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.
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•Composition and sources of PM2.5 and PM2.5–10 are investigated in South-eastern Italy.•Secondary organic and inorganic components were 43% of PM2.5 with opposite seasonal trends.•Two forms of nitrate were observed: sodium nitrate and ammonium nitrate (only in winter).•PMF and mass-closure identified two soil sources accounting for 29% of PM2.5–10.•Biomass burning is an important source at the urban background site even during warm seasons.
Studies on recent climate trends from the Himalayan range are limited, and even completely absent at high elevation (> 5000 m a.s.l.). This study specifically explores the southern slopes of Mt. ...Everest, analyzing the time series of temperature and precipitation reconstructed from seven stations located between 2660 and 5600 m a.s.l. during 1994–2013, complemented with the data from all existing ground weather stations located on both sides of the mountain range (Koshi Basin) over the same period. Overall we find that the main and most significant increase in temperature is concentrated outside of the monsoon period. Above 5000 m a.s.l. the increasing trend in the time series of minimum temperature (+0.072 °C yr−1) is much stronger than of maximum temperature (+0.009 °C yr−1), while the mean temperature increased by +0.044 °C yr−1. Moreover, we note a substantial liquid precipitation weakening (−9.3 mm yr−1) during the monsoon season. The annual rate of decrease in precipitation at higher elevations is similar to the one at lower elevations on the southern side of the Koshi Basin, but the drier conditions of this remote environment make the fractional loss much more consistent (−47% during the monsoon period). Our results challenge the assumptions on whether temperature or precipitation is the main driver of recent glacier mass changes in the region. The main implications are the following: (1) the negative mass balances of glaciers observed in this region can be more ascribed to a decrease in accumulation (snowfall) than to an increase in surface melting; (2) the melting has only been favoured during winter and spring months and close to the glaciers terminus; (3) a decrease in the probability of snowfall (−10%) has made a significant impact only at glacier ablation zone, but the magnitude of this decrease is distinctly lower than the observed decrease in precipitation; (4) the decrease in accumulation could have caused the observed decrease in glacier flow velocity and the current stagnation of glacier termini, which in turn could have produced more melting under the debris glacier cover, leading to the formation of numerous supraglacial and proglacial lakes that have characterized the region in the last decades.
Aerosol mass and the absorbing fraction are important variables, needed to constrain the role of atmospheric particles in the Earth radiation budget, both directly and indirectly through CCN ...activation. In particular, their monitoring in remote areas and mountain sites is essential for determining source regions, elucidating the mechanisms of long range transport of anthropogenic pollutants, and validating regional and global models. Since March 2006, aerosol mass and black carbon concentration have been monitored at the Nepal Climate Observatory-Pyramid, a permanent high-altitude research station located in the Khumbu valley at 5079 m a.s.l. below Mt. Everest. The first two-year averages of PM1 and PM1−10 mass were 1.94 μg m−3 and 1.88 μg m−3, with standard deviations of 3.90 μg m−3 and 4.45 μg m−3, respectively, while the black carbon concentration average is 160.5 ng m−3, with a standard deviation of 296.1 ng m−3. Both aerosol mass and black carbon show well defined annual cycles, with a maximum during the pre-monsoon season and a minimum during the monsoon. They also display a typical diurnal cycle during all the seasons, with the lowest particle concentration recorded during the night, and a considerable increase during the afternoon, revealing the major role played by thermal winds in influencing the behaviour of atmospheric compounds over the high Himalayas. The aerosol concentration is subject to high variability: in fact, as well as frequent "background conditions" (55% of the time) when BC concentrations are mainly below 100 ng m−3, concentrations up to 5 μg m−3 are reached during some episodes (a few days every year) in the pre-monsoon seasons. The variability of PM and BC is the result of both short-term changes due to thermal wind development in the valley, and long-range transport/synoptic circulation. At NCO-P, higher concentrations of PM1 and BC are mostly associated with regional circulation and westerly air masses from the Middle East, while the strongest contributions of mineral dust arrive from the Middle East and regional circulation, with a special contribution from North Africa and South-West Arabian Peninsula in post-monsoon and winter season.
