching losses were also very large, and compounded by the lack of reliable data on organic nitrogen and N2 losses by denitrification. Nitrogen losses in the form of NO, N2O and especially NO3- were on average 27 % (range 6 %–54 %) of Ndep at sites with Ndep  3 g N m−2 yr−1. Such large levels of Nr loss likely indicate that different stages of N saturation occurred at a number of sites. The joint analysis of the C and N budgets provided further hints that N saturation could be detected in altered patterns of forest growth. Net ecosystem productivity increased with Nr deposition up to 2–2.5 g N m−2 yr−1, with large scatter associated with a wide range in carbon sequestration efficiency (CSE, defined as the NEP ∕ GPP ratio). At elevated Ndep levels (〉 2.5 g N m−2 yr−1), where inorganic Nr losses were also increasingly large, NEP levelled off and then decreased. The apparent increase in NEP at low to intermediate Ndep levels was partly the result of geographical cross-correlations between Ndep and climate, indicating that the actual mean dC∕dN response at individual sites was significantly lower than would be suggested by a simple, straightforward regression of NEP vs. Ndep.

Description: A 5-year greenhouse gas (GHG) exchange study of the three major gas species (CO2, CH4 and N2O) from an intensively managed permanent grassland in Switzerland is presented. Measurements comprise 2 years (2010 and 2011) of manual static chamber measurements of CH4 and N2O, 5 years of continuous eddy covariance (EC) measurements (CO2–H2O – 2010–2014), and 3 years (2012–2014) of EC measurement of CH4 and N2O. Intensive grassland management included both regular and sporadic management activities. Regular management practices encompassed mowing (three to five cuts per year) with subsequent organic fertilizer amendments and occasional grazing, whereas sporadic management activities comprised grazing or similar activities. The primary objective of our measurements was to compare pre-plowing to post-plowing GHG exchange and to identify potential memory effects of such a substantial disturbance on GHG exchange and carbon (C) and nitrogen (N) gains and losses. In order to include measurements carried out with different observation techniques, we tested two different measurement techniques jointly in 2013, namely the manual static chamber approach and the eddy covariance technique for N2O, to quantify the GHG exchange from the observed grassland site. Our results showed that there were no memory effects on N2O and CH4 emissions after plowing, whereas the CO2 uptake of the site considerably increased when compared to pre-restoration years. In detail, we observed large losses of CO2 and N2O during the year of restoration. In contrast, the grassland acted as a carbon sink under usual management, i.e., the time periods 2010–2011 and 2013–2014. Enhanced emissions and emission peaks of N2O (defined as exceeding background emissions 0.21 ± 0.55 nmol m−2 s−1 (SE = 0.02) for at least 2 sequential days and the 7 d moving average exceeding background emissions) were observed for almost 7 continuous months after restoration as well as following organic fertilizer applications during all years. Net ecosystem exchange of CO2 (NEECO2) showed a common pattern of increased uptake of CO2 in spring and reduced uptake in late fall. NEECO2 dropped to zero and became positive after each harvest event. Methane (CH4) exchange fluctuated around zero during all years. Overall, CH4 exchange was of negligible importance for both the GHG budget and the carbon budget of the site. Our results stress the inclusion of grassland restoration events when providing cumulative sums of C sequestration potential and/or global warming potential (GWP). Consequently, this study further highlights the need for continuous long-term GHG exchange observations as well as for the implementation of our findings into biogeochemical process models to track potential GHG mitigation objectives as well as to predict future GHG emission scenarios reliably.