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Integrated water vapor during rain and rain-free conditions above the Swiss Plateau
Water vapor column density, or vertically-integrated water vapor (IWV), is monitored by ground-based microwave radiometers (MWR) and ground-based receivers of the Global Navigation Satellite System (GNSS). For rain periods, the retrieval of IWV from GNSS Zenith Wet Delay (ZWD) neglects the atmospheric propagation delay of the GNSS signal by rain droplets. Similarly, it is difficult for ground-based dual-frequency single-polarisation microwave radiometers to separate the microwave emission of water vapor and cloud droplets from the rather strong microwave emission of rain. For ground-based microwave radiometry at Bern (Switzerland), we take the approach that IWV during rain is derived from linearly interpolated opacities before and after the rain period. The intermittent rain periods often appear as spikes in the time series of integrated liquid water (ILW) and are indicated by ILW ≥ 0.4 mm. In the present study, we assume that IWV measurements from radiosondes are not affected by rain. We intercompare the climatologies of IWV(rain), IWV(no rain), and IWV(all) obtained by radiosonde, ground-based GNSS atmosphere sounding, ground-based MWR, and ECMWF reanalysis (ERA5) at Payerne and Bern in Switzerland. In all seasons, IWV(rain) is 3.75 to 5.94 mm greater than IWV(no rain). The mean IWV differences between GNSS and radiosonde at Payerne are less than 0.26 mm. The datasets at Payerne show a better agreement than the datasets at Bern. However, the MWR at Bern agrees with the radiosonde at Payerne within 0.41 mm for IWV(rain) and 0.02 mm for IWV(no rain). Using the GNSS and rain gauge measurements at Payerne, we find that IWV(rain) increases with increase of the precipitation rate during summer as well as during winter. IWV(rain) above the Swiss Plateau is quite well estimated by GNSS and MWR though the standard retrievals are limited or hampered during rain periods.
2021
A portion of Colombia’s water resources is located on the Pacific coast within the territory of the Community Council of Alto and Medio Dagua (CC-AMDA). Though a harmonious balance between the communities’ subsistent activities and nature was maintained for centuries, the appearance of modern modes of resource extraction has negatively affected the environment, especially the water resources. The Driver-Pressure-State- Impact-Response (DPSIR) framework was used to analyze water quality problems within this community council. The DPSIR analysis revealed that agriculture, mining, logging and infrastructure development constitute important sectoral drivers with some contribution from tourism and fisheries. Pressures included inputs of organic matter, sediment, nutrients and chemical contaminants to the Dagua river, and to the Bay of Buenaventura. These produced corresponding State changes in the water bodies. Impacts on human welfare were poor public health, reduced food and water security, economic loss and some displacement. Societal Responses included public protests and campaigns, legal actions and policy changes for improved governance. As a future policy option, the formation of community-based water resources management is recommended. Though DPSIR was able to link cause-effect relations, further empirical research on these water bodies is necessary to fill in existing gaps in the data set, particularly for public health threatening contaminants.
2018
Fate of Springtime Atmospheric Reactive Mercury: Concentrations and Deposition at Zeppelin, Svalbard
Mid-latitude atmospheric elemental mercury (Hg) emissions undergo extensive oxidation to reactive Hg (RM) compounds during Arctic polar sunrise, resulting in enhanced atmospheric deposition that impacts Arctic marine wildlife and humans. It has been difficult to estimate RM dry deposition, because RM concentrations, compounds, and their deposition velocities are ill-defined. Here, we investigate RM concentrations sampled with membrane-based methods and find these to exceed denuder-based RM detection by 5 times at the Zeppelin Observatory on Svalbard (March 26–July 24, 2019). Measured dry deposition of gaseous oxidized Hg was about half of the modeled RM deposition, demonstrating that particulate-bound Hg was an important component of dry deposition. Using thermal membrane desorption, RM chemistry was found to be dominated by Hg–Cl/Br (51%) and Hg–N (45%) compounds. Back-trajectory analysis indicated that Hg–Br/Cl compounds were predominantly advected from within the marine boundary layer (sea ice exposure), while Hg–N originated from the free troposphere. Weekly average RM compound-specific dry deposition velocities ranged from 0.12 to 0.49 cm s–1, with a net RM dry deposition of 1.9 μg m–2 (1.5–2.5 μg m–2; 95% confidence interval) that exceeds the mean annual Hg wet deposition flux in Svalbard. Overall, we find that springtime atmospheric RM deposition has been underestimated in the Arctic marine environment.
