Browsing by Autor "Victoria A. Sinclair"

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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 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;
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.