Browsing by Autor "Alkuin Maximilian Koenig"

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Comment on egusphere-2022-1182
(2023) Qiaozhi Zha; Wei Huang; Diego Aliaga; Otso Peräkylä; Liine Heikkinen; Alkuin Maximilian Koenig; Cheng Wu; Joonas Enroth; Yvette Gramlich; Jing Cai
Air ions are the key components for a series of atmospheric physicochemical interactions, such as ion-catalyzed reactions, ion-molecule reactions, and ion-induced new particle formation. They also control atmospheric electrical properties with effects on global climate. We performed molecular-level measurements of cluster ions at the high-altitude research station Chacaltaya (CHC; 5240 m a.s.l.), located in the Bolivian Andes, from January to May 2018 using an atmospheric pressure interface time-of-flight mass spectrometer. The negative ions mainly consisted of (H2SO4)0–3•HSO4−, (HNO3)0–2•NO3−, SO5−, (NH3)1–6•(H2SO4)3–7•HSO4−, malonic acid-derived, and CHO/CHON•(HSO4−/NO3−) cluster ions. Their temporal variability exhibited distinct diurnal and seasonal patterns due to the changes in the corresponding neutral species’ molecular properties (such as electron affinity and proton affinity) and concentrations resulting from the air masses arriving at CHC from different source regions. The positive ions were mainly composed of protonated amines and organic cluster ions, but exhibited no clear diurnal variation. H2SO4-NH3 cluster ions likely contributed to the new particle formation process, particularly during wet-to-dry transition period and dry season when CHC was more impacted by air masses originating from source regions with elevated SO2 emissions. Our study provides new insights into the chemical composition of atmospheric cluster ions and their role in new particle formation in the high-altitude mountain environment of the Bolivian Andes.
Comment on egusphere-2022-1182
(2023) Qiaozhi Zha; Wei Huang; Diego Aliaga; Otso Peräkylä; Liine Heikkinen; Alkuin Maximilian Koenig; Cheng Wu; Joonas Enroth; Yvette Gramlich; Jing Cai
Air ions are the key components for a series of atmospheric physicochemical interactions, such as ion-catalyzed reactions, ion-molecule reactions, and ion-induced new particle formation. They also control atmospheric electrical properties with effects on global climate. We performed molecular-level measurements of cluster ions at the high-altitude research station Chacaltaya (CHC; 5240 m a.s.l.), located in the Bolivian Andes, from January to May 2018 using an atmospheric pressure interface time-of-flight mass spectrometer. The negative ions mainly consisted of (H2SO4)0–3•HSO4−, (HNO3)0–2•NO3−, SO5−, (NH3)1–6•(H2SO4)3–7•HSO4−, malonic acid-derived, and CHO/CHON•(HSO4−/NO3−) cluster ions. Their temporal variability exhibited distinct diurnal and seasonal patterns due to the changes in the corresponding neutral species' molecular properties (such as electron affinity and proton affinity) and concentrations resulting from the air masses arriving at CHC from different source regions. The positive ions were mainly composed of protonated amines and organic cluster ions, but exhibited no clear diurnal variation. H2SO4-NH3 cluster ions likely contributed to the new particle formation process, particularly during wet-to-dry transition period and dry season when CHC was more impacted by air masses originating from source regions with elevated SO2 emissions. Our study provides new insights into the chemical composition of atmospheric cluster ions and their role in new particle formation in the high-altitude mountain environment of the Bolivian Andes.
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.
Evidence for Interhemispheric Mercury Exchange in the Pacific Ocean Upper Troposphere
(Wiley, 2022) Alkuin Maximilian Koenig; Jeroen E. Sonke; Olivier Magand; Marcos Andrade; Isabel Moreno; Fernando Velarde; Ricardo Forno; René Gutierrez; Luis Blacutt; Paolo Laj
Abstract Even though anthropogenic mercury (Hg) emissions to the atmosphere are ∼2.5 times higher in the Northern Hemisphere (NH) than in the Southern Hemisphere (SH), atmospheric Hg concentrations in the NH are only ∼1.5 times higher than in the SH. Global Hg models attribute this apparent discrepancy to large SH oceanic Hg emissions or to interhemispheric exchange of Hg through the atmosphere. However, no observational data set exists to serve as a benchmark to validate whether these coarse‐resolution models adequately represent the complex dynamics of interhemispheric Hg exchange. During the 2015–2016 El Niño, we observed at mount Chacaltaya in the tropical Andes a ∼50% increase in ambient Hg compared to the year before, coinciding with a shift in synoptic transport pathways. Using this event as a case study, we investigate the impact of interhemispheric exchange on atmospheric Hg in tropical South America. We use HYSPLIT to link Hg observations to long‐range transport and find that the observed Hg increase relates strongly to air masses from the tropical Pacific upper troposphere (UT), a region directly impacted by interhemispheric exchange. Inclusion of the modeled seasonality of interhemispheric air mass exchange strengthens this relationship significantly. We estimate that interhemispheric exchange drives Hg seasonality in the SH tropical Pacific UT, with strongly enhanced Hg between July and October. We validate this seasonality with previously published aircraft Hg observations. Our results suggest that the transport of NH‐influenced air masses to tropical South America via the Pacific UT occurs regularly but became more detectable at Chacaltaya in 2015–2016 because of a westward shift in air mass origin.
