Browsing by Autor "Radovan Krejčí"

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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;
Analysis of atmospheric particle growth based on vapor concentrations measured at the high-altitude GAW station Chacaltaya in the Bolivian Andes
(2023) Arto Heitto; Cheng Wu; Diego Aliaga; Luis Blacutt; Xuemeng Chen; Yvette Gramlich; Liine Heikkinen; Wei Huang; Radovan Krejčí; Paolo Laj
Abstract. Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at Chacaltaya Global Atmosphere Watch station in Bolivia (5240 m a.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign . The simulations showed that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modelled and measured particle growth rates. This study gives an insight on the key factors affecting the particle growth on the site. Low volatile organic compounds were found to be the main contributor to the particle growth, covering on average 65 % of simulated particle mass in particle with diameter of 40 nm In addition, sulfuric acid had a major contribution to the particle growth, covering at maximum 39 % of simulated particle mass in 40 nm particle during periods when volcanic activity was detected on the area, suggesting that volcanic emissions can greatly enhance the particle growth.
Analysis of atmospheric particle growth based on vapor concentrations measured at the high-altitude GAW station Chacaltaya in the Bolivian Andes
(Copernicus Publications, 2024) Arto Heitto; Cheng Wu; Diego Aliaga; Luis Blacutt; Xuemeng Chen; Yvette Gramlich; Liine Heikkinen; Wei Huang; Radovan Krejčí; Paolo Laj
Abstract. Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at the Chacaltaya Global Atmosphere Watch station in Bolivia (5240 m a.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign. Despite the challenging topography and ambient conditions around the station, the simple particle growth model used in the study was able to show that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modeled and measured particle growth rates. This study, one of the first of such studies conducted on high altitude, gives insight on the key factors affecting the particle growth on the site and helps to improve the understanding of important factors on high-altitude sites and the atmosphere in general. Low-volatility organic compounds originating from multiple surrounding sources such as the Amazonia and La Paz metropolitan area were found to be the main contributor to the particle growth, covering on average 65 % of the simulated particle mass in particles with a diameter of 30 nm. In addition, sulfuric acid made a major contribution to the particle growth, covering at maximum 37 % of the simulated particle mass in 30 nm particles during periods when volcanic activity was detected on the area, compared to around 1 % contribution on days without volcanic activity. This suggests that volcanic emissions can greatly enhance the particle growth.
Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240 m a.s.l.)
(Copernicus Publications, 2019) Aurélien Chauvigné; Diego Aliaga; Karine Sellegri; Nadège Montoux; Radovan Krejčí; Griša Močnik; Isabel Moreno; Thomas Müller; Marco Pandolfi; Fernando Velarde
Abstract. This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz–El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm−1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm−1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm−1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz–El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.
Biomass-burning and urban emission impacts in the Andes Cordillera region based on in-situ measurements from the Chacaltaya observatory, Bolivia (5240 m a.s.l.)
(2019) Chauvigné Aurélien; Diego Aliaga; Marcos Andrade; Patrick Ginot; Radovan Krejčí; Griša Močnik; Nadège Montoux; Isabel Moreno; Thomas Müller; Marco Pandolfi
Abstract. We present the variability of aerosol particle optical properties measured at the global Atmosphere Watch (GAW) station Chacaltaya (5240 m a.s.l.). The in-situ mountain site is ideally located to study regional impacts of the densely populated urban area of La Paz/El Alto, and the intensive activity in the Amazonian basin. Four year measurements allow to study aerosol particle properties for distinct atmospheric conditions as stable and turbulent layers, different airmass origins, as well as for wet and dry seasons, including biomass-burning influenced periods. The absorption, scattering and extinction coefficients (median annual values of 0.74, 12.14 and 12.96 Mm−1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94 and 8.68 Mm−1 respectively) and higher values during the dry season (0.80, 11.23 and 14.51 Mm−1 respectively). These parameters also show a pronounced diurnal variation (maximum during daytime, minimum during night-time, as a result of the dynamic and convective effects of leading to lower atmospheric layers reaching the site during daytime. Retrieved intensive optical properties are significantly different from one season to the other, showing the influence of different sources of aerosols according to the season. Both intensive and extensive optical properties of aerosols were found to be different among the different atmospheric layers. The particle light absorption, scattering and extinction coefficients are in average 1.94, 1.49 and 1.55 times higher, respectively, in the turbulent layer compared to the stable layer. We observe that the difference is highest during the wet season and lowest during the dry season. Using wavelength dependence of aerosol particle optical properties, we discriminated contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass-burning and urban transport or industries) emissions according to seasons and tropospheric layers. The main sources influencing measurements at CHC are arising from the urban area of La Paz/El Alto, and regional biomass-burning from the Amazonian basin. Results show a 28 % to 80 % increase of the extinction coefficients during the biomass-burning season with respect to the dry season, which is observed in both tropospheric layers. From this analyse, long-term observations at CHC provides the first direct evidence of the impact of emissions in the Amazonian basin on atmospheric optical properties far away from their sources, all the way to the stable layer.
