Browsing by Autor "Alfred Wiedensohler"

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A decade of atmospheric composition observations in the undersampled Central Andes
(2022) Marcos Andrade; Diego Aliaga; Luis Blacutt; Ricardo Forno; René Gutierrez; Fernando Velarde; Isabel Moreno; Laura Ticona; Alfred Wiedensohler; Radovan Krejčí
&lt;p&gt;Ten years of almost continuous observations at the highest Global Atmosphere Watch Regional station in the world are presented here. The Chacaltaya observatory (5240 m asl, 16.3&amp;#186;S, 68.1&amp;#186;W) was set up in December 2011. It is currently the only operational station characterizing optical and chemical properties of climate-relevant aerosol and gases in Bolivia and in a radius of about 1500 kilometers from the station. The observations show a clear influence of the well-marked dry and wet meteorological seasons. In addition, the impact on the Andean mountains of long and mid-range transport of biomass burning products from the lowlands is clearly recorded in different parameters measured at the station. Furthermore, the nearby presence of the largest metropolitan area in the region (~1.8 million inhabitants) is observed almost on a daily basis, and therefore different campaigns were carried out to characterize the area and its influence on our measurements. Specific results from these campaigns are discussed elsewhere. Finally, the topographic complexity represents an important challenge for modeling efforts in order to understand sources and sinks (and associated processes) of the observed parameters, requiring not only high spatial resolution and the correct choice of model options, but a novel way of interpreting these results. The decade of collaboration of an international consortium made it possible to keep the station running successfully. The challenge is now to preserve its functioning for the coming decades in a region with historically few high-quality observations while disrupting environmental and socio-economic changes take place.&lt;/p&gt;
A global analysis of climate-relevant aerosol properties retrieved from the network of GAW near-surface observatories
(2020) Paolo Laj; Alessandro Bigi; Clémence Rose; Elisabeth Andrews; Cathrine Lund Myhre; Martine Collaud Coen; Alfred Wiedensohler; Michael Schultz; J. A. Ogren; Markus Fiebig
Abstract. 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.
A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
(Copernicus Publications, 2020) Paolo Laj; Alessandro Bigi; Clémence Rose; Elisabeth Andrews; Cathrine Lund Myhre; Martine Collaud Coen; Yong Lin; Alfred Wiedensohler; Michael Schulz; J. A. Ogren
Abstract. 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 times, 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 observation 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 almost 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 measurement 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.
Aerosols in the Andes: Microphysical Properties and Long-Term Variability
(2026) Diego Aliaga; Fernando Velarde; Marcos Antônio Ribeiro Andrade; Paolo Laj; Gaëlle Uzu; Kay Weinhold; Alfred Wiedensohler; Ilona Riipinen; Radovan Krejci
Aerosol properties, loading, trends, and variability in the upper troposphere are key to understanding the evolving state of the atmosphere and the role of aerosols in climate and cloud processes. However, long-term in-situ aerosol observations at high altitudes remain scarce worldwide, particularly in the Global South. This observational gap limits our ability to develop a global perspective on aerosol sources, processes, and impacts within the climate system.Here we present 13 years (2012–2024) of continuous aerosol-related measurements conducted at the world’s highest Global Atmosphere Watch (GAW) station, located on Mount Chacaltaya (CHC) in the central Andes of Bolivia at an elevation of 5.2 km a.s.l. This dataset is one of the longest in existence on the South American continent and therefore provides a unique opportunity to evaluate trends in aerosol concentrations and properties. These trends and properties are influenced by, for example, biomass burning in the Amazon, the transport of pollution from the conurbation of La Paz and El Alto, located 18 km to the south, and the subsidence of air masses from the upper troposphere.We focus on particle number size distributions (PNSD), equivalent black carbon (eBC), and related meteorological and chemical tracers, including water vapor mixing ratio (WVMR) and carbon monoxide (CO). We characterize aerosol properties and loading by combining traditional time-series analysis (e.g., separation by hour of day, season, and year) with an unsupervised k-means clustering approach that disentangles the dominant atmospheric regimes influencing aerosol properties at CHC. The clustering uses PNSD, eBC, and WVMR as input variables and identifies seven distinct categories of days, hereafter