This work introduces an index to identify deep stratospheric intrusions (SI) from measurement data alone, without requiring additional model-based information. This stratospheric intrusion index (SI2) provides a qualitative description of SI event behaviour by summarizing the information from different tracer variations. Moreover, being independent from any model constraint, the SI2 can also represent a valid tool to help in evaluating the capacity of chemistry-transport and chemistry-climate models in simulating deep stratosphere to troposphere transport. The in situ variations of ozone, beryllium-7 and relative humidity were used to calculate the index. The SI2 was applied on 8-year data recorded at the regional GAW station of Mt. Cimone (2165 m asl; 44.10N, 10.70E: Italy). The comparison of the SI2 behaviour with a pre-existing database obtained by also using model products, permitted us to tune a SI2-threshold value capable of identifying SI events efficiently. In good agreement with previous climatological studies across Europe, at Mt. Cimone, the averaged monthly SI frequency obtained by the SI2 analysis showed a clear seasonal cycle with a winter maximum and a spring-summer minimum. These results suggest that the presented methodology is efficient for both identifying SI events and evaluating their annual frequency at the considered baseline measurement site.

High levels of trace gas (O3 and CO) and aerosol (BC, fine and coarse particle volumes), as well as high scattering coefficient values, were recorded at the regional GAW-WMO station of Mt. Cimone (CMN, 2165 m a.s.l., Italy) during the period 26–30 August 2007. Analysis of air-mass circulation, aerosol chemical characterization and trace gas and aerosol enhancement ratios (ERs), showed that high O3 and aerosol levels were likely linked to (i) the transport of anthropogenic pollution from northern Italy, and (ii) the advection of air masses rich in mineral dust and biomass burning (BB) products from North Africa. In particular, during the advection of air masses from North Africa, the CO and aerosol levels (CO: 175 ppbv, BC: 1015 ng/m3, fine particle volume: 3.00 µm3 cm-3, ðp: 84.5 Mm-1) were even higher than during the pollution event (CO: 138 ppbv, BC: 733 ng/m3, fine particles volume: 1.58 µm3 cm-3, ðp: 44.9 Mm-1). Moreover, despite the presence of mineral dust able to affect significantly the O3 concentration, the analysis of ERs showed that the BB event represented an efficient source of fine aerosol particles (e.g. BC), but also of the O3 recorded at CMN. In particular, the calculated O3/CO ERs (0.10–0.17 ppbv/ppbv) were in the range of values found in literature for relatively aged (2–4 days) BB plumes and suggested significant photochemical O3 production during the air-mass transport. For fine particles and ðp, the calculated ERs was higher in the BB plumes than during the anthropogenic pollution events, stressing the importance of the identified BB event as a source of atmospheric aerosol able to affect the atmospheric radiation budget. These results suggest that episodes of mineral dust mobilization and wildfire emissions over North Africa could significantly influence radiative properties (as deduced from ðp observations at CMN) and air quality over the Mediterranean basin and northern Italy.

Particle size distribution in the range 0.3 < Dp < 20 µm, has been analysed from August 2002 to July 2006 at the GAW Station of Mt. Cimone (44.10 N, 10.42 E; 2165 m asl) in the northern Italian Apennines. The seasonal aerosol number size distribution, characterized by a bimodal shape, showed a behaviour typical for background conditions, characterized by highest values in summer and lowest in winter. The seasonal and diurnal variations of the larger accumulation mode (0.3 < Dp < 1 µm average values: 26.15 cm- 3) and the coarse mode (1 < Dp < 20 µm, average value: 0.17 cm-3) particle number concentrations (N0.3–1 and N1–20, respectively) exhibited a seasonal cycle with the highest values in spring–summer and the lowest value in autumn–winter. Except in winter, N0.3–1 showed a clear diurnal variation with high values during day-time. N1–20 showed a less marked diurnal variation (but with higher variability), suggesting the influence of non-continuous sources of coarse particle (i.e. Saharan dust events). Since July 2005, continuous measurement of black carbon (BC) concentrations was also available at the measurement site. On average low BC concentrations were recorded (average value: 0.28 µg m-3) even if a few events of high concentrations were recorded both in warm and cold season. Apart from wet scavenging processes which strongly affected aerosol concentrations, combined analysis of N0.3–1, BC, meteorological parameters and air mass back-trajectories, suggests that the transport of polluted air masses from the lower troposphere (by local, regional or long-range transport) represents an important mechanism favouring N0.3–1 and BC increases at Mt. Cimone. In particular, a trajectory statistical analysis for the period July 2005–July 2006 allowed the identification of the main source regions of BC and N0.3–1 for Mt. Cimone: north Italy, west Europe and east Europe.

During the period May 12-23, 1992, an intercomparisono of Various ground-based remote sensing UV-visible spectrometers for the measurement of stratospheric NO2 slant columns was held at Lauder (New Zealand). All groups' results from Lauder were reported by the intercomparison referee, David Hofmann,in a special paper [Hofmann et al., 1995].