2021
Black Carbon Emission Reduction Due to COVID-19 Lockdown in China
During the Lunar New Year Holiday of 2020, China implemented an unprecedented lockdown to fight the COVID-19 outbreak, which strongly affected the anthropogenic emissions. We utilized elemental carbon observations (equivalent to black carbon, BC) from 42 sites and performed inverse modeling to determine the impact of the lockdown on the weekly BC emissions and quantify the effect of the stagnant conditions on BC observations in densely populated eastern and northern China. BC emissions declined 70% (eastern China) and 48% (northern China) compared to the first half of January. In northern China, under the stagnant conditions of the first week of the lockdown, the observed BC concentrations rose unexpectedly (29%) even though the BC emissions fell. The emissions declined substantially thereafter until a week after the lockdown ended. On the contrary, in eastern China, BC emissions dropped sharply in the first week and recovered synchronously with the end of the lockdown.
2021
Accurate modeling of ash clouds from volcanic eruptions requires knowledge about the eruption source parameters including eruption onset, duration, mass eruption rates, particle size distribution, and vertical-emission profiles. However, most of these parameters are unknown and must be estimated somehow. Some are estimated based on observed correlations and known volcano parameters. However, a more accurate estimate is often needed to bring the model into closer agreement with observations.
This paper describes the inversion procedure implemented at the Norwegian Meteorological Institute for estimating ash emission rates from retrieved satellite ash column amounts and a priori knowledge. The overall procedure consists of five stages: (1) generate a priori emission estimates, (2) run forward simulations with a set of unit emission profiles, (3) collocate/match observations with emission simulations, (4) build system of linear equations, and (5) solve overdetermined systems. We go through the mathematical foundations for the inversion procedure, performance for synthetic cases, and performance for real-world cases. The novelties of this paper include a memory efficient formulation of the inversion problem, a detailed description and illustrations of the mathematical formulations, evaluation of the inversion method using synthetic known-truth data as well as real data, and inclusion of observations of ash cloud-top height. The source code used in this work is freely available under an open-source license and is able to be used for other similar applications.
2024
Machine learning-based stocks and flows modeling of road infrastructure
This paper introduces a new method to account for the stocks and flows of road infrastructure at the national level based on material flow accounting (MFA). The proposed method closes some of the current shortcomings in road infrastructures that were identified through MFA: (1) the insufficient implementation of prospective analysis, (2) heavy use of archetypes as a way to represent road infrastructure, (3) inadequate attention to the inclusion of dissipative flows, and (4) limited coverage of the uncertainties. The proposed dynamic bottom-up MFA method was tested on the Norwegian road network to estimate and predict the material stocks and flows between 1980 and 2050. Here, a supervised machine learning model was introduced to estimate the road infrastructure instead of archetypical mapping of different roads. The dissipation of materials from the road infrastructure based on tire–pavement interaction was incorporated. Moreover, this study utilizes iterative classified and regression trees, lifetime distributions, randomized material intensities, and sensitivity analyses to quantify the uncertainties.
2022
Black Carbon (BC) aerosol is a major climate forcer in the Arctic. Here, we present 15 years (2001–2015) of surface observations of the aerosol absorption coefficient babs (corresponding to Equivalent BC), obtained at the Zeppelin Observatory, Ny Ålesund, Svalbard, coupled with backward transport modeling with Flexpart in order to calculate the Potential Source Contribution Function (PSCF) for BC. The observed long-term variability superimposed on a strong annual cycle is studied as a function of large-scale circulation patterns represented by monthly index values for the North Atlantic Oscillation (NAO) and the Scandinavian pattern (SCAN). We find a 35% increase of babs values at Zeppelin during the SCAN+ phase in the winter half-year compared to the SCAN+ phase but no significant difference in babs values between the NAO index phases. Both NAO and SCAN induce significant regional variability on the areas of origin of babs, mainly Siberia, Europe, and North America.
