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The Zeppelin Observatory (78.90∘ N, 11.88∘ E) is located on Zeppelin Mountain at 472 m a.s.l. on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of Ny-Ålesund Research Station and an important atmospheric measurement site, one of only a few in the high Arctic, and a part of several European and global monitoring programmes and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP); the Arctic Monitoring and Assessment Programme (AMAP); the Global Atmosphere Watch (GAW); the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS); the Advanced Global Atmospheric Gases Experiment (AGAGE) network; and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University, and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena, and provide an outline of future research directions.

A total of 22 polycyclic aromatic hydrocarbons (PAHs), 29 oxy-PAHs, and 35 nitro-PAHs (polycyclic aromatic compounds, PACs) were measured in gaseous and particulate phases in the ambient air of Longyearbyen, the most populated settlement in Svalbard, the European Arctic. The sampling campaign started in the polar night in November 2017 and lasted for 8 months until June 2018, when a light cycle reached a sunlit period with no night. The transport regimes of the near-surface, potentially polluted air masses from midlatitudes to the Arctic and the polar boundary layer meteorology were studied. The data analysis showed the observed winter PAC levels were mainly influenced by the lower-latitude sources in northwestern Eurasia, while local emissions dominated in spring and summer. The highest PAC concentrations observed in spring, with PAH concentrations a factor of 30 higher compared to the measurements at the closest background station in Svalbard (Zeppelin, 115 km distance from Longyearbyen), were attributed to local snowmobile-driving emissions. The lowest PAC concentrations were expected in summer due to enhanced photochemical degradation under the 24 h midnight sun conditions and inhibited long-range atmospheric transport. In contrast, the measured summer concentrations were notably higher than those in winter due to the harbour (ship) emissions.

Long-term monitoring of regulated organic chemicals, such as legacy persistent organic pollutants (POPs) and polycyclic aromatic hydrocarbons (PAHs), in ambient air provides valuable information about the compounds' environmental fate as well as temporal and spatial trends. This is the foundation to evaluate the effectiveness of national and international regulations for priority pollutants. Extracts of high-volume air samples, collected on glass fibre filters (GFF for particle phase) and polyurethane foam plugs (PUF for gaseous phase), for targeted analyses of legacy POPs are commonly cleaned by treatment with concentrated sulfuric acid, resulting in extracts clean from most interfering compounds and matrices that are suitable for multi-quantitative trace analysis. Such standardised methods, however, severely restrict the number of analytes for quantification and are not applicable when targeting new and emerging compounds as some may be less stable under acid treatment. Recently developed suspect and non-target screening analytical strategies (SUS and NTS, respectively) are shown to be effective evaluation tools aimed at identifying a high number of compounds of emerging concern. These strategies, combining highly sophisticated analytical technology with extensive data interpretation and statistics, are already widely accepted in environmental sciences for investigations of various environmental matrices, but their application to air samples is still very limited. In order to apply SUS and NTS for the identification of organic contaminants in air samples, an adapted and more wide-scope sample clean-up method is needed compared to the traditional method, which uses concentrated sulfuric acid. Analysis of raw air sample extracts without clean-up would generate extensive contamination of the analytical system, especially with PUF matrix-based compounds, and thus highly interfered mass spectra and detection limits which are unacceptable high for trace analysis in air samples. In this study, a novel wide-scope sample clean-up method for high-volume air samples has been developed and applied to real high-volume air samples, which facilitates simultaneous target, suspect and non-target analyses. The scope and efficiency of the method were quantitatively evaluated with organic compounds covering a wide range of polarities (logP 2–11), including legacy POPs, brominated flame retardants (BFRs), chlorinated pesticides and currently used pesticides (CUPs). In addition, data reduction and selection strategies for SUS and NTS were developed for comprehensive two-dimensional gas chromatography separation with low-resolution time-of-flight mass spectrometric detection (GC × GC-LRMS) data and applied to real high-volume air samples. Combination of the newly developed clean-up procedure and data treatment strategy enabled the prioritisation of over 600 compounds of interest in the particle phase (on GFF) and over 850 compounds in the gas phase (on PUF) out of over 25 000 chemical features detected in the raw dataset. Of these, 50 individual compounds were identified and confirmed with reference standards, 80 compounds were identified with a probable structure, and 774 compounds were assigned to various compound classes. In the dataset available here, 11 hitherto unknown halogenated compounds were detected. These unknown compounds were not yet listed in the available mass spectral libraries.

Polycyclic aromatic hydrocarbons (PAHs) are not declining in Arctic air despite reductions in their global emissions. In Svalbard, the Longyearbyen coal-fired power plant is considered to be one of the major local sources of PAHs. Power plant stack emissions and ambient air samples, collected simultaneously at 1 km (UNIS) and 6 km (Adventdalen) transect distance, were analysed (gaseous and particulate phases separately) for 22 nitro-PAHs, 8 oxy-PAHs, and 16 parent PAHs by gas chromatography in combination with single quadrupole electron capture negative ionization mass spectrometry (GC-ECNI-MS) and gas chromatography in combination with triple quadrupole electron ionization mass spectrometry (GC-EI-MS/MS). Results confirm low levels of PAH emissions (∑16 PAHs =1.5 µg kg−1 coal) from the power plant. Phenanthrene, 9,10-anthraquinone, 9-fluorenone, fluorene, fluoranthene, and pyrene accounted for 85 % of the plant emission (not including naphthalene). A dilution effect was observed for the transect ambient air samples: 1.26±0.16 and 0.63±0.14 ng m−3 were the sum of all 47 PAH derivatives for UNIS and Adventdalen, respectively. The PAH profile was homogeneous for these recipient stations with phenanthrene and 9-fluorenone being most abundant. Multivariate statistical analysis confirmed coal combustion and vehicle and marine traffic as the predominant sources of PAHs. Secondary atmospheric formation of 9-nitroanthracene and 2+3-nitrofluoranthene was evaluated and concluded. PAHs partitioning between gaseous and particulate phases showed a strong dependence on ambient temperatures and humidity. The present study contributes important data which can be utilized to eliminate uncertainties in model predictions that aim to assess the extent and impacts of Arctic atmospheric contaminants.

