Browsing by Autor "Cheng Wu"

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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.
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.
Data and Code for figures of "Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes"
(European Organization for Nuclear Research, 2022) Wiebke Scholz; Jiali Shen; Diego Aliaga; Cheng Wu; Samara Carbone; Isabel Moreno; Qiaozhi Zha; Wei Huang; Liine Heikkinen; Jean‐Luc Jaffrezo
This database includes the material to create the figures in "Measurement Report: Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes" and the analyzed time series of all atmospheric variables presented.
Data and Code for figures of "Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes"
(2022) Wiebke Scholz; Jiali Shen; Diego Aliaga; Cheng Wu; Samara Carbone; Isabel Moreno; Qiaozhi Zha; Wei Huang; Liine Heikkinen; Jean‐Luc Jaffrezo
This database includes the material to create the figures in "Measurement Report: Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes" and the analyzed time series of all atmospheric variables presented.
Data and Code for figures of "Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes"
(European Organization for Nuclear Research, 2022) Wiebke Scholz; Jiali Shen; Diego Aliaga; Cheng Wu; Samara Carbone; Isabel Moreno; Qiaozhi Zha; Wei Huang; Liine Heikkinen; Jean‐Luc Jaffrezo
This database includes the material to create the figures in "Measurement Report: Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes" and the analyzed time series of all atmospheric variables presented.
Direct high-altitude observations of 2-methyltetrols in the gas- and particle phase in air masses from Amazonia
(Royal Society of Chemistry, 2025) Claudia Mohr; Joel A. Thornton; Manish Shrivastava; Anouck Chassaing; Ilona Riipinen; Federico Bianchi; Marcos Andrade; Cheng Wu
We present direct observations of 2-methyltetrol (C5H12O4) in the gas- and particle phase from the deployment of a Filter Inlet for Gases and Aerosols coupled to a Time-of-Flight Chemical Ionization Mass Spectrometer (FIGAERO-CIMS) during the Southern Hemisphere High Altitude Experiment on Particle Nucleation and Growth (SALTENA), which took place between December 2017 and June 2018 at the high-altitude Global Atmosphere Watch station Chacaltaya (CHC) located at 5240 m a s l in the Bolivian Andes. 2-Methyltetrol signals were dominant in a factor resulting from Positive Matrix Factorization (PMF) identified as influenced by Amazon emissions. We combine these observations with investigations of isoprene oxidation chemistry and uptake in an isolated deep convective cloud in the Amazon using a photochemical box model with coupled cloud microphysics and show that, likely, 2-methyltetrol is taken up by hydrometeors or formed in situ in the convective cloud, and then transported in the particle phase in the cold environment of the Amazon outflow and to the station, where it partially evaporates.
Measurement Report: Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
(2022) Wiebke Scholz; Jiali Shen; Diego Aliaga; Cheng Wu; Samara Carbone; Isabel Moreno; Qiaozhi Zha; Wei Huang; Liine Heikkinen; Jean‐Luc Jaffrezo
Abstract. Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products H2SO4, MSA, DMSO, DMSO2, MSIA, MTF, CH3S(O)2OOH and CH3SOH in the gas-phase as well as measurements of the sulfate and methane- sulfonate aerosol mass fractions at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs dimethyl sulfone (DMSO2) in the gas phase and methanesulfonate (MS−) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethyl sulfoxide, and methane sulfinic acid. Also for this event, backtrajectory calculations show, that the air masses came from above the ocean (distance >330 km) with no local sur- face contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.
Measurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
(Copernicus Publications, 2023) Wiebke Scholz; Jiali Shen; Diego Aliaga; Cheng Wu; Samara Carbone; Isabel Moreno; Qiaozhi Zha; Wei Huang; Liine Heikkinen; Jean‐Luc Jaffrezo
Abstract. Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)2OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS−) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance >330 km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.
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.