Multispectral measurements of direct solar irradiance were simultaneously taken employing various sun-photometers at five stations located at different altitudes along the western slope of the Leo valley, in the Apennines (Italy), on a number of clear-sky autumn days in 1981 and 1982. Using precise estimates of the calibration constants of the various sun-photometers, obtained through a rigorous intercomparison procedure, the measurements were examined following the most up-to-date criteria of the sun-photometry method to determine daily homogeneous sets of aerosol optical depths at three window-wavelengths, at all five stations. The values of aerosol optical depth obtained from the 1982 measurements were corrected for the extinction effects produced by the stratospheric cloud of El Chichón volcanic aerosols, following a procedure based on the multimodal aerosol extinction model proposed by Pueschel et al. (Pueschel, R.F., Kinne, S.A., Russell, P.B., Snetsinger, K.G., 1993. Effects of the 1991 Pinatubo volcanic eruption on the physical and radiative properties of stratospheric aerosols. Keevallik, S. Kärner, O. (Eds.), IRS '92: Current Problems in Atmospheric Radiation. Proceedings of the International Radiation Symposium, A. Deepak Publ., Hampton, Va., 183–186.) for 6-month-old volcanic particles (see Appendix). The results show that the tropospheric aerosol optical depth at 500-nm wavelength usually assumed low values in the early morning, most generally decreasing from 0.08 to 0.01 with the station altitude, and considerably increased during the morning, especially at the lower stations, as a result of the vertical transport of particulate matter due to the upslope breezes. The corresponding daily percentage increases varied between 60% and 370%, presenting a median value of 175% and quartiles of 140% and 230%. The time-variations of the volume aerosol extinction coefficient at the 500-nm wavelength were evaluated within the four atmospheric layers defined by the station altitudes, presenting early morning values mainly varying from 0.02 to 0.20 km(-1) in the first layer, from 0.02 to 0.11 km(-1) in both second and third layers and from 0.01 to 0.03 km(-1) in the fourth. Therefore, greater increases were found to occur within the three lower layers situated below 1500 m height, with hourly mean percentage variations ranging between 10% and 420%, with a median value of 230% and quartiles of 70% and 270%.

Multispectral sun-photometric measurements of aerosol optical depth were performed at five stations located at different altitudes from about 500 to 2165 m amsl in the Leo valley in the Apennines (Italy), on some clear-sky autumn days of 1981 and 1982. These measurements showed that the aerosol optical depth greatly increased during the morning at all stations due to the convective transport of particulate matter induced by the local upslope breezes. To evaluate the corresponding variations of the vertical mass loading of particulate matter, two continental and rural aerosol extinction models were determined: the first provides the spectral series of both volume and mass aerosol extinction coefficients at nine visible and near-infrared wavelengths for 27 aerosol particle size-distribution curves of Junge-type with values of the Ångström exponent ? varying between 0.15 and 1.99; the second is based on linear combinations of three monomodal particle size-distribution curves determined to give form to a nuclei mode, an accumulation mode and a coarse particle mode, respectively, whose particle number concentrations were defined to fit the values of ? characterising the spectral series of aerosol optical depth. These aerosol extinction models were used to obtain estimates of the columnar aerosol mass content at the five stations, finding values mostly ranging between 0.03 and 0.12 g m?2 at the two lower stations, 0.02 and 0.08 g m?2 at the two intermediate stations and between 0.01 and 0.03 g m?2 at the high-altitude Mt. Cimone station. The corresponding hourly mean percentage variations of the vertical aerosol mass loading were found to vary between a few percentages and nearly 100%, with median values ranging from 14% to 29% at the various stations. From these estimates, evaluations of the aerosol mass concentration were obtained within the four layers, varying from 15 to 160 ?g m?3 in the first layer, from 15 to 95 ?g m?3 in the second, from 10 to 60 ?g m?3 in the third and from 5 to 20 ?g m?3 in the fourth. Correspondingly, the hourly mean percentage variations were found to range between ?26% and +124% within the four layers, with median values gradually increasing from +4% to +20%, passing from the first to the fourth layer.

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 6µg 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., 3.6µg/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.

In the frame of the MIUR-AEROCLOUDS project (Study of Direct and Indirect Aerosol Effects on Climate), night-time and daytime size-segregated aerosol samples were collected concurrently at five different sites (near-city, urban, rural, marine and mountain background sites). The paper reports on the daily evolution of the main aerosol chemical characteristics as a function of particle size in different environments over the Italian Peninsula, spanning from the Po Valley to the south Tyrrhenian coast. Two 4-day intensive observation periods (IOPs) were undertaken in July 2007 and February 2008, under meteorological conditions typical of the summer and winter climate for Italy. In the summer IOP, under stable atmospheric conditions, at the low-altitude continental sites the diurnal evolution of the planetary boundary layer (PBL), induces an atmospheric dilution effect driving the particulate matter (PM) concentrations, while, at the mountain site, it determines the upward motion of polluted air masses from the Po Valley PBL in daytime. The fine fraction was dominated by ammonium salts and carbonaceous matter (water-soluble organic matter, WSOM, and water-insoluble carbonaceous matter, WINCM). High concentrations of ammonium sulphate and WSOM due to enhanced photochemical activity constituted the background aerosol composition over the whole country, whereas, ammonium nitrate and WINCM were more associated to local emissions (e.g. urban site with concentrations peaking in the finest size range due to strong local traffic-related sources of ultrafine particles). During the winter IOP in the Po Valley, the shallow PBL depths and low wind velocity, especially at night, favoured the condensation of semi-volatile species (i.e. organic matter and ammonium nitrate), causing the high fine PM concentration observed at ground level.

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