The Norwegian Arctic possesses a unique environment for the detection of new potential chemicals of emerging Arctic concern (CEACs) due to remoteness, sparse population and the low number of local contamination sources. Hence, a contaminant present in Arctic air is still considered a priority indication for its environmental stability and environmental mobility. Today, legacy persistent organic pollutants (POPs) and related conventional environmental pollutants are already well-studied because of their identification as Arctic pollutants in the 1980s. Many of them are implemented and reported in various national and international monitoring activities including the Arctic Monitoring and Assessment Programme (AMAP). These standard monitoring schemes, however, are based on compound-specific quantitative analytical methods. Under such conditions, the possibility for the identification of hitherto unidentified contaminants is limited and random at best. Today, new and advanced technological developments allow a broader, unspecific analytical approach as either targeted multicomponent analysis or suspect and non-target screening strategies. In order to facilitate such a wide range of compounds, a wide-scope sample clean-up method for high-volume air samples based on a combination of adsorbents was applied, followed by comprehensive two-dimensional gas chromatography separation and low-resolution time-of-flight mass spectrometric detection (GC × GC-LRMS). During the study reported here, simultaneous non-target and suspect screening were applied. The detection of over 700 compounds of interest in the particle phase and over 1200 compounds in the gaseous phase is reported. Of those, 62 compounds were confirmed with reference standards and 90 compounds with a probable structure (based upon mass spectrometric interpretation and library spectrum comparison). These included compounds already detected in Arctic matrices and compounds not detected previously (see also Fig. 1). In addition, 241 compounds were assigned a tentative structure or compound class. Hitherto unknown halogenated compounds, which are not listed in the mass spectral libraries used, were also detected and partly identified.

A first long-term monitoring of selected persistent organic pollutants (POPs) in Antarctic air has been conducted at the Norwegian research station Troll (Dronning Maud Land). As target contaminants 32 PCB congeners, α- and γ-hexachlorocyclohexane (HCH), trans- and cis-chlordane, trans- and cis-nonachlor, p,p'- and o,p-DDT, DDD, DDE as well as hexachlorobenzene (HCB) were selected. The monitoring program with weekly samples taken during the period 2007–2010 was coordinated with the parallel program at the Norwegian Arctic monitoring site (Zeppelin mountain, Ny-Ålesund, Svalbard) in terms of priority compounds, sampling schedule as well as analytical methods. The POP concentration levels found in Antarctica were considerably lower than Arctic atmospheric background concentrations. Similar to observations for Arctic samples, HCB is the predominant POP compound, with levels of around 22 pg m−3 throughout the entire monitoring period. In general, the following concentration distribution was found for the Troll samples analyzed: HCB > Sum HCH > Sum PCB > Sum DDT > Sum chlordanes. Atmospheric long-range transport was identified as a major contamination source for POPs in Antarctic environments. Several long-range transport events with elevated levels of pesticides and/or compounds with industrial sources were identified based on retroplume calculations with a Lagrangian particle dispersion model (FLEXPART).

The cryosphere is an important component of global organic contaminant cycles. Snow is an efficient scavenger of atmospheric organic pollutants while a seasonal snowpack, sea ice, glaciers and ice caps are contaminant reservoirs on time scales ranging from days to millennia. Important physical and chemical processes occurring in the various cryospheric compartments impact contaminant cycling and fate. A variety of interactions and feedbacks also occur within the cryospheric system, most of which are susceptible to perturbations due to climate change. In this article, we review the current state of knowledge regarding the transport and processing of organic contaminants in the global cryosphere with an emphasis on the role of a changing climate. Given the complexity of contaminant interactions with the cryosphere and limitations on resources and research capacity, interdisciplinary research and extended collaborations are essential to close identified knowledge gaps and to improve our understanding of contaminant fate under a changing climate.

An extensive database of organochlorine (OC) pesticide concentrations measured at the Norwegian Arctic monitoring station at Ny-Ålesund, Svalbard, was analysed to assess longer-term trends in the Arctic atmosphere. Dynamic Harmonic Regression (DHR) is employed to investigate the seasonal and cyclical behaviour of chlordanes, DDTs and hexachlorobenzene (HCB), and to isolate underlying inter-annual trends. Although a simple comparison of annual mean concentrations (1994–2005) suggest a decline for all of the OCs investigated, the longer-term trends identified by DHR only show a significant decline for p,p'-DDT. Indeed, HCB shows an increase from 2003–2005. This is thought to be due to changes in source types and the presence of impurities in current use pesticides, together with retreating sea ice affecting air-water exchange. Changes in source types were revealed by using isomeric ratios for the chlordanes and DDTs. Declining trends in ratios of trans-chlordane/cis-chlordane (TC/CC) indicate a shift from primary sources, to more "weathered" secondary sources, whereas an increasing trend in o,p'-DDT/p,p'-DDT ratios indicate a shift from use of technical DDT to dicofol. Continued monitoring of these OC pesticides is required to fully understand the influence of a changing climate on the behaviour and environmental cycling of these chemicals in the Arctic as well as possible impacts from "new" sources.