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.
Comment on egusphere-2023-1298
(2023) Isabel Moreno; Radovan Krejčí; Jean‐Luc Jaffrezo; Gaëlle Uzu; Andrés Alástuey; Marcos Andrade; Valeria Mardóñez; Alkuin Maximilian Koenig; Diego Aliaga; Claudia Mohr
Abstract. The chemical composition of PM10 and PM2.5 was studied at the summit of Mt. Chacaltaya (5380 masl, lat.-16.346950º, lon. -68.128250º) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya GAW site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz – El Alto. Concentration levels are clearly influenced by seasons with minimum occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC+OC) and saccharide concentrations range between 558–1785, 384–1120 and 4.3–25.5 ng m-3 for bulk PM10 and 917–2308, 519–1175 and 3.9–24.1 ng m-3 for PM2.5, respectively. Such concentrations are overall lower compared to other high-altitude stations around the globe, but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33–56 % of the mass), organic matter (7–34 %) and secondary inorganic aerosol (15–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, C2O4-2 for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formiate, levoglucosan, some F- and Br- for biomass burning; MeSO3-, Na+, Mg2+, Br- for aged marine emissions from the Pacific Ocean; arabitol, mannitol, K+ for biogenic emissions; Na+, Ca2+, Mg2+ for soil dust, and SO42-, F-, and some Cl- for volcanism. Regional biomass-burning practices influence the soluble fraction of the aerosol particularly between July and September. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5±38.9). Peruvian volcanism dominates the SO42- concentration since 2014, though it presents a strong temporal variability due to the intermittence of the sources and seasonal changes on the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern hemisphere.
Comment on egusphere-2023-1298
(2023) Isabel Moreno; Radovan Krejčí; Jean‐Luc Jaffrezo; Gaëlle Uzu; Andrés Alástuey; Marcos Andrade; Valeria Mardóñez; Alkuin Maximilian Koenig; Diego Aliaga; Claudia Mohr
Abstract. The chemical composition of PM10 and PM2.5 was studied at the summit of Mt. Chacaltaya (5380 masl, lat.-16.346950º, lon. -68.128250º) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya GAW site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz – El Alto. Concentration levels are clearly influenced by seasons with minimum occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC+OC) and saccharide concentrations range between 558–1785, 384–1120 and 4.3–25.5 ng m-3 for bulk PM10 and 917–2308, 519–1175 and 3.9–24.1 ng m-3 for PM2.5, respectively. Such concentrations are overall lower compared to other high-altitude stations around the globe, but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33–56 % of the mass), organic matter (7–34 %) and secondary inorganic aerosol (15–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, C2O4-2 for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formiate, levoglucosan, some F- and Br- for biomass burning; MeSO3-, Na+, Mg2+, Br- for aged marine emissions from the Pacific Ocean; arabitol, mannitol, K+ for biogenic emissions; Na+, Ca2+, Mg2+ for soil dust, and SO42-, F-, and some Cl- for volcanism. Regional biomass-burning practices influence the soluble fraction of the aerosol particularly between July and September. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5±38.9). Peruvian volcanism dominates the SO42- concentration since 2014, though it presents a strong temporal variability due to the intermittence of the sources and seasonal changes on the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern hemisphere.