2021
The Tibetan Plateau (TP), referred to as the “Asian water tower,” contains one of the largest land ice masses on Earth. The local glacier shrinkage and frozen-water storage are strongly affected by variations in surface air temperature over the TP (TPSAT), especially in springtime. This study reveals that the relationship between the February North Atlantic Oscillation (NAO) and March TPSAT is unstable with time and regulated by the phase of the Atlantic multidecadal variability (AMV). The significant out-of-phase connection occurs only during the warm phase of AMV (AMV+). The results show that during the AMV+, the negative phase of the NAO persists from February to March, and is accompanied by a quasi-stationary Rossby wave train trapped along a northward-shifted subtropical westerly jet stream across Eurasia, inducing an anomalous adiabatic descent that warms the TP. However, during the cold phase of the AMV, the negative NAO cannot persist into March. The Rossby wave train propagates along the well-separated polar and subtropical westerly jets, and the NAO–TPSAT connection is broken. Further investigation suggests that the enhanced synoptic eddy and low-frequency flow (SELF) interaction over the North Atlantic in February and March during the AMV+, caused by the southward-shifted storm track, helps maintain the NAO pattern via positive eddy feedback. This study provides a new detailed perspective on the decadal variability of the North Atlantic–TP connection in late winter to early spring.
2021
Rapid identification of in vitro cell toxicity using an electrochemical membrane screening platform
This study compares the performance and output of an electrochemical phospholipid membrane platform against respective in vitro cell-based toxicity testing methods using three toxicants of different biological action (chlorpromazine (CPZ), colchicine (COL) and methyl methanesulphonate (MMS)). Human cell lines from seven different tissues (lung, liver, kidney, placenta, intestine, immune system) were used to validate this physicochemical testing system. For the cell-based systems, the effective concentration at 50 % cell death (EC50) values are calculated. For the membrane sensor, a limit of detection (LoD) value was extracted as a quantitative parameter describing the minimum concentration of toxicant which significantly affects the structure of the phospholipid sensor membrane layer. LoD values were found to align well with the EC50 values when acute cell viability was used as an end-point and showed a similar toxicity ranking of the tested toxicants. Using the colony forming efficiency (CFE) or DNA damage as end-point, a different order of toxicity ranking was observed. The results of this study showed that the electrochemical membrane sensor generates a parameter relating to biomembrane damage, which is the predominant factor in decreasing cell viability when in vitro models are acutely exposed to toxicants. These results lead the way to using electrochemical membrane-based sensors for rapid relevant preliminary toxicity screens.
2023
The white-tailed eagle (Haliaeetus albicilla) in Scandinavia has suffered from impaired reproduction due to high exposure to industrial pollution between the 1960s and 1980s. While population numbers are rising again, new contaminants, such as per- and polyfluoroalkyl substances (PFAS), are increasingly found in high trophic avifauna and are of concern to potentially impact once again on population health. In the present study, we examined PFAS levels in plasma of white-tailed eagle nestlings from northern Norway over the last decade (2008–2017). While PFOA and PFNA exposure did not follow a significant time trend, PFOS and PFHxS concentrations decreased over time, and ≥C11 perfluorinated carboxylic acids only seem to level off during the last four years. This may in fact be the first evidence for a change in the trend for some of these compounds. Furthermore, since several PFAS are expected to be highly present in aqueous film-forming foams used at airports, we also investigate the potential of the two main airports in the region to act as hotspots for PFAS. Our results indeed show decreasing exposure to PFOA with distance to the airports. Altogether, our results seem to show that legislation actions are effective, and continued concern for PFAS exposure of high trophic wildlife is still warranted, even in the northern environment.
