Browsing by Autor "Kay Weinhold"

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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)
(European Organization for Nuclear Research, 2018) A. Wiedensohler; Manuel Olivera 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; 5240m 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 (4040m a.s.l.) can be seen as representative of the urban and Altiplano background, the road site located in Central La Paz (3590m a.s.l.) is representative for heavy traffic-dominated conditions. Peaks of eBC mass concentrations up to 5 μgm−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 μgm−3. A complete traffic ban on the specific Bolivian Day of Census (November 21, 2012) led to a decrease of eBC below 1 μgm−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.
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.
Frequent nucleation events at the high altitude station of Chacaltaya (5240 m a.s.l.), Bolivia
(Elsevier BV, 2014) Clémence Rose; Karine Sellegri; Fernando Velarde; Isabel Moreno; Michel Ramonet; Kay Weinhold; Radovan Krejčí; Patrick Ginot; Marcos Andrade; A. Wiedensohler
Mobility Particle Size Spectrometers: Calibration Procedures And Measurement Uncertainties
(European Organization for Nuclear Research, 2017) A. Wiedensohler; A. Wiesner; Kay Weinhold; W. Birmili; M. Hermann; Maik Merkel; Thomas Müller; Sascha Pfeifer; Andres Schmidt; T. 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.
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.