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
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.
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 dynamics in the central Andes: Contrasting urban and mountain-top environments
(2024) Diego Aliaga; Victoria A. Sinclair; Radovan Krejčí; Marcos Andrade; Paulo Artaxo; Luis Blacutt; Runlong Cai; Samara Carbone; Yvette Gramlich; Liine Heikkinen
Abstract. In this study, we investigate atmospheric new particle formation (NPF) across 65 days in the Bolivian Central Andes at two locations: the mountain-top Chacaltaya station (CHC, 5.2 km above sea level) and an urban site in El Alto-La Paz (EAC), 19 km apart and at 1.1 km lower altitude. We categorize days into four groups based on NPF intensity, determined with the daily maximum concentration of 4–7 nm particles: (A) high at both sites, (B) medium at both, (C) high at EAC but low at CHC, (D) and low at both. This categorization was premised on the assumption that similar NPF intensities imply similar atmospheric processes. Our findings show significant differences across the categories in terms of particle size and volume, precursor gases, aerosol compositions, pollution levels, meteorological conditions, and air mass origins. Specifically, intense NPF events (A) increased Aitken-mode particle concentrations (14–100 nm) significantly on 28 % of the days when air masses passed over the Altiplano. At CHC, larger Aitken-mode particle concentrations (40–100 nm) increased from 1.1×103 cm-3 (background) to 6.2×103 cm-3 very likely linked to the ongoing NPF process. High pollution levels from urban emissions on 24 % of the days (B) were found to interrupt particle growth at CHC and diminish nucleation at EAC. Meanwhile, on 14 % of the days, high concentrations of sulphate and large particle volumes (C) were observed, correlating with significant influences from air masses originating from the actively degassing Sabancaya Volcano and a depletion of positive 2–4 nm ions at CHC. During these days, reduced NPF intensity was observed at CHC but not at EAC. The study highlights the role of NPF in modifying atmospheric particles and underscores the varying impacts of urban versus mountain-top environments on particle formation processes in the Andean region.
New particle formation dynamics in the central Andes: contrasting urban and mountaintop environments
(2025) Diego Aliaga; Victoria A. Sinclair; Radovan Krejčí; Marcos Andrade; Paulo Artaxo; Luis Blacutt; Runlong Cai; Samara Carbone; Yvette Gramlich; Liine Heikkinen
Abstract. In this study, we investigate atmospheric new particle formation (NPF) across 65 d in the Bolivian central Andes at two locations: the mountaintop Chacaltaya station (CHC, 5.2 km above sea level) and an urban site in El Alto–La Paz (EAC), 19 km apart and at 1.1 km lower altitude. We classified the days into four categories based on the intensity of NPF, determined by the daily maximum concentration of 4–7 nm particles: (1) high at both sites, (2) medium at both, (3) high at EAC but low at CHC, and (4) low at both. These categories were then named after their emergent and most prominent characteristics: (1) Intense-NPF, (2) Polluted, (3) Volcanic, and (4) Cloudy. This classification was premised on the assumption that similar NPF intensities imply similar atmospheric processes. Our findings show significant differences across the categories in terms of particle size and volume, sulfuric acid concentration, aerosol compositions, pollution levels, meteorological conditions, and air mass origins. Specifically, intense NPF events (1) increased Aitken mode particle concentrations (14–100 nm) significantly on 28 % of the days when air masses passed over the Altiplano. At CHC, larger Aitken mode particle concentrations (40–100 nm) increased from 1.1 × 103 cm−3 (background) to 6.2 × 103 cm−3, and this is very likely linked to the ongoing NPF process. High pollution levels from urban emissions on 24 % of the days (2) were found to interrupt particle growth at CHC and diminish nucleation at EAC. Meanwhile, on 14 % of the days, high concentrations of sulfate and large particle volumes (3) were observed, correlating with significant influences from air masses originating from the actively degassing Sabancaya volcano and a depletion of positive 2–4 nm ions at CHC but not at EAC. During these days, reduced NPF intensity was observed at CHC but not at EAC. Lastly, on 34 % of the days, overcast conditions (4) were associated with low formation rates and air masses originating from the lowlands east of the stations. In all cases, event initiation (∼ 09:00 LT) generally occurred about half an hour earlier at CHC than at EAC and was likely modulated by the daily solar cycle. CHC at dawn is in an air mass representative of the regional residual layer with minimal local surface influence due to the barren landscape. As the day progresses, upslope winds bring in air masses affected by surface emissions from lower altitudes, which may include anthropogenic or biogenic sources. This influence likely develops gradually, eventually creating the right conditions for an NPF event to start. At EAC, the start of NPF was linked to the rapid growth of the boundary layer, which favored the entrainment of air masses from above. The study highlights the role of NPF in modifying atmospheric particles and underscores the varying impacts of urban versus mountain top environments on particle formation processes in the Andean region.