The Kathmandu Valley in south Asia is considered as one of the global "hot spots" in terms of urban air pollution. It is facing severe air quality problems as a result of rapid urbanization and land ...use change, socioeconomic transformation, and high population growth. In this paper, we present the first full year (February 2013-January 2014) analysis of simultaneous measurements of two short-lived climate forcers/pollutants (SLCF/P), i.e., ozone (O3) and equivalent black carbon (hereinafter noted as BC) and aerosol number concentration at Paknajol, in the city center of Kathmandu. The diurnal behavior of equivalent BC and aerosol number concentration indicated that local pollution sources represent the major contributions to air pollution in this city. In addition to photochemistry, the planetary boundary layer (PBL) and wind play important roles in determining O3 variability, as suggested by the analysis of seasonal changes of the diurnal cycles and the correlation with meteorological parameters and aerosol properties. Especially during pre-monsoon, high values of O3 were found during the afternoon/evening. This could be related to mixing and entrainment processes between upper residual layers and the PBL. The high O3 concentrations, in particular during pre-monsoon, appeared well related to the impact of major open vegetation fires occurring at the regional scale. On a synoptic-scale perspective, westerly and regional atmospheric circulations appeared to be especially conducive for the occurrence of the high BC and O3 values. The very high values of SLCF/P, detected during the whole measurement period, indicated persisting adverse air quality conditions, dangerous for the health of over 3 million residents of the Kathmandu Valley, and the environment. Consequently, all of this information may be useful for implementing control measures to mitigate the occurrence of acute pollution levels in the Kathmandu Valley and surrounding area.
The possible minimal range of reduction in snow surface albedo due to dry deposition of black carbon (BC) in the pre-monsoon period (March–May) was estimated as a lower bound together with the ...estimation of its accuracy, based on atmospheric observations at the Nepal Climate Observatory – Pyramid (NCO-P) sited at 5079 m a.s.l. in the Himalayan region. A total BC deposition rate was estimated as 2.89 μg m−2 day−1 providing a total deposition of 266 μg m−2 for March–May at the site, based on a calculation with a minimal deposition velocity of 1.0×10−4 m s−1 with atmospheric data of equivalent BC concentration. Main BC size at NCO-P site was determined as 103.1–669.8 nm by correlation analyses between equivalent BC concentration and particulate size distributions in the atmosphere. The BC deposition from the size distribution data was also estimated. It was found that 8.7% of the estimated dry deposition corresponds to the estimated BC deposition from equivalent BC concentration data. If all the BC is deposited uniformly on the top 2-cm pure snow, the corresponding BC concentration is 26.0–68.2 μg kg−1, assuming snow density variations of 195–512 kg m−3 of Yala Glacier close to NCO-P site. Such a concentration of BC in snow could result in 2.0–5.2% albedo reductions. By assuming these albedo reductions continue throughout the year, and then applying simple numerical experiments with a glacier mass balance model, we estimated reductions would lead to runoff increases of 70–204 mm of water. This runoff is the equivalent of 11.6–33.9% of the annual discharge of a typical Tibetan glacier. Our estimates of BC concentration in snow surface for pre-monsoon season is comparable to those at similar altitudes in the Himalayan region, where glaciers and perpetual snow regions begin, in the vicinity of NCO-P. Our estimates from only BC are likely to represent a lower bound for snow albedo reductions, because we used a fixed slower deposition velocity. In addition, we excluded the effects of atmospheric wind and turbulence, snow aging, dust deposition, and snow albedo feedbacks. This preliminary study represents the first investigation of BC deposition and related albedo on snow, using atmospheric aerosol data observed at the southern slope in the Himalayas.
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.
•We tested and used an inter-species correlation approach to calculate anthropogenic CH4 emissions from the Po basin.•Atmospheric observations from a mountain site were used.•Differences with bottom-up inventories were pointed out for 4 investigated years.•An accurate selection of the atmospheric data is pivotal for getting reliable information.•Yearly aggregation of data and input CO emissions led to further uncertainties.
We report chemical composition data for PM10 and PM1 from the Nepal Climate Observatory-Pyramid (NCO-P), the world's highest aerosol observatory, located at 5079 m a.s.l. at the foothills of Mt. ...Everest. Despite its high altitude, the average PM10 mass apportioned by the chemical analyses is of the order of 6 μg m-3 (i.e., 10 μg/scm), with almost a half of this mass accounted for by organic matter, elemental carbon (EC) and inorganic ions, the rest being mineral dust. Organic matter, in particular, accounted for by 2.0 μg m-3 (i.e., 3.6 μg/scm) on a yearly basis, and it is by far the major PM10 component beside mineral oxides. Non-negligible concentrations of EC were also observed (0.36 μg/scm), confirming that light-absorbing aerosol produced from combustion sources can be efficiently transported up the altitudes of Himalayan glaciers. The concentrations of carbonaceous and ionic aerosols follow a common time trend with a maximum in the premonsoon season, a minimum during the monsoon and a slow recovery during the postmonsoon and dry seasons, which is the same phenomenology observed for other Nepalese Himalayan sites in previous studies. Such seasonal cycle can be explained by the seasonal variations of dry and moist convection and of wet scavenging processes characterizing the climate of north Indian subcontinent. We document the effect of orographic transport of carbonaceous and sulphate particles upslope the Himalayas, showing that the valley breeze circulation, which is almost permanently active during the out-of-monsoon season, greatly impacts the chemical composition of PM10 and PM1 in the high Himalayas and provides an efficient mechanism for bringing anthropogenic aerosols into the Asian upper troposphere (>5000 m a.s.l.). The concentrations of mineral dust are impacted to a smaller extent by valley breezes and follow a unique seasonal cycle which suggest multiple source areas in central and south-west Asia. Our findings, based on two years of observations of the aerosol chemical composition, provide clear evidence that the southern side of the high Himalayas is impacted by transport of anthropogenic aerosols which constitute the Asian brown cloud.
