Browsing by Autor "Carbone, Samara"

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Comment on acp-2021-126
(2021) Aliaga, Diego; Sinclair, Victoria A.; Andrade, Marcos; Artaxo, Paulo; Carbone, Samara; Kadantsev, Evgeny; Laj, Paolo; Wiedensohler, Alfred; Krejci, Radovan; Bianchi, Federico
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.
Comment on ar-2024-15
(2024) Aliaga, Diego; Sinclair, Victoria A.; Krejci, Radovan; Andrade, Marcos; Artaxo, Paulo; Blacutt, Luis; Cai, Runlong; Carbone, Samara; Gramlich, Yvette; Heikkinen, Liine
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.
Comment on ar-2024-15
(2024) Aliaga, Diego; Sinclair, Victoria A.; Krejci, Radovan; Andrade, Marcos; Artaxo, Paulo; Blacutt, Luis; Cai, Runlong; Carbone, Samara; Gramlich, Yvette; Heikkinen, Liine
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.
Comment on egusphere-2022-887
(2022) Scholz, Wiebke; Shen, Jiali; Aliaga, Diego; Wu, Cheng; Carbone, Samara; Moreno, Isabel; Zha, Qiaozhi; Huang, Wei; Heikkinen, Liine; Jaffrezo, Jean Luc
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.