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Cloud radiative properties, cloud lifetime, and precipitation initiation are strongly influenced by the cloud phase. Between ~ 235 and 273 K, ice nucleating particles (INPs) are responsible for the initial phase transition from the liquid to the ice phase in cloud hydrometeors. This study analyzes immersion-mode INP concentrations measured at 243 K at the High Altitude Research Station Jungfraujoch (3580 m a.s.l.) between February 2020 and January 2021, thereby presenting 5 the longest continuous, high-resolution (20 min) data set of online INP measurements to date. The high time resolution and continuity allow to study the seasonal and the diurnal variability of INPs. After exclusion of special events, like Saharan dust events (SDEs), we found a seasonal cycle of INPs, highest in April (median in spring 3.1 INP std L-1), followed by summer (median: 1.6 INP std L-1) and lowest in fall and winter (median: 0.5 INP std L-1 and 0.7 INP std L-1, respectively). Pollen or subpollen particles were deemed unlikely to be responsible for elevated INP concentrations in spring and summer, as periods with high pollen loads from nearby measurement stations do not coincide with the periods of high INP concentrations. Furthermore, for days when the site was purely in the free troposphere (FT), no diurnal cycle in INP concentrations was observed, while days with boundary layer intrusions (BLI) showed a diurnal cycle. The seasonal and diurnal variability of INPs during periods excluding SDEs is with a factor of 7 and 3.3, respectively, significantly lower than the overall variability observed in INP concentration including SDEs of more than three orders of magnitude, when peak values result from SDEs. The median INP concentration over the analyzed 12 months was 1.2 INP std L-1 for FT periods excluding SDEs, and 1.4 INP std L-1 for both FT and BLI, and incl. SDEs, reflecting that despite SDEs showing strong but comparatively brief INP signals, they have a minor impact on the observed annual median INP concentration. [ABSTRACT FROM AUTHOR]

The ice phase in mixed-phase clouds has a pivotal role in global precipitation formation as well as for Earth's radiative budget. Above 235 K, sparse particles with the special ability to initiate ice formation, ice nucleating particles (INPs), are responsible for primary ice formation within these clouds. However, the abundance and distribution of INPs remains largely unknown. Mineral dust is known to be the most abundant INP in the atmosphere at temperatures colder than 258 K. To better constrain and quantify the impact of mineral dust on ice nucleation, we investigate the frequency of Saharan dust events (SDEs) and their contribution to the INP number concentration at 243 K and at a saturation ratio with respect to liquid water (Sw) of 1.04 at the High Altitude Research Station Jungfraujoch (JFJ; 3580 m a.s.l.) from February to December 2020. Using the single scattering albedo Ångström exponent, satellite retrieved dust mass concentrations, simulated tropospheric residence times, and the attenuated backscatter signal from a ceilometer as proxies, we detected 26 SDEs, which in total contributed to 17% of the time span analyzed. We found every SDE to show an increase in median INP concentrations compared to that of all non-SDE periods, however, not always statistically significant. Median INP concentrations of individual SDEs spread between 1.7 and 161 INP std L-1, thus, two orders of magnitude. In the entire period analyzed, 74.7 ± 0.2% of all INPs were measured during SDEs. Based on satellite retrieved dust mass concentrations, we argue that mineral dust is also present at the JFJ outside of SDEs, but at much lower concentrations, thus still contributing to the INP population. We estimate 97.0 ± 0.3% of all INPs active in the immersion mode at 243 K Sw = 1.04 at the JFJ to be mineral dust particles. Overall, we found INP number concentrations to follow a leptokurtic log-normal frequency distribution. We found the INP number concentrations during SDEs to correlate with the ceilometer backscatter signals from a ceilometer located 4.5 km north of the JFJ and 1510 m lower in altitude, thus scanning the air masses at the same altitude as the JFJ. Using the European ceilometer network allows to study the atmospheric pathway of mineral dust plumes over a large domain, which we demonstrate in two case studies. These studies showed that mineral dust plumes form ice crystals at cirrus altitudes, which then sediment to lower altitudes. Upon sublimation in dryer air layers, the residual particles are left potentially pre-activated. Future improvements to the sampling lines of INP counters are required to study if these particles are indeed pre-activated, leading to larger INP number concentrations than reported here. [ABSTRACT FROM AUTHOR]

Aerosol particles are a complex component of the atmospheric system that influences climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport, result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50% and 60% were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75%) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (~10² cm-3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general barely marked, due notably to the absence of a regular day-night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (~10³-104 cm-3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (~10²-10³ cm-3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (i.e. > 50 -- 100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians in the order of ~10 to 1000 cm-3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in-situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol-cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate. [ABSTRACT FROM AUTHOR]