This work investigates the variability of ozone (O3), carbon monoxide (CO) and equivalent black carbon (BC) at the Italian Climate Observatory "O. Vittori" (ICO-OV), part of the Mt. Cimone global ...GAW-WMO station (Italy). For this purpose, ICO-OV observations carried out in the period January 2007–June 2009, have been analyzed and correlated with the outputs of the FLEXPART Lagrangian dispersion model to specifically evaluate the influence of biomass burning (BB) and anthropogenic emissions younger than 20 days. During the investigation period, the average O3, CO and BC at ICO-OV were 54 ± 3 ppb, 122 ± 7 ppb and 213 ± 34 ng m−3 (mean ± expanded uncertainty with p < 95%), with clear seasonal cycles characterized by summer maxima and winter minima for O3 and BC and spring maximum and summer minimum for CO. According to FLEXPART outputs, BB impact is maximized during the warm months from July to September but appeared to have a significant contribution to the observed tracers only during specific transport events. We characterised in detail five "representative" events with respect to transport scales (i.e. global, regional and local), source regions and O3, CO and BC variations. For these events, very large variability of enhancement ratios O3/CO (from −0.22 to 0.71) and BC/CO (from 2.69 to 29.83 ng m−3 ppb−1) were observed. CO contributions related with anthropogenic emissions (COant) contributed to 17.4% of the mean CO value observed at ICO-OV, with the warm months appearing particularly affected by transport events of air-masses rich in anthropogenic pollution. The proportion of tracer variability that is described by FLEXPART COant peaked to 37% (in May–September) for CO, 19% (in May–September) for O3 and 32% (in January–April) for BC. During May–September, the analysis of the correlation among CO, O3 and BC as a function of the COant indicated that ICO-OV was influenced by air-masses rich in anthropogenic pollution transported from the regional to the global scale. On the other side, CO and O3 were negatively correlated during October–December, when FLEXPART does not show significant presence of recent anthropogenic emissions and only a few observations are characterized by enhanced BC. Such behaviour may be attributed to an ensemble of processes concurrent in enhancing O3 with low CO (upper troposphere/lower stratosphere intrusions) and to O3 titration by NO in polluted air-masses along with lower photochemical activity. An intermediate situation occurs in January–April when CO and O3 were almost uncorrelated and BC enhancements were associated to relatively old (10 days) anthropogenic emissions.
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 ⁰C decade−1, 1.1 ± 0.2 ⁰C decade−1 and -0.3 ± 0.2 ⁰C 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.
•Surface ozone trend at El Arenosillo observatory was explored (2000–2021).•A significant background ozone increase was obtained with 2.2 ± 0.3 ppb decade−1.•Monthly and hourly trends were studied based on daily and hourly averages.•A monthly pattern was observed, opposite to the typical monthly ozone variability.•In the ozone trends for every hour of the day, two patterns were identified.
This work aims at determining the characteristics and the preferred source regions of stratospheric air masses at the Mt. Cimone World Meteorological Organization‐Global Atmosphere Watch station ...located in the Italian northern Apennines (44°11′N, 10°42′E, 2165 m above sea level) , a site which is considered representative of Southern Europe‐Mediterranean free troposphere. Source regions of high concentrations of 7Be, 7Be/210Pb, and O3 and regions originating high potential vorticity values are analyzed by means of trajectory statistical methods applied over the time series collected in the period of 1998–2011 to this aim. Our analysis points out the frequent occurrence of stratosphere‐to‐troposphere exchange in the North America and northern Atlantic region, which can be linked to the usual location of the polar‐front and subtropical jet streams in these two regions, but also to the tropopause discontinuity and to the high cyclogenetic activity in the Atlantic region. High 7Be concentrations associated with trajectories of high‐latitude origin descend from high altitudes to the study site, while at midlatitudes trajectories arrive from relatively lower levels. The geographical distribution of the tropopause crossing of air masses before arriving the study site points out particularly to Greenland. Our results also suggest the importance of the interaction between upper level disturbances and the Alps mountain range as a driver for stratosphere‐to‐troposphere exchange. In this case, the time between the tropopause crossing and the arrival at the elevated study site is less than 24 h and frequently below 6 h. The Atlas range in northern Africa plays a similar role though with lower influence.
Key Points
First long‐term analysis of stratospheric intrusions by using 7Be/210Pb ratio in the Mediterranean region
Stratospheric influence of the North Atlantic and high 7Be from Northern Africa
Importance of lee cyclogenesis as STE promoting mechanism
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