ALBERT

Description: Wind-induced waves play a key role in air–sea momentum and heat exchange. Fetch-limited shallow lakes differ significantly from open ocean circumstances since the wave field is characterized by young and growing waves that (i) are steeper and can collapse by white-capping at lower wind speeds, and (ii) travel with lower phase velocity. Consequently, momentum (and heat) flux estimation methods arising from oceanographic observations cannot be directly applied; however, few attempts have been made to describe air–water turbulent exchange in case of large, but still fetch-limited shallow lakes. Within a Croatian-Hungarian measurement campaign, turbulent flux measurements were performed in Lake Balaton. Momentum and heat fluxes were measured with eddy-covariance technique at an offshore station, while waves were simultaneously recorded with underwater acoustic surface tracking. Momentum fluxes were also recorded at two further stations closer to the shore. In this study, we analyze the measured wind stress and surface waves to reveal surface drag in case of highly fetch-limited conditions. We compare our results with relevant model formulations that attempt to estimate momentum flux using different wave state parameterizations (i.e. wave age and wave slope modified Charnock formulations) and show that derived drag and roughness length parameterizations differ significantly from oceanographic formulas.

Description: Multiple atmospheric properties were measured semi-continuously in the Budapest platform for Aerosol Research and Training laboratory, which represents the urban background for the time interval of 2008–2018. Data of 6 full measurement years during a decennial time interval were subjected to statistical time trend analyses by an advanced dynamic linear model and a generalized linear mixed model. The main interest in the analysed data set was on particle number concentrations in the diameter ranges from 6 to 1000 nm (N6−1000), from 6 to 100 nm (N6−100, ultrafine particles), from 25 to 100 nm (N25−100) and from 100 to 1000 nm (N100−1000). These data were supported by concentrations of SO2, CO, NO, NOx, O3, PM10 mass, as well as air temperature, relative humidity, wind speed, atmospheric pressure, global solar radiation, condensation sink, gas-phase H2SO4 proxy, classes of new aerosol particle formation (NPF), and growth events and meteorological macro-circulation patterns. The trend of the particle number concentrations derived as a change in the statistical properties of background state of the data set decreased in all size fractions over the years. Most particle number concentrations showed decreasing decennial statistical trends. The estimated annual mean decline of N6−1000 was (4–5) % during the 10-year measurement interval, which corresponds to a mean absolute change of −590 cm−3 in a year. This was interpreted as a consequence of the decreased anthropogenic emissions at least partly from road traffic alongside household heating and industry. Similar trends were not observed for the air pollutant gases. Diurnal statistical patterns of particle number concentrations showed tendentious variations, which were associated with a typical diurnal activity–time pattern of inhabitants in cities, particularly of vehicular road traffic. The trend patterns for NPF event days contained a huge peak from late morning to late afternoon, which is unambiguously caused by NPF and growth processes. These peaks were rather similar to each other in the position, shape and area on workdays and holidays, which implies that the dynamic and timing properties of NPF events are not substantially influenced by anthropogenic activities in central Budapest. The diurnal pattern for N25−100 exhibited the largest relative changes, which were related to particle emissions from high-temperature sources. The diurnal pattern for N100−1000 – which represents chemically and physically aged particles of larger spatial scale – were different from the diurnal patterns for the other size fractions.