Molecular characterization and volatility of organonitrates: Latest observations from field and laboratory
(2020) Claudia Mohr; Cheng Wu; Huang Wei; Emelie Graham; Federico Bianchi; Marcos Andrade; David M. Bell
&lt;p&gt;Here we show recent results from different field and laboratory campaigns focusing on organonitrate (ON) formation, mass concentration, and physicochemical properties such as volatility. ONs are formed via volatile organic compounds (VOC) and NO&lt;sub&gt;x&lt;/sub&gt;. They are therefore key species for our understanding of the interaction between the biosphere and anthropogenic activities, and the effects of altering both VOC and NO&lt;sub&gt;x&lt;/sub&gt; emissions due to climate change and/or air quality mitigation measures. Recently, we were able to show that ONs from different precursor VOC can also contribute significantly to the growth of newly formed particles in the atmosphere to sizes where they can become active and cloud condensation nuclei (Huang et al., 2019).&lt;/p&gt;&lt;p&gt;We present direct, real-time observations of ONs in the gas and particle phase at the highest atmospheric research station in the world, Chacaltaya (5240 m a. s. l) in Bolivia. This southern hemisphere station is often located in the free troposphere during night time, and influenced by the emissions from the nearby El Alto-La Paz metropolitan area, and biogenic emissions from surrounding forests as well as from the Amazon through long-range transport. ONs were measured using a Chemical Ionization Mass Spectrometer with a Filter Inlet for Gases and Aerosols. We observed hundreds of highly functionalized ONs with different molecular composition during day- and nighttime, indicating different sources and formation processes. A large contribution of the highly functionalized ONs was found especially during new particle formation events regularly observed at this location (Rose et al., 2015). Observations from the field will be compared to results from the Nitrate Aerosol and Volatility Experiment (NArVE) at the EUROCHAMP 2020 PACS-C3 smog chamber (PSI, Switzerland), where we investigated the ON fraction, chemical composition, and volatility of secondary organic aerosol (SOA) formed via nitrate radical initiated oxidation reactions of biogenic and anthropogenic VOC.&lt;/p&gt;
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.
Polychlorinated Alkane Profiles and Concentrations in Bolivian Andes Soils Point to a Long-Range Transport Influence
(American Chemical Society, 2026) Bo Yuan; Cheng Wu; Cynthia A. de Wit; Claudia Mohr; Marcos Andrade; Isabel Moreno; Volker Brüchert; Rienk H. Smittenberg; Matthew MacLeod
High-altitude terrain may intersect the upper atmospheric boundary layer and exhibit distinct environmental dynamics. We investigated the anthropogenic pollutants polychlorinated alkanes (PCAs, also known as chlorinated paraffins) in surface soils along a transect from the La Paz-El Alto metropolitan area in Bolivia (3200-4100 masl) to the upper slopes of Mount Chacaltaya (>5200 masl), around 16 km away. Concentrations of PCAs in urban soils (750-5,230 ng/g organic carbon [OC]) decreased exponentially with increasing distance from the urban boundary, declining to ∼150 ng/g OC at elevations below 4,700 masl. Beyond 4,700 masl concentrations increased again, reaching levels comparable to those in the urban area, 1,670-4,300 ng/g OC, above 5,000 masl. Given that pollutant concentrations typically decline with distance from their source, this altitudinal trend, together with a pronounced shift in PCA forensic fingerprints near 4,700 masl, strongly suggests contributions from sources beyond the local metropolitan area. Carbon and nitrogen isotope signatures in organic carbon further support long-range transport as a source, consistent with previous modeling and observations that the upper slopes of Mount Chacaltaya predominantly receive air masses and organic carbon from distant regions via transport in the free troposphere. Our observation that pollutant levels in high-altitude areas are comparable to those in the metropolis of 1.8-million inhabitants underscores the efficiency of long-range atmospheric transport.
Quantifying the effect of SVOC condensation on cloud droplet number in different airmass types
(2020) Liine Heikkinen; Samuel Lowe; Cheng Wu; Diego Aliaga; Wei Huang; Yvette Gramlich; Samara Carbone; Qiaozhi Zha; Fernando Velarde; Valeria Mardóñez
&lt;p&gt;Clouds are made of droplets that arise from the activation of suitable aerosol particles (termed cloud condensation nuclei, CCN). In the activation process, water vapor saturation ratio exceeds a critial ratio enabling CCN runaway-growth to cloud droplet sizes. The number concentration of cloud droplets (CDNC) is highly dependent on the aerosol population properties (size distribution and composition), relative humidity, and the vertical wind component. While the activation of CCN consisting of non-volatile particulate matter is fairly well understood, the same process involving semi-volatile organic vapors (SVOCs) has received less attention despite their significant presence in ambient air. A recent cloud parcel modeling study shows substanial CDNC enhancement due to SVOC condensation (Topping &lt;em&gt;et al&lt;/em&gt;., 2013). Surprisingly, the topic has not been widely investigated nor the results replicated with other cloud parcel models (CPM). Thus, in the current study we seek to quantify the CDNC enhancement by SVOC condensation using a recently developed CPM framework (Lowe &lt;em&gt;et al.