The most widely used non-parametric method for trend analysis is the Mann-Kendall test associated with the Sen's slope. The Mann-Kendall test requires serially uncorrelated time series, whereas most of the atmospheric processes exhibit positive autocorrelation. Several prewhitening methods have been designed to overcome the presence of lag-1 autocorrelation. These include a prewhitening, a detrending and/or a correction for the detrended slope and the original variance of the time series. The choice of which prewhitening method and temporal segmentation to apply has consequences for the statistical significance, the value of the slope and of the confidence limits. Here, the effects of various prewhitening methods are analyzed for seven time series comprising in-situ aerosol measurements (scattering coefficient, absorption coefficient, number concentration and aerosol optical depth), Raman Lidar water vapor mixing ratio and the tropopause and zero degree levels measured by radio-sounding. These time series are characterized by a broad variety of distributions, ranges and lag-1 autocorrelation values and vary in length between 10 and 60 years. A common way to work around the autocorrelation problem is to decrease it by averaging the data over longer time intervals than in the original time series. Thus, the second focus of this study is evaluation of the effect of time granularity on long-term trend analysis. Finally, a new algorithm involving three prewhitening methods is proposed in order to maximize the power of the test, to minimize the amount of erroneous detected trends in the absence of a real trend and to ensure the best slope estimate for the considered length of the time series. [ABSTRACT FROM AUTHOR]

Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system. [ABSTRACT FROM AUTHOR]

In order to assess the global evolution of aerosol parameters affecting climate change, a long-term trend analyses of aerosol optical properties were performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several prewhitening methods and with the Sen's slope were used as main trend analysis methods. Comparisons with General Least Mean Square associated with Autoregressive Bootstrap (GLS/ARB) and with standard Least Mean Square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficients trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficients time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, Eastern/Northern Europe and Arctic, 18 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 30 % of sites have trends, which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10 year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10 year trends are primarily found for earlier periods (10 year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10 year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10 year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10 year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2010-2011 for all stations in the eastern and central US. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage enables a better global view of potential aerosol effects on climate changes. [ABSTRACT FROM AUTHOR]

This study focuses on the analysis of aerosol hygroscopicity using remote sensing technique. Continuous observations of aerosol backscatter coefficient, temperature and water vapour mixing ratio are performed by means of a Raman lidar system at the aerological station of MeteoSwiss at Payerne (Switzerland) since 2008. These measurements allow us to monitor in a continuous way any change of aerosol properties as a function of the relative humidity (RH). These changes can be observed either in time at constant altitude or in altitude at a constant time. The accuracy and precision of RH measurements from the lidar have been evaluated using the radiosonde (RS) technique as reference. A total of 172 RSs were used in this intercomparison which revealed a small bias (<4%RH) and standard deviation (<10%RH) in the whole troposphere between both techniques indicating the good performance of the lidar for characterizing RH. A methodology to identify aerosol hygroscopic conditions has been established and the aerosol hygroscopicity has been characterized by means of the backscatter enhancement factor (fβ). Two case studies, corresponding to different types of aerosol are used to illustrate the potential of this methodology. The first case corresponds to a mixture of rural aerosol and smoke particles which showed a higher hygroscopicity (fβ355 = 2.8 and fβ1064 = 1.8 in the RH range 73%-97%) than the second case, in which mineral dust was present(fβ355 = 1.2 and fβ1064 = 1.1 in the RH range 68%-84%). The higher sensitivity of the shortest wavelength to hygroscopic growth is qualitatively reproduced using Mie simulations. In addition, a good agreement was found between the hygroscopic analysis done in the vertical and in time for case I, where the latter also allowed to observe the hydration and dehydration of this type of aerosol. Finally, the impact of aerosol hygroscopicity on the Earth's radiative balance has been evaluated using the GAME (Global Atmospheric Model) radiative transfer model. The model showed a significant impact with an increase in absolute value of 2.4W/m² at the surface with respect to the dry conditions for the hygroscopic layer of case I (with presence of smoke). [ABSTRACT FROM AUTHOR]

