Abstract
Frequency and intensity of warm and moist air-mass intrusions into the Arctic have increased over the past decades and have been related to sea ice melt. During our year-long expedition in ...the remote central Arctic Ocean, a record-breaking increase in temperature, moisture and downwelling-longwave radiation was observed in mid-April 2020, during an air-mass intrusion carrying air pollutants from northern Eurasia. The two-day intrusion, caused drastic changes in the aerosol size distribution, chemical composition and particle hygroscopicity. Here we show how the intrusion transformed the Arctic from a remote low-particle environment to an area comparable to a central-European urban setting. Additionally, the intrusion resulted in an explosive increase in cloud condensation nuclei, which can have direct effects on Arctic clouds’ radiation, their precipitation patterns, and their lifetime. Thus, unless prompt actions to significantly reduce emissions in the source regions are taken, such intrusion events are expected to continue to affect the Arctic climate.
Aerosol particles acting as cloud condensation nuclei (CCN) or ice-nucleating particles (INPs) play a major role in the formation and glaciation of clouds. Thereby they exert a strong impact on the ...radiation budget of the Earth. Data on abundance and properties of both types of particles are sparse, especially for remote areas of the world, such as the Southern Ocean (SO). In this work, we present unique results from ship-borne aerosol-particle-related in situ measurements and filter sampling in the SO region, carried out during the Antarctic Circumnavigation Expedition (ACE) in the austral summer of 2016–2017. An overview of CCN and INP concentrations over the Southern Ocean is provided and, using additional quantities, insights regarding possible CCN and INP sources and origins are presented.
CCN number concentrations spanned 2 orders of magnitude, e.g. for a supersaturation of 0.3 % values ranged roughly from 3 to 590 cm−3.
CCN showed variable contributions of organic and inorganic material (inter-quartile range of hygroscopicity parameter κ from 0.2 to 0.9).
No distinct size dependence of κ was apparent, indicating homogeneous composition across sizes (critical dry diameter on average between 30 and 110 nm).
The contribution of sea spray aerosol (SSA) to the CCN number concentration was on average small.
Ambient INP number concentrations were measured in the temperature range from −5 to −27 ∘C using an immersion freezing method. Concentrations spanned up to 3 orders of magnitude, e.g. at −16 ∘C from 0.2 to 100 m−3.
Elevated values (above 10 m−3 at −16 ∘C) were measured when the research vessel was in the vicinity of land (excluding Antarctica), with lower and more constant concentrations when at sea. This, along with results of backward-trajectory analyses, hints towards terrestrial and/or coastal INP sources being dominant close to ice-free (non-Antarctic) land.
In pristine marine areas INPs may originate from both oceanic sources and/or long-range transport.
Sampled aerosol particles (PM10) were analysed for sodium and methanesulfonic acid (MSA). Resulting mass concentrations were used as tracers for primary marine and secondary aerosol particles, respectively.
Sodium, with an average mass concentration around 2.8 µg m−3, was found to dominate the sampled, identified particle mass.
MSA was highly variable over the SO, with mass concentrations up to 0.5 µg m−3 near the sea ice edge.
A correlation analysis yielded strong correlations between sodium mass concentration and particle number concentration in the coarse mode, unsurprisingly indicating a significant contribution of SSA to that mode.
CCN number concentration was highly correlated with the number concentration of Aitken and accumulation mode particles. This, together with a lack of correlation between sodium mass and Aitken and accumulation mode number concentrations, underlines the important contribution of non-SSA, probably secondarily formed particles, to the CCN population. INP number concentrations did not significantly correlate with any other measured aerosol physico-chemical parameter.
Aerosol measurements over the Southern Ocean are used to constrain
aerosol–cloud interaction radiative forcing (RFaci) uncertainty in a global climate model. Forcing uncertainty is quantified using 1 ...million climate model variants that sample the uncertainty in nearly 30 model parameters. Measurements of cloud condensation nuclei and other aerosol properties from an Antarctic circumnavigation expedition strongly constrain natural aerosol emissions: default sea spray emissions need to be increased by around a factor of 3 to be consistent with measurements. Forcing uncertainty is reduced by around 7 % using this set of several hundred measurements, which is comparable to the 8 % reduction achieved using a diverse and extensive set of over 9000 predominantly Northern Hemisphere measurements. When Southern Ocean and Northern Hemisphere measurements are combined, uncertainty in RFaci is reduced by 21 %, and the strongest 20 % of forcing values are ruled out as implausible. In this combined constraint, observationally plausible RFaci is around 0.17 W m−2 weaker (less negative) with 95 % credible values ranging from −2.51 to
−1.17 W m−2 (standard deviation of −2.18 to −1.46 W m−2). The Southern Ocean and Northern Hemisphere measurement datasets are complementary because they constrain different processes. These results
highlight the value of remote marine aerosol measurements.
Ambient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in ...oceanic regions.
The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately −36 ∘C but none at warmer temperatures that could bias ship-based measurements.