2020
Knowledge architecture for the wise governance of sustainability transitions
The need for sustainability transitions is widely recognised, along with a concurrent need for the evolution of knowledge systems to inform more effective policy action. Although there are many new policy targets relating to net zero emissions and other sustainability challenges, cities, regional and national governments are struggling to rapidly develop transformational policies to achieve them. As academics and practitioners who work at the science-policy interface, we identify specific knowledge and competency needs for governing sustainability transitions related to the interlinked phases of envisioning, implementing and evaluating. In short, coordinated reforms of both policy and knowledge systems are urgently needed to address the speed and scale of sustainability challenges. These include embedding systems thinking literacy, mainstreaming participatory policy making, expanding the capacity to undertake transdisciplinary research, more adaptive governance and continuous organisational learning. These processes must guide further knowledge development, uptake and use as part of an iterative and holistic process. Such deep-seated change in policy-knowledge systems will be disruptive and presents challenges for traditional organisational models of knowledge delivery, but is essential for successful sustainability transformations.
2021
Modeling the Time-Variant Dietary Exposure of PCBs in China over the Period 1930 to 2100
This study aimed for the first time to reconstruct historical exposure profiles for PCBs to the Chinese population, by examining the combined effect of changing temporal emissions and dietary transition. A long-term (1930–2100) dynamic simulation of human exposure using realistic emission scenarios, including primary emissions, unintentional emissions, and emissions from e-waste, combined with dietary transition trends was conducted by a multimedia fate model (BETR-Global) linked to a bioaccumulation model (ACC-HUMAN). The model predicted an approximate 30-year delay of peak body burden for PCB-153 in a 30-year-old Chinese female, compared to their European counterpart. This was mainly attributed to a combination of change in diet and divergent emission patterns in China. A fish-based diet was predicted to result in up to 8 times higher body burden than a vegetable-based diet (2010–2100). During the production period, a worst-case scenario assuming only consumption of imported food from a region with more extensive production and usage of PCBs would result in up to 4 times higher body burden compared to consumption of only locally produced food. However, such differences gradually diminished after cessation of production. Therefore, emission reductions in China alone may not be sufficient to protect human health from PCB-like chemicals, particularly during the period of mass production. The results from this study illustrate that human exposure is also likely to be dictated by inflows of PCBs via the environment, waste, and food.
2018
Observation of turbulent dispersion of artificially released SO2 puffs with UV cameras
In atmospheric tracer experiments, a substance is released into the turbulent atmospheric flow to study the dispersion parameters of the atmosphere. That can be done by observing the substance's concentration distribution downwind of the source. Past experiments have suffered from the fact that observations were only made at a few discrete locations and/or at low time resolution. The Comtessa project (Camera Observation and Modelling of 4-D Tracer Dispersion in the Atmosphere) is the first attempt at using ultraviolet (UV) camera observations to sample the three-dimensional (3-D) concentration distribution in the atmospheric boundary layer at high spatial and temporal resolution. For this, during a three-week campaign in Norway in July 2017, sulfur dioxide (SO2), a nearly passive tracer, was artificially released in continuous plumes and nearly instantaneous puffs from a 9m high tower. Column-integrated SO2 concentrations were observed with six UV SO2 cameras with sampling rates of several hertz and a spatial resolution of a few centimetres. The atmospheric flow was characterised by eddy covariance measurements of heat and momentum fluxes at the release mast and two additional towers. By measuring simultaneously with six UV cameras positioned in a half circle around the release point, we could collect a data set of spatially and temporally resolved tracer column densities from six different directions, allowing a tomographic reconstruction of the 3-D concentration field. However, due to unfavourable cloudy conditions on all measurement days and their restrictive effect on the SO2 camera technique, the presented data set is limited to case studies. In this paper, we present a feasibility study demonstrating that the turbulent dispersion parameters can be retrieved from images of artificially released puffs, although the presented data set does not allow for an in-depth analysis of the obtained parameters. The 3-D trajectories of the centre of mass of the puffs were reconstructed enabling both a direct determination of the centre of mass meandering and a scaling of the image pixel dimension to the position of the puff. The latter made it possible to retrieve the temporal evolution of the puff spread projected to the image plane. The puff spread is a direct measure of the relative dispersion process. Combining meandering and relative dispersion, the absolute dispersion could be retrieved. The turbulent dispersion in the vertical is then used to estimate the effective source size, source timescale and the Lagrangian integral time. In principle, the Richardson–Obukhov constant of relative dispersion in the inertial subrange could be also obtained, but the observation time was not sufficiently long in comparison to the source timescale to allow an observation of this dispersion range. While the feasibility of the methodology to measure turbulent dispersion could be demonstrated, a larger data set with a larger number of cloud-free puff releases and longer observation times of each puff will be recorded in future studies to give a solid estimate for the turbulent dispersion under a variety of stability conditions.
