Continuous atmospheric in-situ measurements of the CH4/CO ratio at the Mt. Cimone station (Italy, 2165 m a.s.l.) and their possible use for estimating regional CH4 emissions.

Methane (CH4) is an important climate forcer, contributing about 17% of the total radiative forcing by long living greenhouse gases. The Po basin is one of the most polluted and densely populated areas in Europe representing an important source region for CH4. The aim of this work was to test an inter-species correlation approach to derive estimates of anthropogenic CH4 emissions for the period 2015-2019 from the Po basin by combining CO bottom-up inventory data and continuous CH4 and CO observations from a mountain site in the northern Italy. The tested methodology suggested lower emissions in respect to EDGAR (-17%) and the Italian National Inventory (-40%) for the Po basin. However, despite the two bottom-up inventories, the emissions derived from the atmospheric observations reported an increasing tendency from 2015 to 2019 for the CH4 emissions. A sensitivity study revealed that using different subsets of the atmospheric observations implied a difference of 26% in the CH4 emission estimates. The highest agreement with two bottom-up CH4 inventories (EDGAR and the Italian national inventory) were obtained when atmospheric data were strictly selected for periods representative of air mass transport from the Po basin. Our study identified various challenges when using this methodology as a benchmark to verify bottom-up CH4 inventories. Issues could be attributed to the annual aggregation of the proxies used to derive the emission amounts, to the CO bottom-up inventory used as input information and to the relatively high sensitivity of the results to the different subsets of the atmospheric observations. However, the use of different bottom-up inventories as input data for CO emissions can potentially provide information that should be carefully considered for the purpose of integrating CH4 bottom-up inventories.

Surface ozone trends at El Arenosillo observatory from a new perspective.

Surface ozone trends observed at El Arenosillo observatory for the last 22 years (2000-2021) were investigated. The trends for daily averages and daily 5th and 95th percentiles were 1.2 ± 0.3 ppb decade-1, 2.2 ± 0.3 ppb decade-1 and -0.03 ± 0.43 ppb decade-1, respectively, thus showing a significant increase of background ozone. The surface temperature trends were also explored, obtaining trends of 0.5 ± 0.2 °C decade-1, 1.1 ± 0.2 °C decade-1 and -0.3 ± 0.2 °C decade-1 for daily averages, 5th and 95th percentiles, respectively. To identify potential changes in the ozone drivers, the weather pattern shifts were analyzed through the horizontal distribution trends of temperature at 2 m and geopotential height at 850 hPa. A strengthening of the Azores anticyclone and a regional warming were detected, which could contribute to the ozone trends obtained. The surface ozone trend in every month was explored, identifying a monthly pattern, with remarkable opposite trends in December-January (2.4 ± 0.9 ppb decade-1) vs July-August (-0.5 ± 1.1 ppb decade-1). The surface ozone trends for every hour of the day were also explored, identifying two clear patterns. The first pattern occurred from spring to autumn and was characterized by a behavior opposite to the typical daily ozone cycle. The second pattern was observed in winter, and it shows two relative peaks in the ozone trends (around 13:00 and 19:00 UTC). In a context of ozone precursor's depletion, changes in the weather conditions and warmer climate, to improve our knowledge of the ozone trends, we suggest exploring them based on daily and hourly averages.

The fingerprint of the 2018 drought in Europe on ground-based atmospheric CO2 measurements.

During the summer of 2018, a widespread drought developed over Northern and Central Europe. The increase in temperature and the reduction of soil moisture have influenced carbon dioxide (CO2) exchange between the atmosphere and terrestrial ecosystems in various ways, such as a reduction of photosynthesis, changes in ecosystem respiration, or allowing more frequent fires. In this study, we characterize the resulting perturbation of the atmospheric CO2 seasonal cycles. 2018 has a good coverage of European regions affected by drought, allowing the investigation of how ecosystem flux anomalies impacted spatial CO2 gradients between stations. This density of stations is unprecedented compared to previous drought events in 2003 and 2015, particularly thanks to the deployment of the Integrated Carbon Observation System (ICOS) network of atmospheric greenhouse gas monitoring stations in recent years. Seasonal CO2 cycles from 48 European stations were available for 2017 and 2018. Earlier data were retrieved for comparison from international databases or national networks. Here, we show that the usual summer minimum in CO2 due to the surface carbon uptake was reduced by 1.4 ppm in 2018 for the 10 stations located in the area most affected by the temperature anomaly, mostly in Northern Europe. Notwithstanding, the CO2 transition phases before and after July were slower in 2018 compared to 2017, suggesting an extension of the growing season, with either continued CO2 uptake by photosynthesis and/or a reduction in respiration driven by the depletion of substrate for respiration inherited from the previous months due to the drought. For stations with sufficiently long time series, the CO2 anomaly observed in 2018 was compared to previous European droughts in 2003 and 2015. Considering the areas most affected by the temperature anomalies, we found a higher CO2 anomaly in 2003 (+3 ppm averaged over 4 sites), and a smaller anomaly in 2015 (+1 ppm averaged over 11 sites) compared to 2018. This article is part of the theme issue 'Impacts of the 2018 severe drought and heatwave in Europe: from site to continental scale'.

Seasonal variability of PM2.5 and PM10 composition and sources in an urban background site in Southern Italy.