Measurement report: Molecular-level investigation of atmospheric cluster ions at the tropical high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
(Copernicus Publications, 2023) Qiaozhi Zha; Wei Huang; Diego Aliaga; Otso Peräkylä; Liine Heikkinen; Alkuin Maximilian Koenig; Cheng Wu; Joonas Enroth; Yvette Gramlich; Jing Cai
Abstract. Air ions are the key components for a series of atmospheric physicochemical interactions, such as ion-catalyzed reactions, ion-molecule reactions, and ion-induced new particle formation (NPF). They also control atmospheric electrical properties with effects on global climate. We performed molecular-level measurements of cluster ions at the high-altitude research station Chacaltaya (CHC; 5240 m a.s.l.), located in the Bolivian Andes, from January to May 2018 using an atmospheric-pressure-interface time-of-flight mass spectrometer. The negative ions mainly consisted of (H2SO4)0–3⚫HSO4-, (HNO3)0–2⚫NO3-, SO5-, (NH3)1–6⚫(H2SO4)3–7⚫HSO4-, malonic-acid-derived, and CHO / CHON⚫(HSO4- / NO3-) cluster ions. Their temporal variability exhibited distinct diurnal and seasonal patterns due to the changes in the corresponding neutral species' molecular properties (such as electron affinity and proton affinity) and concentrations resulting from the air masses arriving at CHC from different source regions. The positive ions were mainly composed of protonated amines and organic cluster ions but exhibited no clear diurnal variation. H2SO4–NH3 cluster ions likely contributed to the NPF process, particularly during the wet-to-dry transition period and the dry season, when CHC was more impacted by air masses originating from source regions with elevated SO2 emissions. Our study provides new insights into the chemical composition of atmospheric cluster ions and their role in new particle formation in the high-altitude mountain environment of the Bolivian Andes.
Measurement report: Molecular-level investigation of atmospheric cluster ions at the tropical high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
(2022) Qiaozhi Zha; Wei Huang; Diego Aliaga; Otso Peräkylä; Liine Heikkinen; Alkuin Maximilian Koenig; Cheng Wu; Joonas Enroth; Yvette Gramlich; Jing Cai
Abstract. Air ions are the key components for a series of atmospheric physicochemical interactions, such as ion-catalyzed reactions, ion-molecule reactions, and ion-induced new particle formation. They also control atmospheric electrical properties with effects on global climate. We performed molecular-level measurements of cluster ions at the high-altitude research station Chacaltaya (CHC; 5240 m a.s.l.), located in the Bolivian Andes, from January to May 2018 using an atmospheric pressure interface time-of-flight mass spectrometer. The negative ions mainly consisted of (H2SO4)0–3•HSO4−, (HNO3)0–2•NO3−, SO5−, (NH3)1–6•(H2SO4)3–7•HSO4−, malonic acid-derived, and CHO/CHON•(HSO4−/NO3−) cluster ions. Their temporal variability exhibited distinct diurnal and seasonal patterns due to the changes in the corresponding neutral species’ molecular properties (such as electron affinity and proton affinity) and concentrations resulting from the air masses arriving at CHC from different source regions. The positive ions were mainly composed of protonated amines and organic cluster ions, but exhibited no clear diurnal variation. H2SO4-NH3 cluster ions likely contributed to the new particle formation process, particularly during wet-to-dry transition period and dry season when CHC was more impacted by air masses originating from source regions with elevated SO2 emissions. Our study provides new insights into the chemical composition of atmospheric cluster ions and their role in new particle formation in the high-altitude mountain environment of the Bolivian Andes.