2018
The Arctic is warming two to three times faster than the global average, and the role of aerosols is not well constrained. Aerosol number concentrations can be very low in remote environments, rendering local cloud radiative properties highly sensitive to available aerosol. The composition and sources of the climate-relevant aerosols, affecting Arctic cloud formation and altering their microphysics, remain largely elusive due to a lack of harmonized concurrent multi-component, multi-site, and multi-season observations. Here, we present a dataset on the overall chemical composition and seasonal variability of the Arctic total particulate matter (with a size cut at 10 μm, PM10, or without any size cut) at eight observatories representing all Arctic sectors. Our holistic observational approach includes the Russian Arctic, a significant emission source area with less dedicated aerosol monitoring, and extends beyond the more traditionally studied summer period and black carbon/sulfate or fine-mode pollutants. The major airborne Arctic PM components in terms of dry mass are sea salt, secondary (non-sea-salt, nss) sulfate, and organic aerosol (OA), with minor contributions from elemental carbon (EC) and ammonium. We observe substantial spatiotemporal variability in component ratios, such as EC/OA, ammonium/nss-sulfate and OA/nss-sulfate, and fractional contributions to PM. When combined with component-specific back-trajectory analysis to identify marine or terrestrial origins, as well as the companion study by Moschos et al 2022 Nat. Geosci. focusing on OA, the composition analysis provides policy-guiding observational insights into sector-based differences in natural and anthropogenic Arctic aerosol sources. In this regard, we first reveal major source regions of inner-Arctic sea salt, biogenic sulfate, and natural organics, and highlight an underappreciated wintertime source of primary carbonaceous aerosols (EC and OA) in West Siberia, potentially associated with the oil and gas sector. The presented dataset can assist in reducing uncertainties in modelling pan-Arctic aerosol-climate interactions, as the major contributors to yearly aerosol mass can be constrained. These models can then be used to predict the future evolution of individual inner-Arctic atmospheric PM components in light of current and emerging pollution mitigation measures and improved region-specific emission inventories.
2022
2024
Fine particulate matter (PM2.5) is a key air quality indicator due to its adverse health impacts. Accurate PM2.5 assessment requires high-resolution (e.g., atleast 1 km) daily data, yet current methods face challenges in balancing accuracy, coverage, and resolution. Chemical transport models such as those from the Copernicus Atmosphere Monitoring Service (CAMS) offer continuous data but their relatively coarse resolution can introduce uncertainties. Here we present a synergistic Machine Learning (ML)-based approach called S-MESH (Satellite and ML-based Estimation of Surface air quality at High resolution) for estimating daily surface PM2.5 over Europe at 1 km spatial resolution and demonstrate its performance for the years 2021 and 2022. The approach enhances and downscales the CAMS regional ensemble 24 h PM2.5 forecast by training a stacked XGBoost model against station observations, effectively integrating satellite-derived data and modeled meteorological variables. Overall, against station observations, S-MESH (mean absolute error (MAE) of 3.54 μg/m3) shows higher accuracy than the CAMS forecast (MAE of 4.18 μg/m3) and is approaching the accuracy of the CAMS regional interim reanalysis (MAE of 3.21 μg/m3), while exhibiting a significantly reduced mean bias (MB of −0.3 μg/m3 vs. −1.5 μg/m3 for the reanalysis). At the same time, S-MESH requires substantially less computational resources and processing time. At concentrations >20 μg/m3, S-MESH outperforms the reanalysis (MB of −7.3 μg/m3 and -10.3 μg/m3 respectively), and reliably captures high pollution events in both space and time. In the eastern study area, where the reanalysis often underestimates, S-MESH better captures high levels of PM2.5 mostly from residential heating. S-MESH effectively tracks day-to-day variability, with a temporal relative absolute error of 5% (reanalysis 10%). Exhibiting good performance at high pollution events coupled with its high spatial resolution and rapid estimation speed, S-MESH can be highly relevant for air quality assessments where both resolution and timeliness are critical.
