scholarly journals Identifying source regions of air masses sampled at the tropical high-altitude site of Chacaltaya using WRF-FLEXPART and cluster analysis

2021 ◽  
Author(s):  
Diego Aliaga ◽  
Victoria A. Sinclair ◽  
Marcos Andrade ◽  
Paulo Artaxo ◽  
Samara Carbone ◽  
...  

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.

2021 ◽  
Vol 21 (21) ◽  
pp. 16453-16477
Author(s):  
Diego Aliaga ◽  
Victoria A. Sinclair ◽  
Marcos Andrade ◽  
Paulo Artaxo ◽  
Samara Carbone ◽  
...  

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.


2020 ◽  
Author(s):  
Diego Aliaga ◽  
Victoria Sinclair ◽  
Zha Qiaozhi ◽  
Marcos Andrade ◽  
Claudia Mohr ◽  
...  

<p>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 ‘K-means’ 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 (<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 (>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.</p>


2019 ◽  
Vol 19 (19) ◽  
pp. 12477-12494 ◽  
Author(s):  
Armin Sigmund ◽  
Korbinian Freier ◽  
Till Rehm ◽  
Ludwig Ries ◽  
Christian Schunk ◽  
...  

Abstract. To assist atmospheric monitoring at high-alpine sites, a statistical approach for distinguishing between the dominant air masses was developed. This approach was based on a principal component analysis using five gas-phase and two meteorological variables. The analysis focused on the Schneefernerhaus site at Zugspitze Mountain, Germany. The investigated year was divided into 2-month periods, for which the analysis was repeated. Using the 33.3 % and 66.6 % percentiles of the first two principal components, nine air mass regimes were defined. These regimes were interpreted with respect to vertical transport and assigned to the BL (recent contact with the boundary layer), UFT/SIN (undisturbed free troposphere or stratospheric intrusion), and HYBRID (influences of both the boundary layer and the free troposphere or ambiguous) air mass classes. The input data were available for 78 % of the investigated year. BL accounted for 31 % of the cases with similar frequencies in all seasons. UFT/SIN comprised 14 % of the cases but was not found from April to July. HYBRID (55 %) mostly exhibited intermediate characteristics, whereby 17 % of the HYBRID class suggested an influence from the marine boundary layer or the lower free troposphere. The statistical approach was compared to a mechanistic approach using the ceilometer-based mixing layer height from a nearby valley site and a detection scheme for thermally induced mountain winds. Due to data gaps, only 25 % of the cases could be classified using the mechanistic approach. Both approaches agreed well, except in the rare cases of thermally induced uplift. The statistical approach is a promising step towards a real-time classification of air masses. Future work is necessary to assess the uncertainty arising from the standardization of real-time data.


2004 ◽  
Vol 4 (2) ◽  
pp. 497-509 ◽  
Author(s):  
S. Henne ◽  
M. Furger ◽  
S. Nyeki ◽  
M. Steinbacher ◽  
B. Neininger ◽  
...  

Abstract. Net vertical air mass export by thermally driven flows from the atmospheric boundary layer (ABL) to the free troposphere (FT) above deep Alpine valleys was investigated. The vertical export of pollutants above mountainous terrain is presently poorly represented in global chemistry transport models (GCTMs) and needs to be quantified. Air mass budgets were calculated using aircraft observations obtained in deep Alpine valleys. The results show that on average 3 times the valley air mass is exported vertically per day under fair weather conditions. During daytime the type of valleys investigated in this study can act as an efficient "air pump" that transports pollutants upward. The slope wind system within the valley plays an important role in redistributing pollutants. Nitrogen oxide emissions in mountainous regions are efficiently injected into the FT. This could enhance their ozone (O3) production efficiency and thus influences tropospheric pollution budgets. Once lifted to the FT above the Alps pollutants are transported horizontally by the synoptic flow and are subject to European pollution export. Forward trajectory studies show that under fair weather conditions two major pathways for air masses above the Alps dominate. Air masses moving north are mixed throughout the whole tropospheric column and further transported eastward towards Asia. Air masses moving south descend within the subtropical high pressure system above the Mediterranean.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
S. Allen ◽  
D. Allen ◽  
F. Baladima ◽  
V. R. Phoenix ◽  
J. L. Thomas ◽  
...  

AbstractThe emerging threat of atmospheric microplastic pollution has prompted researchers to study areas previously considered beyond the reach of plastic. Investigating the range of atmospheric microplastic transport is key to understanding the global extent of this problem. While atmospheric microplastics have been discovered in the planetary boundary layer, their occurrence in the free troposphere is relatively unexplored. Confronting this is important because their presence in the free troposphere would facilitate transport over greater distances and thus the potential to reach more distal and remote parts of the planet. Here we show evidence of 0.09–0.66 microplastics particles/m3 over 4 summer months from the Pic du Midi Observatory at 2877 meters above sea level. These results exhibit true free tropospheric transport of microplastic, and high altitude microplastic particles <50 µm (aerodynamic diameter). Analysis of air/particle history modelling shows intercontinental and trans-oceanic transport of microplastics illustrating the potential for global aerosol microplastic transport.


