Abstract. During the 1-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, the German icebreaker Polarstern drifted through Arctic Ocean ice from October 2019 to May 2020, mainly at latitudes between 85 and 88.5∘ N. A multiwavelength polarization Raman lidar was operated on board the research vessel and continuously monitored aerosol and cloud layers up to a height of 30 km. During our mission, we expected to observe a thin residual volcanic aerosol layer in the stratosphere, originating from the Raikoke volcanic eruption in June 2019, with an aerosol optical thickness (AOT) of 0.005–0.01 at 500 nm over the North Pole area during the winter season. However, the highlight of our measurements was the detection of a persistent, 10 km deep aerosol layer in the upper troposphere and lower stratosphere (UTLS), from about 7–8 to 17–18 km height, with clear and unambiguous wildfire smoke signatures up to 12 km and an order of magnitude higher AOT of around 0.1 in the autumn of 2019. Case studies are presented to explain the specific optical fingerprints of aged wildfire smoke in detail. The pronounced aerosol layer was present throughout the winter half-year until the strong polar vortex began to collapse in late April 2020. We hypothesize that the detected smoke originated from extraordinarily intense and long-lasting wildfires in central and eastern Siberia in July and August 2019 and may have reached the tropopause layer by the self-lifting process. In this article, we summarize the main findings of our 7-month smoke observations and characterize the aerosol in terms of geometrical, optical, and microphysical properties. The UTLS AOT at 532 nm ranged from 0.05–0.12 in October–November 2019 and 0.03–0.06 during the main winter season. The Raikoke aerosol fraction was estimated to always be lower than 15 %. We assume that the volcanic aerosol was above the smoke layer (above 13 km height). As an unambiguous sign of the dominance of smoke in the main aerosol layer from 7–13 km height, the particle extinction-to-backscatter ratio (lidar ratio) at 355 nm was found to be much lower than at 532 nm, with mean values of 55 and 85 sr, respectively. The 355–532 nm Ångström exponent of around 0.65 also clearly indicated the presence of smoke aerosol. For the first time, we show a distinct view of the aerosol layering features in the High Arctic from the surface up to 30 km height during the winter half-year. Finally, we provide a vertically resolved view on the late winter and early spring conditions regarding ozone depletion, smoke occurrence, and polar stratospheric cloud formation. The latter will largely stimulate research on a potential impact of the unexpected stratospheric aerosol perturbation on the record-breaking ozone depletion in the Arctic in spring 2020.

Abstract. An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30 km height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5∘ N. The lidar was integrated into a complex remote-sensing infrastructure aboard the Polarstern. In this article, novel lidar techniques, innovative concepts to study aerosol–cloud interaction in the Arctic, and unique MOSAiC findings will be presented. The highlight of the lidar measurements was the detection of a 10 km deep wildfire smoke layer over the North Pole region between 7–8 km and 17–18 km height with an aerosol optical thickness (AOT) at 532 nm of around 0.1 (in October–November 2019) and 0.05 from December to March. The dual-wavelength Raman lidar technique allowed us to unambiguously identify smoke as the dominating aerosol type in the aerosol layer in the upper troposphere and lower stratosphere (UTLS). An additional contribution to the 532 nm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15 %. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper (Ohneiser et al., 2021). This smoke event offered the unique opportunity to study the influence of organic aerosol particles (serving as ice-nucleating particles, INPs) on cirrus formation in the upper troposphere. An example of a closure study is presented to explain our concept of investigating aerosol–cloud interaction in this field. The smoke particles were obviously able to control the evolution of the cirrus system and caused low ice crystal number concentration. After the discussion of two typical Arctic haze events, we present a case study of the evolution of a long-lasting mixed-phase cloud layer embedded in Arctic haze in the free troposphere. The recently introduced dual-field-of-view polarization lidar technique was applied, for the first time, to mixed-phase cloud observations in order to determine the microphysical properties of the water droplets. The mixed-phase cloud closure experiment (based on combined lidar and radar observations) indicated that the observed aerosol levels controlled the number concentrations of nucleated droplets and ice crystals.

Abstract. Continuous height-resolved observations of aerosol profiles over the central Arctic throughout a full year were performed for the first time. Such measurements covering aerosol layering features are required for an adequate modeling of Arctic climate conditions, especially with respect to a realistic consideration of cloud formation and here, in particular, of ice nucleation processes. MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) offered this favorable opportunity to monitor aerosol and clouds over the central Arctic over all four seasons, from October 2019 to September 2020. In this article, a summary of MOSAiC lidar observations aboard the icebreaker Polarstern of tropospheric aerosol products is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties (cloud condensation nucleus, CCN, and ice-nucleating particle concentrations, INPs) are discussed, separately for the lowest part of the troposphere (near the surface at 250 m height), within the lower free troposphere (2000 m height), and regarding INPs also near the tropopause (cirrus level, 8–10 km height). In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. Strong differences between summer and winter aerosol conditions were found. During the winter months (Arctic haze period) a strong decrease of the aerosol light extinction coefficient (532 nm) with height up to about 4–5 km height was found with values of 20–100 Mm-1 close to the surface and an order of magnitude less at 1500–2000 m height. Lofted aged wildfire smoke layers caused a re-increase of the aerosol concentration from the middle troposphere up to stratospheric heights and were continuously observable from October 2019 to May 2020. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm-1, were observed. Aerosol removal, controlled by cloud scavenging processes (widely suppressed in winter, very efficient in summer) in the lowermost 1–2 km of the atmosphere, seem to be the main reason for the strong differences between winter and summer aerosol conditions. In line with this pronounced annual cycle in the aerosol optical properties, CCN concentrations (0.2 % supersaturation level) ranged from 50–500 cm-3 in the atmospheric boundary layer (ABL) in winter and 1–40 cm-3 in summer. In the lower free troposphere, however, the CCN level was roughly constant throughout the year with values mostly from 30–100 cm-3. A strong contrast between winter to summer was also given in terms of ABL INPs which control ice production in low-level clouds. INP concentration of 0.01–0.2 L-1 prevailed in the ABL in winter at typical ice-nucleating cloud temperatures of -25 °C and assuming soil dust as the main INP type, and were roughly 2 orders of magnitude lower in the ABL in summer at typical cloud top temperatures of -10 °C. In the summer ABL, marine aerosol (biogenic components) is most probably the main INP type, continental INP contributions (e.g., soil dust INPs) are suppressed by efficient wet removal during long-range transport. A strong reduction in the INP population was also found in the lower free troposphere at 2000 m height from winter to summer (2 orders of magnitude), mostly due to the change in the prevailing ice-nucleation temperatures. Estimated INP concentration accumulated from 0.004–0.02 L-1 during the winter months. The highlight of the MOSAiC lidar studies was the detection of a persistent wildfire smoke layer in the upper troposphere and lower stratosphere from October 2019 to May 2020. The smoke particles (organic aerosol) triggered continuously cirrus formation at INP concentrations mostly from 1–20 L-1 close to the tropopause during the entire winter period.