Comparison of fine and coarse fractions in terms of sources and dynamics is scarce in southeast Mediterranean countries; differences are relevant because of the importance of natural sources like sea spray and Saharan dust advection, because most of the monitoring networks are limited to PM10. In this work, the main seasonal variabilities of sources and processes involving fine and coarse PM (particulate matter) were studied at the Environmental-Climate Observatory of Lecce (Southern Italy). Simultaneous PM2.5 and PM10 samples were collected between July 2013 and July 2014 and chemically analysed to determine concentrations of several species: OC (organic carbon) and EC (elemental carbon) via thermo-optical analysis, 9 major ions via IC, and 23 metals via ICP-MS. Data was processed through mass closure analysis and Positive Matrix Factorization (PMF) receptor model characterizing seasonal variabilities of nine sources contributions. Organic and inorganic secondary aerosol accounts for 43% of PM2.5 and 12% of PM2.5-10 with small seasonal changes. SIA (secondary inorganic aerosol) seasonal pattern is opposite to that of SOC (secondary organic carbon). SOC is larger during the cold period, sulphate (the major contributor to SIA) is larger during summer. Two forms of nitrate were identified: NaNO3, correlated with chloride depletion and aging of sea-spray, mainly present in PM2.5-10; NH4NO3 more abundant in PM2.5. Biomass burning is a relevant source with larger contribution during autumn and winter because of the influence of domestic heating, however, is not negligible in spring and summer, because of the contributions of fires and agricultural practices. Mass closure analysis and PMF results identify two soil sources: crustal associated to long range transport and carbonates associated to local resuspended dust. Both sources contributes to the coarse fraction and have different dynamics with crustal source contributing mainly in high winds from SE conditions and carbonates during high winds from North direction.

Influence of open vegetation fires on black carbon and ozone variability in the southern Himalayas (NCO-P, 5079 m a.s.l.).

We analysed the variability of equivalent black carbon (BC) and ozone (O3) at the global WMO/GAW station Nepal Climate Observatory-Pyramid (NCO-P, 5079 m a.s.l.) in the southern Himalayas, for evaluating the possible contribution of open vegetation fires to the variability of these short-lived climate forcers/pollutants (SLCF/SLCP) in the Himalayan region. We found that 162 days (9% of the data-set) were characterised by acute pollution events with enhanced BC and O3 in respect to the climatological values. By using satellite observations (MODIS fire products and the USGS Land Use Cover Characterization) and air mass back-trajectories, we deduced that 56% of these events were likely to be affected by emissions from open fires along the Himalayas foothills, the Indian Subcontinent and the Northern Indo-Gangetic Plain. These results suggest that open fire emissions are likely to play an important role in modulating seasonal and inter-annual BC and O3 variability over south Himalayas.

High black carbon and ozone concentrations during pollution transport in the Himalayas: five years of continuous observations at NCO-P global GAW station.

To study the influence of polluted air-mass transport carrying ozone (O3) and black carbon (BC) in the high Himalayas, since March 2006 the Nepal Climate Observatory at Pyramid (NCO-P) GAW-WMO global station (Nepal, 5079 m a.s.l.) is operative. During the first 5-year measurements, the O3 and BC concentrations have shown a mean value of 48 +/- 12 ppb (+/- standard deviation) and 208 +/- 374 ng/m3, respectively. Both O3 and BC showed well defined seasonal cycles with maxima during pre-monsoon (O3: 61.3 +/- 7.7 ppbV; BC: 444 +/- 433 ng/m3) and minima during the summer monsoon (O3: 40.1 +/- 12.4 ppbV; BC: 64 +/- 101 ng/m3). The analysis of the days characterised by the presence of a significant BC increase with respect to the typical seasonal cycle identified 156 days affected by "acute" pollution events, corresponding to 9.1% of the entire data-set. Such events mostly occur in the pre-monsoon period, when the O3 diurnal variability is strongly related to the transport of polluted air-mass rich on BC. On average, these "acute" pollution events were characterised by dramatic increases of BC (352%) and O3 (29%) levels compared with the remaining days.

Continuous measurements of aerosol physical parameters at the Mt. Cimone GAW Station (2165 m asl, Italy).

Particle size distribution in the range 0.3

The ABC-Pyramid Atmospheric Research Observatory in Himalaya for aerosol, ozone and halocarbon measurements.

In this work we present the new ABC-Pyramid Atmospheric Research Observatory (Nepal, 27.95 N, 86.82 E) located in the Himalayas, specifically in the Khumbu valley at 5079 m a.s.l. This measurement station has been set-up with the aim of investigating natural and human-induced environmental changes at different scales (local, regional and global). After an accurate instrumental set-up at ISAC-CNR in Bologna (Italy) in autumn 2005, the ABC-Pyramid Observatory for aerosol (physical, chemical and optical properties) and trace gas measurements (ozone and climate altering halocarbons) was installed in the high Khumbu valley in February 2006. Since March 2006, continuous measurements of aerosol particles (optical and physical properties), ozone (O3) and meteorological parameters as well as weekly samplings of particulate matter (for chemical analyses) and grab air samples for the determination of 27 halocarbons, have been carried out. These measurements provide data on the typical atmospheric composition of the Himalayan area between India and China and make investigations of the principal differences and similarities between the monsoon and pre-monsoon seasons possible. The study is carried out within the framework of the Ev-K2-CNR "SHARE-Asia" (Stations at High Altitude for Research on the Environment in Asia) and UNEP-"ABC" (Atmospheric Brown Clouds) projects. With the name of "Nepal Climate Observatory-Pyramid" the station is now part of the Observatory program of the ABC project.