2013 ◽  
Vol 13 (19) ◽  
pp. 9837-9853 ◽  
Author(s):  
T. Hamburger ◽  
M. Matisāns ◽  
P. Tunved ◽  
J. Ström ◽  
S. Calderon ◽  
...  

Abstract. First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm−3, refractory particle number concentrations (at 300 °C) 510±420 cm−3 and the absorption coefficient 0.91±1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm−3, 150±94 cm−3 and 0.15±0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño–Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.


2013 ◽  
Vol 13 (5) ◽  
pp. 13079-13117
Author(s):  
T. Hamburger ◽  
M. Matisāns ◽  
P. Tunved ◽  
J. Ström ◽  
S. Calderon ◽  
...  

Abstract. First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron aerosol volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night time and observations of boundary layer air masses during day time and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron aerosol volume reached 1.4 ± 1.3 μm3 cm−3, heated (300 °C) particle number concentrations 510 ± 420 cm−3 and the absorption coefficient 0.91 ± 1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19 ± 0.25 μm3 cm−3, 150 ± 94 cm−3 and 0.15 ± 0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño-Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.


2003 ◽  
Vol 3 (5) ◽  
pp. 5205-5236 ◽  
Author(s):  
S. Henne ◽  
M. Furger ◽  
S. Nyeki ◽  
M. Steinbacher ◽  
B. Neininger ◽  
...  

Abstract. Net vertical air mass export by thermally driven f\\/lows from the atmospheric boundary layer (ABL) to the free troposphere (FT) above deep Alpine valleys was investigated. The vertical export of pollutants above mountainous terrain is presently poorly represented in global chemistry transport models (GCTMs) and needs to be quantified. Air mass budgets were calculated using aircraft observations obtained in deep Alpine valleys. The results show that on average 3 times the valley air mass is exported vertically per day under fair weather conditions. During daytime the type of valleys investigated in this study can act as an efficient "air pump" that transports pollutants upward. The slope wind system within the valley plays an important role in redistributing pollutants. Nitrogen oxide emissions in mountainous regions are efficiently injected into the FT. This enhances their ozone production efficiency and thus influences tropospheric pollution budgets. Once lifted to the FT above the Alps pollutants are transported horizontally by the synoptic flow and are subject to European pollution export. Forward trajectory studies show that under fair weather conditions two major pathways for air masses above the Alps dominate. Air masses moving north are mixed throughout the whole tropospheric column and further transported eastward towards Asia. Air masses moving south descend within the subtropical high pressure system above the Mediterranean.


2017 ◽  
Author(s):  
Bin Chen ◽  
Bärbel Vogel ◽  
Xiangde Xu ◽  
Shuai Yang

Abstract. The Asian summer monsoon (ASM) is associated with an upper-level anticyclone and acts as a well-recognized conduit for troposphere-to-stratosphere transport. The Lagrangian dispersion and transport model FLEXPART forced by ERA-Interim data from 2001–2013 was used to perform climatological modeling of the summer season (May–July). This study examines the properties of the air mass transport from the atmospheric boundary layer (BL) to the tropopause layer (TL), with particular focus on the sub-seasonal variability in the tracer-independent BL sources and the potential controlling mechanisms. The results show that, climatologically, the three most impactful BL source regions are northern India, the Tibetan Plateau, and the southern slope of the Himalayas. These regions are consistent with the locations of sources identified in previous studies. However, upon closer inspection, the different source regions to the BL-to-TL air mass transport are not constant in location or shape and are strongly affected by sub-seasonal variability. The contributions from the Tibetan Plateau are most significant in early May but decrease slightly in mid-May to mid-June. In contrast, the contributions from India and the southern slope of the Himalayas increase dramatically, with peak values occurring in mid-July. Empirical Orthogonal Function (EOF) analysis provides further evidence that the BL sources in the ASM region vary across a wide range of spatiotemporal scales. The sub-seasonal behavior of these BL sources is closely related to the strength of persistent deep convection activity over the northern Bay of Bengal and its neighboring areas.


2008 ◽  
Vol 8 (22) ◽  
pp. 6729-6738 ◽  
Author(s):  
N. Kalivitis ◽  
W. Birmili ◽  
M. Stock ◽  
B. Wehner ◽  
A. Massling ◽  
...  

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October, 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.


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