Abstract. There is a gap between the need for city-wide air-quality simulations considering the intra-urban variability and mircoscale dispersion features and the computational capacities that conventional urban microscale models require. This gap can be bridged by targeting model applications on the gray zone situated between the mesoscale and large-eddy scale. The urban dispersion model CAIRDIO is a new contribution to the class of computational-fluid dynamics models operating in this scale range. It uses a diffuse-obstacle boundary method to represent buildings as physical obstacles at gray-zone resolutions in the order of tens of meters. The main objective of this approach is to find an acceptable compromise between computationally inexpensive grid sizes for spatially comprehensive applications and the required accuracy in the description of building and boundary-layer effects. In this paper, CAIRDIO is applied on the simulation of black carbon and particulate matter dispersion for an entire mid-size city using a uniform horizontal grid spacing of 40 m. For model evaluation, measurements from five operational air monitoring stations representative for the urban background and high-traffic roads are used. The comparison also includes the mesoscale host simulation, which provides the boundary conditions. The measurements show a dominant influence of the mixing layer evolution at background sites, and therefore both the mesoscale and large-eddy simulation (LES) results are in good agreement with the observed air pollution levels. In contrast, at the high-traffic sites the proximity to emissions and the interactions with the building environment lead to a significantly amplified diurnal variability in pollutant concentrations. These urban road conditions can only be reasonably well represented by CAIRDIO while the meosocale simulation indiscriminately reproduces a typical urban-background profile, resulting in a large positive model bias. Remaining model discrepancies are further addressed by a grid-spacing sensitivity study using offline-nested refined domains. The results show that modeled peak concentrations within street canyons can be further improved by decreasing the horizontal grid spacing down to 10 m, but not beyond. Obviously, the default grid spacing of 40 m is too coarse to represent the specific environment within narrow street canyons. The accuracy gains from the grid refinements are still only modest compared to the remaining model error, which to a large extent can be attributed to uncertainties in the emissions. Finally, the study shows that the proposed gray-scale modeling is a promising downscaling approach for urban air-quality applications. The results, however, also show that aspects other than the actual resolution of flow patterns and numerical effects can determine the simulations at the urban microscale.

Abstract. An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, lasting from September 2019 to October 2020, to contiuously monitor aerosol and cloud layers in the Central Arctic up to 30 km height at latitudes mostly between 85° N and 88.5° N. The lidar was integrated in a complex remote sensing infrastructure aboard Polarstern. Modern aerosol lidar methods and new lidar techniques and concepts to explore aerosol-cloud interaction were applied for the first time in the Central Arctic. Aim of the introductory article is to provide an overview of the observational spectrum of the lidar products for representative measurement cases. Highlight of the lidar measurements was the detection of a 10 km deep wildfire smoke layer over the North Pole area from, on average, 7 km to 17 km height with an aerosol optical thickness (AOT) at 532 nm around 0.1 (in October–November 2019) and 0.05 from December to mid of March 2020. The wildfire smoke was trapped within the extraordinarily strong polar vortex and remained detectable until the beginning of May 2020. Arctic haze was also monitored and characterized in terms of backscatter, extinction, and extinction-to-backscatter ratio at 355 and 532 nm. High lidar ratios from 60–100 sr in lofted mixed haze and smoke plumes are indicative for the presence of strongly light-absorbing fine-mode particles. The AOT at 532 nm was of the order of 0.025 for the tropospheric haze layers. In addition, so-called cloud closure experiments were applied to Arctic mixed-phase cloud and cirrus observations. The good match between cloud condensation nucleus concentration (CCNC) and cloud droplet number concentration (CDNC) and, on the other hand, between ice-nucleating particle concentration (INPC) and ice crystal number concentration (ICNC) indicated a clear influence of aerosol particles on the evolution of the cloud systems. CDNC was mostly between 20 and 100 cm−3 in the liquid-water dominated cloud top layer. ICNC was of the order of 0.1–1 L−1. The study of the impact of wildfire smoke particles on cirrus formation revealed that heterogeneous ice formation with smoke particles (organic aerosol particles) as INPs may have prevailed. ICNC values of 10–40 L−1 were clearly below ICNC levels that would indicate homogeneous freezing.