referred to as atmospheric regimes, which represent significantly different source regions and aerosol processing pathways (e.g., cloud processing, wet deposition, and new particle formation). The performance of the clustering is evaluated using independent tracers, namely CO concentrations and HYSPLIT back trajectories. For each regime, the individual days grouped within it exhibit internally consistent CO levels and air-mass provenance that are clearly distinct from those of other regimes. This result is particularly encouraging given that neither CO nor back trajectories were included as inputs to the clustering algorithm.One regime is particularly noteworthy, representing a persistent free-tropospheric state characterized by extremely low WVMR, CO, and eBC, along with signatures of early-morning new particle formation. We find that the concentration of particles in this regime has significantly decreased over the 13-year period which indicates a declining upper-tropospheric particle concentration. A second notable regime is associated with biomass burning. We find that its occurrence has increased over time, from ~10% of days during the biomass-burning season (August–November) in the first years to ~50% in the last years. This suggests an increment on the number of biomass burning episodes measured at the station. Additional categories capture aerosol–cloud processing during Amazonian boundary-layer uplift, local eBC influence from the La Paz–El Alto metropolitan area, and strong nucleation under dry, coastal/Altiplano air masses. Overall, these results emphasize a region in rapid change and the importance and utility of long-term measurements in under sampled areas.
Black carbon emission and transport mechanisms to the free troposphere at the La Paz/El Alto (Bolivia) metropolitan area based on the Day of Census (2012)
(Elsevier BV, 2018) Alfred Wiedensohler; Marcos Andrade; Kay Weinhold; Thomas Müller; W. Birmili; Fernando Velarde; Isabel Moreno; Ricardo Forno; Maria Fernanda Sanchez Barrero; Paolo Laj
Urban development, growing industrialization, and increasing demand for mobility have led to elevated levels of air pollution in many large cities in Latin America, where air quality standards and WHO guidelines are frequently exceeded. The conurbation of the metropolitan area of La Paz/El Alto is one of the fastest growing urban settlements in South America with the particularity of being located in a very complex terrain at a high altitude. As many large cities or metropolitan areas, the metropolitan area of La Paz/El Alto and the Altiplano region are facing air quality deterioration. Long-term measurement data of the equivalent black carbon (eBC) mass concentrations and particle number size distributions (PNSD) from the Global Atmosphere Watch Observatory Chacaltaya (CHC; 5240 m a.s.l., above sea level) indicated a systematic transport of particle matter from the metropolitan area of La Paz/El Alto to this high altitude station and subsequently to the lower free troposphere. To better understand the sources and the transport mechanisms, we conducted eBC and PNSDs measurements during an intensive campaign at two locations in the urban area of La Paz/El Alto from September to November 2012. While the airport of El Alto site (4040 m a.s.l.) can be seen as representative of the urban and Altiplano background, the road site located in Central La Paz (3590 m a.s.l.) is representative for heavy traffic-dominated conditions. Peaks of eBC mass concentrations up to 5 μg m−3 were observed at the El Alto background site in the early morning and evening, while minimum values were detected in the early afternoon, mainly due to thermal convection and change of the planetary boundary layer height. The traffic-related eBC mass concentrations at the road site reached maximum values of 10–20 μg m−3. A complete traffic ban on the specific Bolivian Day of Census (November 21, 2012) led to a decrease of eBC below 1 μg m−3 at the road site for the entire day. Compared to the day before and after, particle number concentrations decreased by a factor between 5 and 25 over the particle size range from 10 to 800 nm, while the submicrometer particle mass concentration dropped by approximately 80%. These results indicate that traffic is the dominating source of BC and particulate air pollution in the metropolitan area of La Paz/El Alto. In general, the diurnal cycle of eBC mass concentration at the Chacaltaya observatory is anti-correlated to the observations at the El Alto background site. This pattern indicates that the traffic-related particulate matter, including BC, is transported to higher altitudes with the developing of the boundary layer during daytime. The metropolitan area of La Paz/El Alto seems to be a significant source for BC of the regional lower free troposphere. From there, BC can be transported over long distances and exert impact on climate and composition of remote southern hemisphere.
