1. Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory : a case study with a long-range transported biomass burning plumeKatja Džepina, Claudio Mazzoleni, Paulo Fialho, Swarup China, Bo Zhang, R. Chris Owen, D. Helmig, J. Hueber, Sumit Kumar, J. A. Perlinger, 2015, izvirni znanstveni članek Opis: Free tropospheric aerosol was sampled at the
Pico Mountain Observatory located at 2225 m above mean
sea level on Pico Island of the Azores archipelago in the
North Atlantic. The observatory is located ∼ 3900 km east
and downwind of North America, which enables studies
of free tropospheric air transported over long distances.
Aerosol samples collected on filters from June to October
2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 µg m−3
. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51 %), followed by
sulfate (23 ± 28 %), nitrate (13 ± 10 %), chloride (2 ± 3 %),
and elemental carbon (2 ± 2 %). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and
9/25) collected consecutively during a pollution event were
analyzed using ultrahigh-resolution electrospray ionization
Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned
to each of the mass spectra in the range of m/z 100–1000.
The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled
air masses were very aged (average plume age > 12 days).
These aged aerosol WSOM compounds had an average O /C
ratio of ∼ 0.45, which is relatively low compared to O /C
ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to
biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM
and with the morphology and mixing state of particles as
determined by scanning electron microscopy. The presence
of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were
more aged and influenced by marine emissions, as indicated
by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for
the two samples was corroborated by the changes in ethane,
propane, and ozone, morphology of particles, as well as by
the FLEXPART retroplume simulations. This paper presents
the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere
remote location and provides evidence of low oxygenation
after long-range transport. We hypothesize this is a result of
the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a
combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and
fragmentation (e.g., photolysis) of components. Ključne besede: organic aerosol, ultrahigh-resolution FT-ICR MS, electron microscopy, remote marine atmosphere, Pico Mountain Observatory Objavljeno v RUNG: 11.04.2021; Ogledov: 3241; Prenosov: 0 Gradivo ima več datotek! Več... |
2. Molecular and physical characteristics of aerosol at a remote free troposphere site : implications for atmospheric agingSimeon K. Schum, Bo Zhang, Katja Džepina, Paulo Fialho, Claudio Mazzoleni, Lynn R. Mazzoleni, 2018, izvirni znanstveni članek Opis: Aerosol properties are transformed by atmospheric processes during long-range transport and play a key role in the Earth’s radiative balance. To understand the molecular and physical characteristics of free tropospheric aerosol, we studied samples collected at the Pico Mountain Observatory in the North Atlantic. The observatory is located in the marine free troposphere at 2225m above sea level, on Pico Island in the Azores archipelago. The site is ideal for the study of long-range-transported free tropospheric aerosol with minimal local influence. Three aerosol samples with elevated organic carbon concentrations were selected for detailed analysis. FLEXPART retroplumes indicated that two
of the samples were influenced by North American wildfire
emissions transported in the free troposphere and one by
North American outflow mainly transported within the marine
boundary layer. Ultrahigh-resolution Fourier transform
ion cyclotron resonance mass spectrometry was used to determine
the detailed molecular composition of the samples.
Thousands of molecular formulas were assigned to each of
the individual samples. On average ~60% of the molecular
formulas contained only carbon, hydrogen, and oxygen
atoms (CHO), ~ 30% contained nitrogen (CHNO), and
~ 10% contained sulfur (CHOS). The molecular formula
compositions of the two wildfire-influenced aerosol samples
transported mainly in the free troposphere had relatively low
average O=C ratios (0:48 ± 0:13 and 0:45 ± 0:11) despite the
7–10 days of transport time according to FLEXPART. In contrast,
the molecular composition of the North American outflow
transported mainly in the boundary layer had a higher
average O=C ratio (0:57 ± 0:17) with 3 days of transport time.
To better understand the difference between free tropospheric
transport and boundary layer transport, the meteorological
conditions along the FLEXPART simulated transport pathways
were extracted from the Global Forecast System analysis
for the model grids. We used the extracted meteorological
conditions and the observed molecular chemistry to predict
the relative-humidity-dependent glass transition temperatures
(Tg) of the aerosol components. Comparisons of the
Tg to the ambient temperature indicated that a majority of
the organic aerosol components transported in the free troposphere were more viscous and therefore less susceptible to
oxidation than the organic aerosol components transported
in the boundary layer. Although the number of observations
is limited, the results suggest that biomass burning organic
aerosol injected into the free troposphere is more persistent
than organic aerosol in the boundary layer having broader
implications for aerosol aging. Ključne besede: secondary organic aerosols, brown carbon, particle dispersion model, ultrahigh-resolution FT-ICR MS, Pico Mountain Observatory Objavljeno v RUNG: 10.04.2021; Ogledov: 3254; Prenosov: 0 Gradivo ima več datotek! Več... |
3. All-sky search for correlations in the arrival directions of astrophysical neutrino candidates and ultrahigh-energy cosmic raysI. Al Samarai, Andrej Filipčič, Gašper Kukec Mezek, Ahmed Saleh, Samo Stanič, Marta Trini, Darko Veberič, Serguei Vorobiov, Lili Yang, Danilo Zavrtanik, Marko Zavrtanik, 2017, objavljeni znanstveni prispevek na konferenci Ključne besede: correlations, astrophysical neutrino, ultrahigh-energy cosmic rays Objavljeno v RUNG: 19.02.2018; Ogledov: 4220; Prenosov: 170 Celotno besedilo (3,07 MB) |
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