&lt;/em&gt;, 2020, &lt;em&gt;in prep&lt;/em&gt;.). Moreover, the CPM initialization is performed, for the first time, with state-of-the art measurement data including measured SVOC data for multiple airmass types.&lt;/p&gt;&lt;p&gt;Here, the CPM, which uses spectral microphysics for the simulation of CCN activation and hydrometeor growth, also includes a SVOC condensation equation analogous to those of water vapor. Equilibrium initialization of the SVOC volatility basis set (VBS) partitioning coefficients is performed iteratively, and constrained by the organic to inorganic ratio in the particle phase determined by ambient measurements performed at the Chacaltaya Global Atmospheric Watch (GAW) Station located at 5240 m a.s.l. in the Bolivian Andes, in spring 2018. The uniquely comprehensive data set recorded, which tracks all of the relevant aerosol population characteristics in near real-time, reveals a high degree of variability in aerosol composition, size distribution and loading depending on the air mass origin. Lagrangian backward simulations during the measurement period at Chacaltaya GAW reveal at least 18 significantly different airmass origins (Aliaga &lt;em&gt;et al.&lt;/em&gt;, 2020, &lt;em&gt;in prep.&lt;/em&gt;). Such variability served multiple model initialization scenarios for individual case studies. We will show a suite of CDNC enhancements by SVOC condensation under different initialization scenarios actualized in data recorded at Chacaltaya GAW Station, including airmasses originating from the Amazon (biomass burning and biogenic VOCs), Andean plateau (volcanic activity), and La Paz/El Alto metropolitan areas (anthropogenic emissions).&lt;/p&gt;&lt;p&gt;&lt;strong&gt;References:&lt;/strong&gt;&lt;/p&gt;&lt;div&gt;Topping, D., Connolly, P. and McFiggans, G., 2013. Cloud droplet number enhanced by co-condensation of organic vapours. &lt;em&gt;Nature Geoscience&lt;/em&gt;, &lt;em&gt;6&lt;/em&gt;(6), p.443.&lt;/div&gt;
Referee comment on egusphere-2022-887
(2022) Wiebke Scholz; Jiali Shen; Diego Aliaga; Cheng Wu; Samara Carbone; Isabel Moreno; Qiaozhi Zha; Wei Huang; Liine Heikkinen; Jean‐Luc Jaffrezo
Abstract. Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products H2SO4, MSA, DMSO, DMSO2, MSIA, MTF, CH3S(O)2OOH and CH3SOH in the gas-phase as well as measurements of the sulfate and methane- sulfonate aerosol mass fractions at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs dimethyl sulfone (DMSO2) in the gas phase and methanesulfonate (MS−) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethyl sulfoxide, and methane sulfinic acid. Also for this event, backtrajectory calculations show, that the air masses came from above the ocean (distance >330 km) with no local sur- face contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.
The SALTENA Experiment: Comprehensive Observations of Aerosol Sources, Formation, and Processes in the South American Andes
(American Meteorological Society, 2021) Federico Bianchi; Victoria A. Sinclair; Diego Aliaga; Qiaozhi Zha; Wiebke Scholz; Cheng Wu; Liine Heikkinen; Robin L. Modini; Eva Partoll; Fernando Velarde
Abstract This paper presents an introduction to the Southern Hemisphere High Altitude Experiment on Particle Nucleation and Growth (SALTENA). This field campaign took place between December 2017 and June 2018 (wet to dry season) at Chacaltaya (CHC), a GAW (Global Atmosphere Watch) station located at 5,240 m MSL in the Bolivian Andes. Concurrent measurements were conducted at two additional sites in El Alto (4,000 m MSL) and La Paz (3,600 m MSL). The overall goal of the campaign was to identify the sources, understand the formation mechanisms and transport, and characterize the properties of aerosol at these stations. State-of-the-art instruments were brought to the station complementing the ongoing permanent GAW measurements, to allow a comprehensive description of the chemical species of anthropogenic and biogenic origin impacting the station and contributing to new particle formation. In this overview we first provide an assessment of the complex meteorology, airmass origin, and boundary layer–free troposphere interactions during the campaign using a 6-month high-resolution Weather Research and Forecasting (WRF) simulation coupled with Flexible Particle dispersion model (FLEXPART). We then show some of the research highlights from the campaign, including (i) chemical transformation processes of anthropogenic pollution while the air masses are transported to the CHC station from the metropolitan area of La Paz–El Alto, (ii) volcanic emissions as an important source of atmospheric sulfur compounds in the region, (iii) the characterization of the compounds involved in new particle formation, and (iv) the identification of long-range-transported compounds from the Pacific or the Amazon basin. We conclude the article with a presentation of future research foci. The SALTENA dataset highlights the importance of comprehensive observations in strategic high-altitude locations, especially the undersampled Southern Hemisphere.