CCN production by new particle formation in the free troposphere
(Copernicus Publications, 2017) Clémence Rose; Karine Sellegri; Isabel Moreno; Fernando Velarde; Michel Ramonet; Kay Weinhold; Radovan Krejčí; Marcos Andrade; Alfred Wiedensohler; Patrick Ginot
Abstract. Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contributes significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, on Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ∼ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between 1 January and 31 December 2012, we found that 61 % of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF, relative to the transport and growth of pre-existing particles, to CCN size. The averaged production of 50 nm particles during those events was 5072, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 53 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud-related radiative processes.
Exposure and Respiratory Tract Deposition Dose of Equivalent Black Carbon in High Altitudes
(Multidisciplinary Digital Publishing Institute, 2020) Leizel Madueño; Simonas Kecorius; Marcos Andrade; Alfred Wiedensohler
The traffic microenvironment accounts for a significant fraction of the total daily dose of inhaled air pollutants. The adverse effects of air pollution may be intensified in high altitudes (HA) due to increased minute ventilation (MV), which may result in higher deposition doses compared to that at sea level. Despite this, air quality studies in regions with combined high pollution levels and enhanced inhalation are limited. The main goals of this study are to investigate how the choice of travel mode (walking, microbus, and cable car ride) determines (i) the personal exposure to equivalent black carbon (eBC) and (ii) the corresponding potential respiratory deposited dose (RDD) in HA. For this investigation, we chose La Paz and El Alto in Bolivia as HA representative cities. The highest eBC exposure occurred in microbus commutes (13 μg m−3), while the highest RDD per trip was recorded while walking (6.3 μg) due to increased MV. On the other hand, the lowest eBC exposure and RDD were observed in cable car commute. Compared with similar studies done at sea level, our results revealed that a HA city should reduce exposure by 1.4 to 1.8-fold to achieve similar RDD at sea level, implying that HA cities require doubly aggressive and stringent road emission policies compared to those at sea level.
Identifying source regions of air masses sampled at the tropical high-altitude site of Chacaltaya using WRF-FLEXPART and cluster analysis
(Copernicus Publications, 2021) Diego Aliaga; Victoria A. Sinclair; Marcos Andrade; Paulo Artaxo; Samara Carbone; Evgeny Kadantsev; Paolo Laj; Alfred Wiedensohler; Radovan Krejčí; Federico Bianchi
Abstract. Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long-term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free-tropospheric air; however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high-altitude sites is required. Here we present a new method, based on the source–receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.; 16.35∘ S, 68.13∘ W) for the 6-month duration of the “Southern Hemisphere high-altitude experiment on particle nucleation and growth” (SALTENA) to identify where sampled air masses originate and to quantify the influence of the surface and the free troposphere. A key aspect of our method is that it is probabilistic, and for each observation time, more than one air mass (cluster) can influence the station, and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced by either boundary layer or free-troposphere air masses. Air sampled at CHC is a mix of different provenance. We find that on average 9 % of the air, at any given observation time, has been in contact with the surface within 4 d prior to arriving at CHC. Furthermore, 24 % of the air has been located within the first 1.5 km above ground level (surface included). Consequently, 76 % of the air sampled at CHC originates from the free troposphere. However, pure free-tropospheric influences are rare, and often samples are concurrently influenced by both boundary layer and free-tropospheric air masses. A clear diurnal cycle is present, with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29 % of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle, whereas the mid- and long-range clusters' (>200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km north-west from the station.
Identifying source regions of air masses sampled at the tropicalhigh-altitude site of Chacaltaya using WRF-FLEXPART and clusteranalysis
(2021) Diego Aliaga; Victoria A. Sinclair; Marcos Andrade; Paulo Artaxo; Samara Carbone; Evgeny Kadantsev; Paolo Laj; Alfred Wiedensohler; Radovan Krejčí; Federico Bianchi
Abstract. Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free tropospheric air however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high altitude sites is required. Here we present a new method, based on the source-receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.,16.35° S, 68.13° W) for the 6-month duration of the “Southern hemisphere high altitude experiment on particle nucleation and growth” (SALTENA) to identify where sampled air masses originate and to quantify the influence of the boundary layer and the free troposphere. A key aspect of our method is that it is probabilistic and for each observation time, more than one air mass (cluster) can influence the station and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced either by boundary layer or free troposphere air masses. We find that on average, 9% of the air sampled at CHC, at any given observation time, has been in contact with the surface within 4 days prior to arriving at CHC, 24% of the air was located below 1.5 km above ground level and consequently, 76% of the measured air masses at CHC represent free tropospheric air. However, pure free-tropospheric influences are rare and often samples are concurrently influenced by both boundary-layer and free-tropospheric air masses. A clear diurnal cycle is present with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29% of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle whereas the mid- and long-range clusters’ (>200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in-situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km northwest from the station.