Within the framework of the RACEPAC (Radiation–Aerosol–Cloud Experiment in
the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based
station in Tuktoyaktuk (Mackenzie River delta ...area, Canada), was
characterized during a period of 3 weeks in May 2014. Basic meteorological
parameters and particle number size distributions (PNSDs) were observed and
two distinct types of air masses were found. One type were typical Arctic
haze air masses, termed accumulation-type air masses, characterized by a
monomodal PNSD with a pronounced accumulation mode at sizes above
100 nm. These air masses were observed during a period when back
trajectories indicate an air mass origin in the north-east of Canada. The
other air mass type is characterized by a bimodal PNSD with a clear minimum
around 90 nm and with an Aitken mode consisting of freshly formed
aerosol particles. Back trajectories indicate that these air masses, termed
Aitken-type air masses, originated from the North Pacific. In addition, the
application of the PSCF receptor model shows that air masses with their
origin in active fire areas in central Canada and Siberia, in areas of
industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and
the north-west Pacific have
enhanced total particle number concentrations (NCN). Generally,
NCN ranged from 20 to 500 cm−3, while cloud
condensation nuclei (CCN) number concentrations were found to cover a range
from less than 10 up to 250 cm−3 for a supersaturation (SS)
between 0.1 and 0.7 %. The hygroscopicity parameter κ of the
CCN was determined to be 0.23 on average and variations in κ were
largely attributed to measurement uncertainties. Furthermore, simultaneous
PNSD measurements at the ground station and on the Polar 6 research
aircraft were performed. We found a good agreement of ground-based PNSDs
with those measured between 200 and 1200 m. During two of the four
overflights, particle number concentrations at 3000 m were found to
be up to 20 times higher than those measured below 2000 m;
for one of these two flights, PNSDs measured above 2000 m showed a
different shape than those measured at lower altitudes. This is indicative of
long-range transport from lower latitudes into the Arctic that can advect
aerosol from different regions in different heights.
Abstract
The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and ...temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity,
κ
, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (
ϵ
org
) and inorganic ions (
ϵ
inorg
) through a linear combination,
κ
=
ϵ
org
⋅
κ
org
+
ϵ
inorg
⋅
κ
inorg
. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of
κ
org
= 0.12 ± 0.02 with
κ
inorg
= 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in
κ
org
and
κ
inorg
is small, we constrain a critically important aspect of global climate modelling.
Abstract As a precursor process to cloud formation, aerosol activation over the Tibetan Plateau (TP) plays a pivotal role in regional cloud-precipitation and global climate. However, its ...characteristics remain unclear due to the absence of targeted observations in the TP. We conducted a ground in-situ aerosol-cloud-precipitation experiment in the southern TP (GACPE-STP), thereby unveiling the aerosol activation characteristics in this crucial region. Our findings reveal a weak aerosol activation capacity with low hygroscopicity ( κ ) values of less than 0.1 through multi-method κ measurements, contrasting starkly with the widely recommended κ value of 0.3 for continental regions. A κ parameterization is developed for predicting aerosol activation in this region, which can significantly reduce the overestimations of cloud droplet number concentration and hence aerosol indirect effects caused by using the recommended κ of 0.3. These findings address the unclear characteristics of aerosol activation in the TP region, contributing to the enhancement of regional cloud precipitation and global climate simulations.
In this study, we investigate the occurrence of primary biological aerosol particles (PBAP) over all sectors of the Southern Ocean (SO) based on a 90‐day data set collected during the Antarctic ...Circumnavigation Expedition (ACE) in austral summer 2016–2017. Super‐micrometer PBAP (1–16 µm diameter) were measured by a wide band integrated bioaerosol sensor (WIBS‐4). Low (3σ) and high (9σ) fluorescence thresholds are used to obtain statistics on fluorescent and hyper‐fluorescent PBAP, respectively. Our focus is on data obtained over the pristine ocean, that is, more than 200 km away from land. The results indicate that (hyper‐)fluorescent PBAP are correlated to atmospheric variables associated with sea spray aerosol (SSA) particles (wind speed, total super‐micrometer aerosol number concentration, chloride and sodium concentrations). This suggests that a main source of PBAP over the SO is SSA. The median percentage contribution of fluorescent and hyper‐fluorescent PBAP to super‐micrometer SSA was 1.6% and 0.13%, respectively. We demonstrate that the fraction of (hyper‐)fluorescent PBAP to total super‐micrometer particles positively correlates with concentrations of bacteria and several taxa of pythoplankton measured in seawater, indicating that marine biota concentrations modulate the PBAP source flux. We investigate the fluorescent properties of (hyper‐)fluorescent PBAP for several events that occurred near land masses. We find that the fluorescence signal characteristics of particles near land is much more variable than over the pristine ocean. We conclude that the source and concentration of fluorescent PBAP over the open ocean is similar across all sampled sectors of the SO.
Key Points
Fluorescent primary bioaerosol particles (PBAP) were measured over all sectors of the Southern Ocean
Moderate to good correlations were observed between PBAP and sea spray aerosol (SSA) proxies
PBAP fractions in SSA were positively correlated to concentrations of certain marine biota
Abstract
The Arctic environment is transforming rapidly due to climate change. Aerosols’ abundance and physicochemical characteristics play a crucial, yet uncertain, role in these changes due to ...their influence on the surface energy budget through direct interaction with solar radiation and indirectly via cloud formation. Importantly, Arctic aerosol properties are also changing in response to climate change. Despite their importance, year-round measurements of their characteristics are sparse in the Arctic and often confined to lower latitudes at Arctic land-based stations and/or short high-latitude summertime campaigns. Here, we present unique aerosol microphysics and chemical composition datasets collected during the year-long Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, in the central Arctic. These datasets, which include aerosol particle number concentrations, size distributions, cloud condensation nuclei concentrations, fluorescent aerosol concentrations and properties, and aerosol bulk chemical composition (black carbon, sulfate, nitrate, ammonium, chloride, and organics) will serve to improve our understanding of high-Arctic aerosol processes, with relevance towards improved modelling of the future Arctic (and global) climate.
Understanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and ...narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1 % to 0.7 %, the median NCCN increases from 399 to 2144 cm−3, which represents 10 % to 48 % of the total particle number concentration with a diameter range of 10–800 nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54 nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SS=0.1 %, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of ∼40 to 100 nm and almost stays constant at Dp of 100 to 200 nm, whereas the degree of the external mixture keeps decreasing at Dp of ∼40 to 200 nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ–Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ–Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ–Dp relationships for different regions and their seasonal variations.
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