Description: An intensive aerosol measurement and sample collection campaign was conducted in central Budapest in a mild winter for 2 weeks. The online instruments included an FDMS-TEOM, RT-OC/EC analyser, DMPS, gas pollutant analysers and meteorological sensors. The aerosol samples were collected on quartz fibre filters by a low-volume sampler using the tandem filter method. Elemental carbon (EC), organic carbon (OC), levoglucosan, mannosan, galactosan, arabitol and mannitol were determined, and radiocarbon analysis was performed on the aerosol samples. Median atmospheric concentrations of EC, OC and PM2.5 mass were 0.97, 4.9 and 25 µg m−3, respectively. The EC and organic matter (1.6  ×  OC) accounted for 4.8 and 37 %, respectively, of the PM2.5 mass. Fossil fuel (FF) combustion represented 36 % of the total carbon (TC  =  EC + OC) in the PM2.5 size fraction. Biomass burning (BB) was a major source (40 %) for the OC in the PM2.5 size fraction, and a substantial source (11 %) for the PM10 mass. We propose and apply here a novel, straightforward, coupled radiocarbon–levoglucosan marker method for source apportionment of the major carbonaceous chemical species. The contributions of EC and OC from FF combustion (ECFF and OCFF) to the TC were 11.0 and 25 %, respectively, EC and OC from BB (ECBB and OCBB) were responsible for 5.8 and 34 %, respectively, of the TC, while the OC from biogenic sources (OCBIO) made up 24 % of the TC. The overall relative uncertainty of the OCBIO and OCBB contributions was assessed to be up to 30 %, while the relative uncertainty for the other apportioned species is expected to be below 20 %. Evaluation of the apportioned atmospheric concentrations revealed some of their important properties and relationships among them. ECFF and OCFF were associated with different FF combustion sources. Most ECFF was emitted by vehicular road traffic, while the contribution of non-vehicular sources such as domestic and industrial heating or cooking using gas, oil or coal to OCFF was substantial. The mean contribution of BB to EC particles was smaller by a factor of approximately 2 than that of road traffic. The main formation processes of OCFF, OCBB and OCBIO from volatile organic compounds were jointly influenced by a common factor, which is most likely the atmospheric photochemistry, while primary organic emissions can also be important. Technological improvements and control measures for various BB appliances, together with efficient education and training of their users, in particular on the admissible fuel types, offer an important potential for improving the air quality in Budapest, and likely in other cities as well.

Description: Number concentrations of atmospheric aerosol particles were measured by a flow-switching type differential mobility particle sizer in an electrical mobility diameter range of 6–1000 nm in 30 channels near central Budapest with a time resolution of 10 min continuously from 3 November 2008 to 2 November 2009. Daily median number concentrations of particles varied from 3.8 × 103 to 29 ×103 cm−3 with a yearly median of 11.8 × 103 cm−3. Contribution of ultrafine particles to the total particle number ranged from 58 to 92% with a mean ratio and standard deviation of (79 ± 6)%. Typical diurnal variation of the particle number concentration was related to the major emission patterns in cities, new particle formation, sinks of particles and meteorology. Shapes of the monthly mean number size distributions were similar to each other. Overall mean for the number median mobility diameter of the Aitken and accumulation modes were 26 and 93 nm, respectively, which are substantially smaller than for rural or background environments. The Aitken and accumulation modes contributed similarly to the total particle number concentrations at the actual measurement location. New particle formation and growth unambiguously occurred on 83 days, which represent 27% of all relevant days. Hence, new particle formation and growth are not rare phenomena in Budapest. Their frequency showed an apparent seasonal variation with a minimum of 7.3% in winter and a maximum of 44% in spring. New particle formation events were linked to increased gas-phase H2SO4 concentrations. In the studied area, new particle formation is mainly affected by condensation sink and solar radiation. The formation process seems to be not sensitive to SO2, which was present in a yearly median concentration of 6.7 μg m−3. This suggests that the precursor gas was always available in excess. Formation rate of particles with a diameter of 6 nm varied between 1.65 and 12.5 cm−3 s−1 with a mean and standard deviation of (4.2 ± 2.5) cm−3 s−1. Seasonal dependency for the formation rate could not be identified. Growth curves of nucleated particles were usually superimposed on the characteristic diurnal pattern of road traffic direct emissions. The growth rate of the nucleation mode with a median diameter of 6 nm varied from 2.0 to 13.3 nm h−1 with a mean and standard deviation of (7.7 ± 2.4) nm h−1. There was an indicative tendency for larger growth rates in summer and for smaller values in winter. New particle formation events increased the total number concentration by a mean factor and standard deviation of 2.3 ± 1.1 relative to the concentration that occurred immediately before the event. Several indirect evidences suggest that the new particle formation events occurred at least over the whole city, and were of regional type. The results and conclusions presented are the first information of this kind for the region over one-year long time period.

Description: Sulfuric acid has been shown to be a key driver for new particle formation and subsequent growth in various environments, mainly due to its low volatility. However, direct measurements of gas-phase sulfuric acid are oftentimes not available, and the current sulfuric acid proxies cannot predict, for example, its nighttime concentrations or result in significant discrepancies with measured values. Here, we define the sources and sinks of sulfuric acid in different environments and derive a new physical proxy for sulfuric acid to be utilized in locations and during periods when it is not measured. We used H2SO4 measurements from four different locations: Hyytiälä, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment and heavily polluted megacity, respectively. The new proxy takes into account the formation of sulfuric acid from SO2 via OH oxidation and other oxidation pathways, specifically via stabilized Criegee intermediates. The sulfuric acid sinks included in the proxy are its condensation sink (CS) and atmospheric clustering starting from H2SO4 dimer formation. Indeed, we found that the observed sulfuric acid concentration can be explained by the proposed sources and sinks with similar coefficients in the four contrasting environments where we have tested it. Thus, the new proxy is a more flexible and an important improvement over previous proxies. Following the recommendations in this paper, a proxy for a specific location can be derived.