Oxidized organic molecules in the tropical free troposphere over Amazonia
(Oxford University Press, 2023) Qiaozhi Zha; Diego Aliaga; Radovan Krejčí; Victoria A. Sinclair; Cheng Wu; Giancarlo Ciarelli; Wiebke Scholz; Liine Heikkinen; Eva Partoll; Yvette Gramlich
New particle formation (NPF) in the tropical free troposphere (FT) is a globally important source of cloud condensation nuclei, affecting cloud properties and climate. Oxidized organic molecules (OOMs) produced from biogenic volatile organic compounds are believed to contribute to aerosol formation in the tropical FT, but without direct chemical observations. We performed in situ molecular-level OOMs measurements at the Bolivian station Chacaltaya at 5240 m above sea level, on the western edge of Amazonia. For the first time, we demonstrate the presence of OOMs, mainly with 4-5 carbon atoms, in both gas-phase and particle-phase (in terms of mass contribution) measurements in tropical FT air from Amazonia. These observations, combined with air mass history analyses, indicate that the observed OOMs are linked to isoprene emitted from the rainforests hundreds of kilometers away. Based on particle-phase measurements, we find that these compounds can contribute to NPF, at least the growth of newly formed nanoparticles, in the tropical FT on a continental scale. Thus, our study is a fundamental and significant step in understanding the aerosol formation process in the tropical FT.
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.
Source region cluster analysis in the high-altitude measuring site of Chacaltaya with WRF and FLEXPART
(2020) Diego Aliaga; Victoria A. Sinclair; Qiaozhi Zha; Marcos Andrade; Claudia Mohr; Radovan Krejčí
&lt;p&gt;Measuring aerosol at high altitude sites is useful as it enables sampling of the free troposphere over long time frames. However, in order to draw conclusions from station measurement data, we need to determine which air mass sources are present at any given sampling time. This task is challenging at mountain sites, due to complex topography which in turn drives complex meteorology. Between December 2017 and May 2018, the Southern hemisphere high ALTitude Experiment on particle Nucleation And growth (SALTENA) campaign was conducted at Chacaltaya in Bolivia at 5240 m a.s.l. The data set obtained in this campaign contains records of nearly all relevant aerosol characteristics and aerosol precursors. To identify the source regions of the observed air masses we performed high resolution (down to 1 km) simulations with the Weather Research and Forecasting Model (WRF). The WRF model output is then used to as input to the Lagrangian particle dispersion model (FLEXPART). FLEXPART simulations are initialised every hour and 20 thousand particles are released per hour and track backwards in time for 96 hours. The FLEXPART footprint output is regridded onto a log-polar cylindrical grid where we perform a &amp;#8216;K-means&amp;#8217; cluster analysis on the 3D cells defined by the grid. The cells are clustered based on the time series of their source receptor relationship (i.e. emission sensitivities), producing regions (clusters) resolved not only in the horizontal but also the vertical domain. Our results show that regions located close to the station (&lt;100km) have a low but persistent influence with diurnal variations and close contact to the surface. Mid-range regions (100-800km) have the highest influence with a higher percentage of air masses from the free troposphere. Long-range regions (&gt;800km) have a higher influence than the short-range regions but lower than the middle-range regions. Most of the air masses from these long-range regions come from the free troposphere. With this method we have successfully resolved the various air mass influences at the measurement site. The high meteorological resolution and the stochastic nature of FLEXPART are seminal for capturing the transport pathways.&lt;/p&gt;