Seasonal patterns of atmospheric mercury in tropical South America as inferred by a continuous total gaseous mercury record at Chacaltaya station (5240 m) in Bolivia
(Copernicus Publications, 2021) Alkuin Maximilian Koenig; Olivier Magand; Paolo Laj; Marcos Andrade; Isabel Moreno; Fernando Velarde; Grover Salvatierra; René Gutierrez; Luis Blacutt; Diego Aliaga
Abstract. High-quality atmospheric mercury (Hg) data are rare for South America, especially for its tropical region. As a consequence, mercury dynamics are still highly uncertain in this region. This is a significant deficiency, as South America appears to play a major role in the global budget of this toxic pollutant. To address this issue, we performed nearly 2 years (July 2014–February 2016) of continuous high-resolution total gaseous mercury (TGM) measurements at the Chacaltaya (CHC) mountain site in the Bolivian Andes, which is subject to a diverse mix of air masses coming predominantly from the Altiplano and the Amazon rainforest. For the first 11 months of measurements, we obtained a mean TGM concentration of 0.89±0.01 ng m−3, which is in good agreement with the sparse amount of data available from the continent. For the remaining 9 months, we obtained a significantly higher TGM concentration of 1.34±0.01 ng m−3, a difference which we tentatively attribute to the strong El Niño event of 2015–2016. Based on HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) back trajectories and clustering techniques, we show that lower mean TGM concentrations were linked to either westerly Altiplanic air masses or those originating from the lowlands to the southeast of CHC. Elevated TGM concentrations were related to northerly air masses of Amazonian or southerly air masses of Altiplanic origin, with the former possibly linked to artisanal and small-scale gold mining (ASGM), whereas the latter might be explained by volcanic activity. We observed a marked seasonal pattern, with low TGM concentrations in the dry season (austral winter), rising concentrations during the biomass burning (BB) season, and the highest concentrations at the beginning of the wet season (austral summer). With the help of simultaneously sampled equivalent black carbon (eBC) and carbon monoxide (CO) data, we use the clearly BB-influenced signal during the BB season (August to October) to derive a mean TGM / CO emission ratio of (2.3±0.6)×10-7 ppbvTGM ppbvCO-1, which could be used to constrain South American BB emissions. Through the link with CO2 measured in situ and remotely sensed solar-induced fluorescence (SIF) as proxies for vegetation activity, we detect signs of a vegetation sink effect in Amazonian air masses and derive a “best guess” TGM / CO2 uptake ratio of 0.058 ±0.017 (ng m−3)TGM ppmCO2-1. Finally, significantly higher Hg concentrations in western Altiplanic air masses during the wet season compared with the dry season point towards the modulation of atmospheric Hg by the eastern Pacific Ocean.
Seasonal patterns of atmospheric mercury in tropical South America as inferred by a TGM continuous record at the Chacaltaya Station (5240 m) in Bolivia
(2020) Alkuin Maximilian Koenig; Olivier Magand; Paolo Laj; Marcos Andrade; Isabel Moreno; Fernando Velarde; Grover Salvatierra; René Gutierrez; Luis Blacutt; Diego Aliaga
Abstract. High-quality data of atmospheric mercury (Hg) is rare for South America, especially for its tropical part. In consequence, mercury dynamics are still highly uncertain in this region, a significant deficiency, as South America appears to play a major role in the global budget of this toxic pollutant. To address this issue, we performed nearly two years (July 2014–February 2016) of continuous high resolution total gaseous mercury (TGM) measurements at the Chacaltaya (CHC) mountain site in the Bolivian Andes, which is subject to a diverse mix of air masses coming predominantly from the Altiplano and the Amazon rainforest. For the first eleven months of measurements, we obtained a mean TGM concentration of 0.89±0.01 ng m−3, in good agreement with the sparse amount of data available from the continent. For the remaining nine months, we obtained a significantly higher TGM concentration of 1.34±0.01 ng m−3, a difference which we tentatively attribute to the strong El Niño event of 2015–2016. Based on HYSPLIT back-trajectories and clustering techniques, we show that lower mean TGM concentrations were linked to either westerly Altiplanic air masses or those originating from the lowlands to the south-east of CHC. Elevated TGM concentrations were related to northerly air masses of Amazonian or southerly air masses of Altiplanic origin, the former possibly linked to artisanal and small scale gold mining (ASGM), while the latter might be explained by volcanic activity. We observed a marked seasonal pattern, with low TGM concentrations in the dry season (austral winter), rising concentrations during biomass burning (BB) season, and highest concentrations at the beginning of the wet season (austral summer). With the help of simultaneously sampled equivalent black carbon (eBC) and carbon monoxide (CO) data, we use the clearly BB influenced signal during BB season (August to October) to derive a mean TGM/CO emission ratio of (2.3±0.6)·10−7 ppbvTGM ppbvCO−1, which could be used to constrain South American BB emissions. Through the link with in-situ measured CO2 and remotely sensed solar-induced fluorescence (SIF) as proxies for vegetation activity, we detect signs of a vegetation sink effect in Amazonian air masses and derive a best guess TGM/CO2 uptake ratio of 0.058±0.017 (ng m−3)TGM ppmCO2−1. Finally, significantly higher Hg concentrations in western Altiplanic air masses during the wet season as compared to the dry season point towards the modulation of atmospheric Hg by the Eastern Pacific Ocean.
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.