Description: After focusing on the changes in Hungarian temperature and preeipitation during this Century, possible hydrological, agricultural and ecological consequences of a future climate change are described. These results have been obtained using a modified version of empirical downscaling techniques, developed to analyse the local effects of global climate change in a twofold concentration of atmospheric greenhouse gases scenario. In addition, regional changes in temperature and precipitation were examined with the help of the more specific stochastic downscaling method. The climate of Hungary has become warmer and drier over the last Century. It is to be expected that an increasing concentration of atmospheric greenhouse gases will enhance the tendency towards aridification.

Description: The impact of atmospheric reactive nitrogen (Nr) deposition on carbon (C) sequestration in soils and biomass of unfertilised, 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., 2019) 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, as well as results of soil incubation experiments for N and greenhouse gas (GHG) emissions, 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 unfertilised 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. Nitrogen losses in the form of NO, N2O and especially NO3− were of the order of 10–20 % of Ndep at sites with Ndep  3 g (N) m−2 yr−1, indicating that perhaps one third of the sites were in a state of early to advanced N saturation. 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: Commonly, the micrometeorological parameters that underline the calculations of surface atmosphere exchange fluxes (e.g. friction velocity and sensible heat flux) and parameters used to model exchange fluxes with SVAT-type parameterisations (e.g. latent heat flux and canopy temperature) are measured with a single set of instrumentation and are analysed with a single methodology. This paper evaluates uncertainties in these measurements with a single instrument, by comparing the independent results from nine different institutes during the international GRAMINAE integrated field experiment over agricultural grassland near Braunschweig, Lower Saxony, Germany. The paper discusses uncertainties in measuring friction velocity, sensible and latent heat fluxes, canopy temperature and investigates the energy balance closure at this site. Although individual 15-min flux calculations show a large variability between the instruments, when averaged over the campaign, fluxes agree within 2% for momentum and 11% for sensible heat. However, the spread in estimates of latent heat flux (λE) is larger, with standard deviations of averages of 18%. While the dataset averaged over the different instruments fails to close the energy budget by 30%, if the largest turbulent fluxes are considered, near perfect energy closure can be achieved, suggesting that most techniques underestimate λE in particular. The uncertainty in λE feeds results in an uncertainty in the bulk stomatal resistance, which further adds to the uncertainties in the estimation of the canopy temperature that controls the exchange. The paper demonstrated how a consensus dataset was derived, which is used by the individual investigators to calculate fluxes and drive their models.

Description: During the GRAMINAE intensive field campaign between 20 May and 15 June 2000, ozone flux was measured and modelled above grassland in northern Germany, Braunschweig. Results of flux measurement and model calculations are presented in this study. Effects of agricultural activities (cut and fertilization) on ozone fluxes have also been analysed. A detailed deposition model for ozone is used to parameterise and to calculate the deposition velocity and flux of the ozone. Model calculations also provide an evaluation of the ratio of stomatal and non-stomatal fluxes. Measured and modelled flux and deposition velocity values have been compared for each period (before cut of grass, after cut, and after fertilization). Results show that agricultural activities hardly have any influence on total O3 fluxes, although both cutting and fertilization have complex impacts on different deposition pathways. Reduced vegetation decreased the stomatal exchange, while at the same time for this short canopy, the role of both soil emission of NO (promoting ozone loss close to the surface) and deposition of ozone to soil surface have increased. These effects demonstrate the importance of canopy structure and non-stomatal pathways on O3 fluxes.

Description: Improved data on biosphere-atmosphere exchange are fundamental to understanding the production and fate of ammonia (NH3) in the atmosphere. The GRAMINAE Integrated Experiment combined novel measurement and modelling approaches to provide the most comprehensive analysis of the interactions to date. Major inter-comparisons of micrometeorological parameters and NH3 flux measurements using the aerodynamic gradient method and relaxed eddy accumulation (REA) were conducted. These showed close agreement, though the REA systems proved insufficiently precise to investigate vertical flux divergence. Grassland management had a large effect on fluxes: Emissions increased after grass cutting (−50 to 700 ng m−2 s−1 NH3) and after N-fertilization (0 to 3800 ng m−2 s