2024
An Unprecedented Arctic Ozone Depletion Event During Spring 2020 and Its Impacts Across Europe
The response of the ozone column across Europe to the extreme 2020 Arctic ozone depletion was examined by analyzing ground-based observations at 38 European stations. The ozone decrease at the northernmost site, Ny-Ålesund (79°N) was about 43% with respect to a climatology of more than 30 years. The magnitude of the decrease declined by about 0.7% deg−1 moving south to reach nearly 15% at 40°N. In addition, it was found that the variations of the ozone column at each of the selected stations in March-May were similar to those observed at Ny-Ålesund but with a delay increasing to about 20 days at mid-latitudes with a gradient of approximately 0.5 days deg−1. The distributions of reconstructed ozone column anomalies over a sector covering a large European area show decreasing ozone that started from the north at the beginning of April 2020 and spread south. Such behavior was shown to be similar to that observed after the Arctic ozone depletion in 2011. Stratospheric dynamical patterns in March–May 2011 and during 2020 suggested that the migration of ozone-poor air masses from polar areas to the south after the vortex breakup caused the observed ozone responses. A brief survey of the ozone mass mixing ratios at three stratospheric levels showed the exceptional strength of the 2020 episode. Despite the stronger and longer-lasting Arctic ozone loss in 2020, the analysis in this work indicates a similar ozone response at latitudes below 50°N to both 2011 and 2020 phenomena.
2023
2020
2023
2025
Optical properties of surface aerosols at Dome C, Antarctica, in 2007–2013 and their potential source areas are presented. Scattering coefficients (σsp) were calculated from measured particle number size distributions with a Mie code and from filter samples using mass scattering efficiencies. Absorption coefficients (σap) were determined with a three-wavelength Particle Soot Absorption Photometer (PSAP) and corrected for scattering by using two different algorithms. The scattering coefficients were also compared with σsp measured with a nephelometer at the South Pole Station (SPO). The minimum σap was observed in the austral autumn and the maximum in the austral spring, similar to other Antarctic sites. The darkest aerosol, i.e., the lowest single-scattering albedo ωo≈0.91, was observed in September and October and the highest ωo≈0.99 in February and March. The uncertainty of the absorption Ångström exponent αap is high. The lowest αap monthly medians were observed in March and the highest in August–October. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the SPO and two coastal sites, Neumayer and Syowa. The maximum monthly median eBC concentrations are almost the same ( ng m−3) at all these sites in October–November. This suggests that there is no significant difference in eBC concentrations between the coastal and plateau sites. The seasonal cycle of the eBC mass fraction exhibits a minimum f(eBC) ≈0.1 % in February–March and a maximum ∼4 %–5 % in August–October. Source areas were calculated using 50 d FLEXPART footprints. The highest eBC concentrations and the lowest ωo were associated with air masses coming from South America, Australia and Africa. Vertical simulations that take BC particle removal processes into account show that there would be essentially no BC particles arriving at Dome C from north of latitude 10∘ S at altitudes
2022
2024
Abating N in Nordic agriculture - Policy, measures and way forward
During the past twenty years, the Nordic countries (Denmark, Sweden, Finland and Norway) have introduced a range of measures to reduce losses of nitrogen (N) to air and to aquatic environment by leaching and runoff. However, the agricultural sector is still an important N source to the environment, and projections indicate relatively small emission reductions in the coming years.
The four Nordic countries have different priorities and strategies regarding agricultural N flows and mitigation measures, and therefore they are facing different challenges and barriers. In Norway farm subsidies are used to encourage measures, but these are mainly focused on phosphorus (P). In contrast, Denmark targets N and uses control regulations to reduce losses. In Sweden and Finland, both voluntary actions combined with subsidies help to mitigate both N and P.
The aim of this study was to compare the present situation pertaining to agricultural N in the Nordic countries as well as to provide recommendations for policy instruments to achieve cost effective abatement of reactive N from agriculture in the Nordic countries, and to provide guidance to other countries.
