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.
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.
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.
Measurements of methane concentrations were made at the Chacaltaya GAW station (16.3ºS, 68.1ºW, 5240m a.s.l.) in the Andean Cordillera from 2015 to date. During this period two high-precision Picarro-CRDS analyzers were used at the station, regularly calibrated with internationally certified gases (WMO X2004A) via the LSCE primary scale. The site has a privileged location not only due to its altitude but also because air masses arriving from the near Altiplano (3 800 m a.s.l.), the Amazon (so-called low-lands), the Pacific Ocean, and the nearby metropolitan area of La Paz/El Alto (~2 million of inhabitants) can be sampled there. The complex topography of the region represents a challenge for deconvoluting the origin of the air masses and therefore to understanding the sources and/or processes associated with the measurements made at Chacaltaya. Here we show some results based on re-analysis data as well as on high and medium - resolution back trajectories in order to identify the influence of different regions on the station. In addition, satellite products and satellite-derived databases, from TROPOMI and GFED4.1s and WAD2M are used to characterize and interpret daily, seasonal and interannual behavior of the methane concentrations observed in Chacaltaya. The influence of the local atmospheric planetary boundary layer is clearly seen in the measurements, especially in the late morning, but collocated measurements of other atmospheric components such as carbon monoxide or equivalent black carbon have proven that identifying free-tropospheric air masses is not an easy task. The contributions of the largest human conglomerate of the region are also discussed in this context.
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.
Ten years of almost continuous observations at the highest Global Atmosphere Watch Regional station in the world are presented here. The Chacaltaya observatory (5240 m asl, 16.3ºS, 68.1ºW) was set up in December 2011. It is currently the only operational station characterizing optical and chemical properties of climate-relevant aerosol and gases in Bolivia and in a radius of about 1500 kilometers from the station. The observations show a clear influence of the well-marked dry and wet meteorological seasons. In addition, the impact on the Andean mountains of long and mid-range transport of biomass burning products from the lowlands is clearly recorded in different parameters measured at the station. Furthermore, the nearby presence of the largest metropolitan area in the region (~1.8 million inhabitants) is observed almost on a daily basis, and therefore different campaigns were carried out to characterize the area and its influence on our measurements. Specific results from these campaigns are discussed elsewhere. Finally, the topographic complexity represents an important challenge for modeling efforts in order to understand sources and sinks (and associated processes) of the observed parameters, requiring not only high spatial resolution and the correct choice of model options, but a novel way of interpreting these results. The decade of collaboration of an international consortium made it possible to keep the station running successfully. The challenge is now to preserve its functioning for the coming decades in a region with historically few high-quality observations while disrupting environmental and socio-economic changes take place.
The Amazon rainforest is a key component of the climate system and one of the main planetary evapotranspiration sources. Over the entire Amazon basin, strong land-atmosphere feedbacks cause almost one third of the regional rainfall to be transpired by the local rainforest. Maximum precipitation recycling ratio takes place on the southwestern edge of the Amazon basin (a.k.a. Amazon-Andes transition region), an area recognized as the rainiest and biologically richest of the whole watershed. Here, high precipitation rates lead to large values of runoff per unit area providing most of the sediment load to Amazon rivers. As a consequence, the transition region can potentially be very sensitive to Amazonian forest loss. In fact, recent acceleration in deforestation rates has been reported over tropical South America. These sustained land-cover changes can alter the regional water and energy balances, as well as the regional circulation and rainfall patterns. In this sense, the use of regional climate models can help to understand the possible impacts of deforestation on the Amazon-Andes zone.This work aims to assess the projected Amazonian deforestation effects on the moisture transport and rainfall behavior over tropical South America and the Amazon-Andes transition region. We perform 10-year austral summer simulations with the Weather Research and Forecasting model (WRF) using 3 one-way nested domains. Our finest domain is located over the south-western part of the basin, comprising two instrumented Andean Valleys (Zongo and Coroico river Valleys). Convective permitting high horizontal resolution (1km) is used over this domain. The outcomes presented here enhance the understanding of biosphere-atmosphere coupling and its deforestation induced disturbances.
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.
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.
Coordinado por la Universidad de Berna, Suiza. DECADE comenzo en 2014 y finalizara a principios de 2018.
An overwhelming number of applications depend on reliable precipitation estimations. However, over complex terrain in regions such as the Andes or the southwestern Amazon, the spatial coverage of rain gauges is scarce. Two reanalysis datasets, a satellite algorithm and a scheme that combines surface observations with satellite estimations were selected for studying rainfall in the following areas of Bolivia: the central Andes, Altiplano, southwestern Amazonia, and Chaco. These Bolivian regions can be divided into three main basins: the Altiplano, La Plata, and Amazon. The selected reanalyses were the Modem-Era Retrospective Analysis for Research and Applications, which has a horizontal resolution (similar to 50 km) conducive for studying rainfall in relatively small precipitation systems, and the Climate Forecast System Reanalysis and Reforecast, which features an improved horizontal resolution (similar to 38 km). The third dataset was the seventh version of the Tropical Rainfall Measurement Mission 3B42 algorithm, which is conducive for studying rainfall at an similar to 25 km horizontal resolution. The fourth dataset utilizes a new technique known as the Combined Scheme, which successfully removes satellite bias. All four of these datasets were aggregated to a coarser resolution. Additionally, the daily totals were calculated to match the cumulative daily values of the ground observations. This research aimed to describe and compare precipitations in the two reanalysis datasets, the satellite-algorithm dataset, and the Combined Scheme with ground observations. Two seasons were selected for studying the precipitation estimates: the rainy season (December-February) and the dry season (June-August). The average, bias, standard deviation, correlation coefficient, and root mean square error were calculated. Moreover, a contingency table was generated to calculate the accuracy, bias frequency, probability of detection, false alarm ratio, and equitable threat score.All four datasets correctly depicted the spatial rainfall pattern. However, CFSR and MERRA overestimated precipitation along the Andes' eastern-facing slopes and exhibited a dry bias over the eastern Amazon; TRMM3B42 and the Combined Scheme depicted a more realistic rainfall distribution over both the Amazon and the Andes. When separating the precipitation into classes, MERRA and CFSR overestimated light to moderate precipitation (1-20 mm/day) and underestimated very heavy precipitation (>50 mm/day). TRMM3B42 and CoSch depicted behaviors similar to the surface observations; however, CoSch underestimated the precipitation in very intense systems (>50 mm/day).The statistical variables indicated that CoSch's correlation coefficient was highest for every season and basin. Additionally, the bias and RMSE values suggested that CoSch closely represented the surface observations. (C) 2015 The Authors. Published by Elsevier B.V.
In July and August 2003 a field campaign was conducted to explore the diurnal circulation of the Bolivian Altiplano. Vertical soundings by remote-controlled aircraft yielded profiles of temperature, pressure, and humidity at six passes and in a valley. Pilot balloon observations provided wind profiles. Two permanent stations collected additional data. Typically, inflow toward the Altiplano commences a few hours after sunrise at about the time when the stable nocturnal layer near the ground is transformed by the solar heating into an almost neutrally stratified convective boundary layer. The depth of the inflow layer is comparable to but normally less than that of this boundary layer. There are indications of return flow aloft. The inflow continues at least until sunset. Moisture is imported at the passes leading to the Yungas in the east. Strong upvalley flows were found in the valley of the Rio de La Paz, which connects the wide canyon of La Paz with the tropical lowlands to the east. Inflow was absent at one of the passes despite favorable synoptic conditions. Cases of synoptically forced flows are presented as well where the diurnal signal is difficult to separate. A simple flow scheme is presented that fits the observations reasonably well.