Mobility particle size spectrometers: Calibration procedures and measurement uncertainties
(Taylor & Francis, 2017) Alfred Wiedensohler; A. Wiesner; Kay Weinhold; W. Birmili; M. Hermann; Maik Merkel; Thomas Müller; Sascha Pfeifer; Andres Schmidt; Thomas Tuch
Mobility particle size spectrometers (MPSS) belong to the essential instruments in aerosol science that determine the particle number size distribution (PNSD) in the submicrometer size range. Following calibration procedures and target uncertainties against standards and reference instruments are suggested for a complete MPSS quality assurance program: (a) calibration of the CPC counting efficiency curve (within 5% for the plateau counting efficiency; within 1 nm for the 50% detection efficiency diameter), (b) sizing calibration of the MPSS, using a certified polystyrene latex (PSL) particle size standard at 203 nm (within 3%), (c) intercomparison of the PNSD of the MPSS (within 10% and 20% of the dN/dlogDP concentration for the particle size range 20–200 and 200–800 nm, respectively), and (d) intercomparison of the integral PNC of the MPSS (within 10%). Furthermore, following measurement uncertainties have been investigated: (a) PSL particle size standards in the range from 100 to 500 nm match within 1% after sizing calibration at 203 nm. (b) Bipolar diffusion chargers based on the radioactive nuclides Kr85, Am241, and Ni63 and a new ionizer based on corona discharge follow the recommended bipolar charge distribution, while soft X-ray-based charges may alter faster than expected. (c) The use of a positive high voltage supply show a 10% better performance than a negative one. (d) The intercomparison of the integral PNC of an MPSS against the total number concentration is still within the target uncertainty at an ambient pressure of approximately 500 hPa.Copyright © 2018 Published with license by American Association for Aerosol Research
New Particle Formation and impact on CCN concentrationsin the boundary layer and free troposphere at the highaltitude station of Chacaltaya (5240 m a.s.l.), Bolivia
(2016) Clémence Rose; Karine Sellegri; Isabel Moreno; Fernando Velarde; Michel Ramonet; Kay Weinhold; Radovan Krejčí; Marcos Andrade; Alfred Wiedensohler; Patrick Ginot
Abstract. Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contribute significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ~ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between January 1 and December 31 2012, we found that 61% of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF events relative to the transport of pre-existing particles to the site. The averaged production of 50 nm particles during those events was 5072 cm−3, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 56 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud related radiative processes.
New Particle Formation: A Review of Ground-Based Observations at Mountain Research Stations
(Multidisciplinary Digital Publishing Institute, 2019) Karine Sellegri; Clémence Rose; Angela Marinoni; Angelo Lupi; Alfred Wiedensohler; Marcos Andrade; Paolo Bonasoni; Paolo Laj
New particle formation (NPF) was predicted to contribute to a major fraction of free tropospheric particle number and cloud condensation nuclei (CCN) concentrations by global models. At high altitudes, pre-existing particle concentrations are low, leading to limited condensational sinks for nucleation precursor gases, and temperatures are cooler compared to lower altitudes, whereas radiation is higher. These factors would all be in favor of nucleation to occur with an enhanced frequency at high altitudes. In the present work, long term data from six altitude stations (and four continents) at various altitudes (from 1465 to 5240 m a.s.l) were used to derive statistically relevant NPF features (frequency, formation rates, and growth rates) and seasonal variability. The combined information together with literature data showed that the frequencies of NPF events at the two Southern hemisphere (SH) stations are some of the highest reported thus far (64% and 67%, respectively). There are indications that NPF would be favored at a preferential altitude close to the interface of the free troposphere (FT) with the planetary boundary layer (PBL) and/or at the vicinity with clouds, which otherwise inhibit the occurrence of NPF. Particle formation rates are found to be lower at high altitudes than at low altitude sites, but a higher fraction of particles are formed via the charged pathway (mainly related to positive ions) compared to boundary layer (BL) sites. Low condensational sinks (CS) are not necessarily needed at high altitudes to promote the occurrence of NPF. For stations at altitudes higher than 1000 m a.s.l., higher CSs favor NPF and are thought to be associated with precursor gases needed to initiate nucleation and early growth.