To further reduce N losses from agriculture, the four countries will have to continue to take different routes. In particular, some countries will need new actions if 2020 and 2030 National Emissions Ceilings Directive (NECD) targets are to be met. Many options are possible, including voluntary action, regulation, taxation and subsidies, but the difficulty is finding the right balance between these policy options for each country.
The governments in the Nordic countries should put more attention to the NECD and consult with relevant stakeholders, researchers and farmer's associations on which measures to prioritize to achieve these goals on time. It is important to pick remaining low hanging fruits through use of the most cost effective mitigation measures. We suggest that N application rate and its timing should be in accordance with the crop need and carrying capacity of environmental recipients. Also, the choice of application technology can further reduce the risk of N losses into air and waters. This may require more region-specific solutions and knowledge-based support with tailored information in combination with further targeted subsidies or regulations.
2019
We analyzed long-term measurements of organic carbon, elemental carbon, and source-specific organic tracers from 2017 to 2020 to constrain carbonaceous aerosol sources in the rapidly changing Arctic. Additionally, we used absorption photometer (Aethalometer) measurements to constrain equivalent black carbon (eBC) from biomass burning and fossil fuel combustion, using positive matrix factorization (PMF).
Our analysis shows that organic tracers are essential for understanding Arctic carbonaceous aerosol sources. Throughout 2017 to 2020, levoglucosan exhibited bimodal seasonality, reflecting emissions from residential wood combustion (RWC) in the heating season (November to May) and from wildfires (WFs) in the non-heating season (June to October), demonstrating a pronounced interannual variability in the influence of WF. Biogenic secondary organic aerosol (BSOA) species (2-methyltetrols) from isoprene oxidation was only present in the non-heating season, peaking in July to August. Warm air masses from Siberia led to a substantial increase in 2-methyltetrols in 2019 and 2020 compared to 2017 to 2018. This highlights the need to investigate the contribution of local sources vs. long-range atmospheric transport (LRT), considering the temperature sensitivity of biogenic volatile organic compound emissions from Arctic vegetation. Tracers of primary biological aerosol particles (PBAPs), including various sugars and sugar alcohols, showed elevated levels in the non-heating season, although with different seasonal trends, whereas cellulose had no apparent seasonality. Most PBAP tracers and 2-methyltetrols peaked during influence of WF emissions, highlighting the importance of measuring a range of source-specific tracers to understand sources and dynamics of carbonaceous aerosol. The seasonality of carbonaceous aerosol was strongly influenced by LRT episodes, as background levels are extremely low. In the non-heating season, the organic aerosol peak was as influenced by LRT, as was elemental carbon during the Arctic haze period.
Source apportionment of carbonaceous aerosol by Latin hypercube sampling showed mixed contributions from RWC (46 %), fossil fuel (FF) sources (27 %), and BSOA (25 %) in the heating season. In contrast, the non-heating season was dominated by BSOA (56 %), with lower contributions from WF (26 %) and FF sources (15 %).
Source apportionment of eBC by PMF showed that FF combustion dominated eBC (70±2.7 %), whereas RWC (22±2.7 %) was more abundant than WF (8.0±2.9 %). Modeled BC concentrations from FLEXPART (FLEXible PARTicle dispersion model) attributed an almost equal share to FF sources (51±3.1 %) and to biomass burning. Both FLEXPART and the PMF analysis concluded that RWC is a more important source of (e)BC than WF. However, with a modeled RWC contribution of 30±4.1 % and WF of 19±2.8 %, FLEXPART suggests relatively higher contributions to eBC from these sources. Notably, the BB fraction of EC was twice as high as that of eBC, reflecting methodological differences between source apportionment by LHS and PMF. However, important conclusions drawn are unaffected, as both methods indicate the presence of RWC- and WF-sourced BC at Zeppelin, with a higher relative BB contribution during the non-heating season.
In summary, organic aerosol (281±106 ng m−3) constitutes a significant fraction of Arctic PM10, although surpassed by sea salt aerosol (682±46.9 ng m−3), mineral dust (613±368 ng m−3), and typically non-sea-salt sulfate SO (314±62.6 ng m−3), originating mainly from anthropogenic sources in winter and from natural sources in summer.
2024