This paper presents the light scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, located mainly in Europe. The data include particle light scattering (σ sp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). A large range of ssp was observed across the network. Low ssp values were on average measured in Nordic and Baltic countries and in Western Europe whereas the highest σsp were measured at regional sites in eastern and central Europe. In these regional areas the SAE was also high indicating the predominance of fine-mode particles. On average, the SAE was lower in the Nordic and Baltic, western and southern countries suggesting a lower fraction of fine-mode particle compared to central and eastern Europe. An increasing gradient of ssp was observed when moving from mountain to regional and to urban sites. Conversely, the mass-independent SAE and g parameters did not show the same gradient. At all sites, both SAE and g varied greatly with aerosol particle loading. The lowest values of g were always observed under low ssp indicating a larger contribution from particles in the smaller accumulation mode. Then, g steeply increased with increasing ssp indicating a progressive shift of the particle size distribution toward the larger end of the accumulation mode. Under periods of high particle mass concentrations, the variation of g was less pronounced whereas the SAE increased or decreased suggesting changes mostly in the coarse aerosol particles mode rather than in the fine mode. The station placement seemed to be the main parameter affecting the intra-annual variability. At mountain sites, higher σsp was measured in summer mainly because of the enhanced boundary layer influence. Conversely, less horizontal and vertical dispersion in winter led to higher σsp at all low altitude sites in central and eastern Europe compared to summer. On average, these sites also showed SAE maxima in summer (and correspondingly g minima). Large intra-annual variability of SAE and g was observed also at Nordic and Baltic countries due to seasonal-dependent transport of different air masses to these remote sites. Statistically significant decreasing trends of σsp were observed at 5 out of 13 stations included in trend analyses. The total reductions of ssp were consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe. [ABSTRACT FROM AUTHOR]

High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude is not a sufficient parameter to characterize the ABL influence. Topography data from the global digital elevation model GTopo30 were used to calculate 5 parameters for 46 high altitude stations situated in five continents. The geometric mean of these 5 parameters determines a topography based index called ABL-TopoIndex which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or plateaus, if the slopes around the station are steep, and finally if the drainage basin for air convection is small. All stations on volcanic islands exhibit a low ABL-TopoIndex whereas stations in the Himalaya and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (s.s.) correlations are found between the 5 and 50 percentiles of all aerosol parameters and the ABL-TopoIndex whereas no s.s. correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a s.s. correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. Finally, the main flow paths for air convection were calculated for various ABL heights. [ABSTRACT FROM AUTHOR]

We present the development of the Pathfinder-TURB algorithm for the analysis of ceilometer backscatter data and the real-time detection of the vertical structure of the planetary boundary layer. Two aerosol layer heights are retrieved by PathfinderTURB: the convective boundary layer (CBL) and the continuous aerosol layer (CAL). PathfinderTURB combines the strengths of gradient- and variancebased methods and addresses the layer attribution problem by adopting a geodesic approach. The algorithm has been applied to 1 year of data measured by two ceilometers of type CHM15k, one operated at the Aerological Observatory of Payerne (491ma.s.l.) on the Swiss plateau and one at the Kleine Scheidegg (2061ma.s.l.) in the Swiss Alps. The retrieval of the CBL has been validated at Payerne using two reference methods: (1) manual detections of the CBL height performed by human experts using the ceilometer backscatter data; (2) values of CBL heights calculated using the Richardson's method from co-located radio sounding data. We found average biases as small as 27m (53 m) with respect to reference method 1 (method 2). Based on the excellent agreement between the two reference methods, PathfinderTURB has been applied to the ceilometer data at the mountainous site of the Kleine Scheidegg for the period September 2014 to November 2015. At this site, the CHM15k is operated in a tilted configuration at 71° zenith angle to probe the atmosphere next to the Sphinx Observatory (3580ma.s.l.) on the Jungfraujoch (JFJ). The analysis of the retrieved layers led to the following results: the CAL reaches the JFJ 41% of the time in summer and 21% of the time in winter for a total of 97 days during the two seasons. The season-averaged daily cycles show that the CBL height reaches the JFJ only during short periods (4% of the time), but on 20 individual days in summer and never during winter. During summer in particular, the CBL and the CAL modify the air sampled in situ at JFJ, resulting in an unequivocal dependence of the measured absorption coefficient on the height of both layers. This highlights the relevance of retrieving the height of CAL and CBL automatically at the JFJ. [ABSTRACT FROM AUTHOR]

Changes of atmospheric methane total columns (CH4) since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns of 0.31 ± 0.03 % year-1 (2σ level of uncertainty) for the 2005-2014 period. Comparisons with in situ methane measurements at both local and global scales show good agreement. We used the GEOS-Chem chemical transport model tagged simulation, which accounts for the contribution of each emission source and one sink in the total methane, simulated over 2005-2012. After regridding according to NDACC vertical layering using a conservative regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane total columns of 0.35 ± 0.03 % year-1 between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30 ± 0.04 % year-1, averaged over 10 stations). Analysis of the GEOS-Chem-tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the interannual variability of methane. However, anthropogenic emissions, such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem-tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained. [ABSTRACT FROM AUTHOR]