Tropical tropospheric aerosol sources and chemical composition observed at high altitude in the Bolivian Andes
(Copernicus Publications, 2024) Isabel Moreno; Radovan Krejčí; Jean‐Luc Jaffrezo; Gaëlle Uzu; Andrés Alástuey; Marcos Andrade; Valeria Mardóñez; Alkuin Maximilian Koenig; Diego Aliaga; Claudia Mohr
Abstract. The chemical composition of PM10 and non-overlapping PM2.5 was studied at the summit of Mt. Chacaltaya (5380 m a.s.l., lat. −16.346950°, long. −68.128250°) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya Global Atmosphere Watch (GAW) site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz–El Alto. Concentration levels are clearly influenced by seasons with minima occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC + OC), and saccharide interquartile ranges for concentrations are 558–1785, 384–1120, and 4.3–25.5 ng m−3 for bulk PM10 and 917–2308, 519–1175, and 3.9–24.1 ng m−3 for PM2.5, respectively, with most of the aerosol seemingly present in the PM2.5 fraction. Such concentrations are overall lower compared to other high-altitude stations around the globe but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33 %–56 % of the mass), organic matter (7 %–34 %), and secondary inorganic aerosol (15 %–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, and C2O42- for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formate, levoglucosan, and some F− and Br− for biomass burning; MeSO3-, Na+, Mg2+, K+, and Ca2+ for aged marine emissions from the Pacific Ocean; arabitol, mannitol, and glucose for biogenic emissions; Na+, Ca2+, Mg2+, and K+ for soil dust; and SO42-, F−, and some Cl− for volcanism. Regional biomass burning practices influence the soluble fraction of the aerosol between June and November. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5 ± 5.7, IQR 8.1–13.3). Peruvian volcanism has dominated the SO42- concentration since 2014, though it presents strong temporal variability due to the intermittence of the sources and seasonal changes in the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern Hemisphere.
Tropical tropospheric aerosol sources and chemical composition observed at high-altitude in the Bolivian Andes
(2023) Isabel Moreno; Radovan Krejčí; Jean‐Luc Jaffrezo; Gaëlle Uzu; Andrés Alástuey; Marcos Andrade; Valeria Mardóñez; Alkuin Maximilian Koenig; Diego Aliaga; Claudia Mohr
Abstract. The chemical composition of PM10 and PM2.5 was studied at the summit of Mt. Chacaltaya (5380 masl, lat.-16.346950º, lon. -68.128250º) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya GAW site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz – El Alto. Concentration levels are clearly influenced by seasons with minimum occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC+OC) and saccharide concentrations range between 558–1785, 384–1120 and 4.3–25.5 ng m-3 for bulk PM10 and 917–2308, 519–1175 and 3.9–24.1 ng m-3 for PM2.5, respectively. Such concentrations are overall lower compared to other high-altitude stations around the globe, but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33–56 % of the mass), organic matter (7–34 %) and secondary inorganic aerosol (15–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, C2O4-2 for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formiate, levoglucosan, some F- and Br- for biomass burning; MeSO3-, Na+, Mg2+, Br- for aged marine emissions from the Pacific Ocean; arabitol, mannitol, K+ for biogenic emissions; Na+, Ca2+, Mg2+ for soil dust, and SO42-, F-, and some Cl- for volcanism. Regional biomass-burning practices influence the soluble fraction of the aerosol particularly between July and September. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5±38.9). Peruvian volcanism dominates the SO42- concentration since 2014, though it presents a strong temporal variability due to the intermittence of the sources and seasonal changes on the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern hemisphere.