Review of acp-2021-126
(2021) Diego Aliaga; Victoria A. Sinclair; Marcos Andrade; Paulo Artaxo; Samara Carbone; Evgeny Kadantsev; Paolo Laj; Alfred Wiedensohler; Radovan Krejčí; Federico Bianchi
Abstract. Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long-term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free-tropospheric air; however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high-altitude sites is required. Here we present a new method, based on the source–receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.; 16.35∘ S, 68.13∘ W) for the 6-month duration of the “Southern Hemisphere high-altitude experiment on particle nucleation and growth” (SALTENA) to identify where sampled air masses originate and to quantify the influence of the surface and the free troposphere. A key aspect of our method is that it is probabilistic, and for each observation time, more than one air mass (cluster) can influence the station, and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced by either boundary layer or free-troposphere air masses. Air sampled at CHC is a mix of different provenance. We find that on average 9 % of the air, at any given observation time, has been in contact with the surface within 4 d prior to arriving at CHC. Furthermore, 24 % of the air has been located within the first 1.5 km above ground level (surface included). Consequently, 76 % of the air sampled at CHC originates from the free troposphere. However, pure free-tropospheric influences are rare, and often samples are concurrently influenced by both boundary layer and free-tropospheric air masses. A clear diurnal cycle is present, with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29 % of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle, whereas the mid- and long-range clusters' (>200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km north-west from the station.
Reviewer comment
(2021) ClÃ©mence Rose; Martine Collaud Coen; Elisabeth Andrews; Yong Lin; Isaline Bossert; Cathrine Lund Myhre; Thomas Tuch; Alfred Wiedensohler; Markus Fiebig; Pasi P. Aalto
Abstract. Aerosol particles are a complex component of the atmospheric system which influence 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 (including wet and dry deposition), 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 less evident, 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 (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on 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.
Seasonality of the particle number concentration and size distribution: a global analysis retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
(Copernicus Publications, 2021) Clémence Rose; Martine Collaud Coen; Elisabeth Andrews; Yong Lin; Isaline Bossert; Cathrine Lund Myhre; Thomas Tuch; Alfred Wiedensohler; Markus Fiebig; Pasi P. Aalto
Abstract. Aerosol particles are a complex component of the atmospheric system which influence 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 (including wet and dry deposition), 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 less evident, 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 (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on 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.
Seasonality of the particle number concentration and sizedistribution: a global analysis retrieved from the network of GlobalAtmosphere Watch (GAW) near-surface observatories
(2021) Clémence Rose; Martine Collaud Coen; Elisabeth Andrews; Yong Lin; Isaline Bossert; Cathrine Lund Myhre; Thomas Tuch; Alfred Wiedensohler; Markus Fiebig; Pasi P. Aalto
Abstract. 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.
Supplementary material to "Seasonality of the particle number concentration and sizedistribution: a global analysis retrieved from the network of GlobalAtmosphere Watch (GAW) near-surface observatories"
(2021) Clémence Rose; Martine Collaud Coen; Elisabeth Andrews; Yong Lin; Isaline Bossert; Cathrine Lund Myhre; Thomas Tuch; Alfred Wiedensohler; Markus Fiebig; Tuula Aalto
The influence on Ntot of cut-off diameters different from 10 nm (either lower or higher) was evaluated based on measurements performed with MPSS detecting particles over broad enough size ranges and sufficient annual data availability (> 60%, See Sect. 4.1). The effect of including sub-10 nm particles in Ntot was investigated first: the ratio of the particle concentration in