Modelling the relationship between liquid water content and cloud droplet number concentration observed in low clouds in the summer Arctic and its radiative effects

Low clouds persist in the summer Arctic with important consequences for the radiation budget. In this study, we simulate the linear relationship between liquid water content (LWC) and cloud droplet number concentration (CDNC) observed during an aircraft campaign based out of Resolute Bay, Canada, conducted as part of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments study in July 2014. Using a single-column model, we find that autoconversion can explain the observed linear relationship between LWC and CDNC. Of the three autoconversion schemes we examined, the scheme using continuous drizzle (Khairoutdinov and Kogan, 2000) appears to best reproduce the observed linearity in the tenuous cloud regime (Mauritsen et al., 2011), while a scheme with a threshold for rain (Liu and Daum, 2004) best reproduces the linearity at higher CDNC. An offline version of the radiative transfer model used in the Canadian Atmospheric Model version 4.3 is used to compare the radiative effects of the modelled and observed clouds. We find that there is no significant difference in the upward longwave cloud radiative effect at the top of the atmosphere from the three autoconversion schemes (p=0.05) but that all three schemes differ at p=0.05 from the calculations based on observations. In contrast, the downward longwave and shortwave cloud radiative effect at the surface for the Wood (2005b) and Khairoutdinov and Kogan (2000) schemes do not differ significantly (p=0.05) from the observation-based radiative calculations, while the Liu and Daum (2004) scheme differs significantly from the observation-based calculation for the downward shortwave but not the downward longwave fluxes.This research has been supported by the Natural Sciences and Engineering Research Council of Canada (Discovery Grants RGPIN-2014-05173 and RGPIN 155649) and the Marine Environmental Observation, Prediction and Response Network (MEOPAR), which is a federally funded Networks of Centres of Excellence (NCE) (EC1-RC-DAL).Peer ReviewedPostprint (published version

Characterization of transport regimes and the polar dome during Arctic spring and summer using in situ aircraft measurements

Abstract. The springtime composition of the Arctic lower troposphere is to a large extent controlled by the transport of midlatitude air masses into the Arctic. In contrast, pre- cipitation and natural sources play the most important role during summer. Within the Arctic region sloping isentropes create a barrier to horizontal transport, known as the polar dome. The polar dome varies in space and time and exhibits a strong influence on the transport of air masses from mid- latitudes, enhancing transport during winter and inhibiting transport during summer. We analyzed aircraft-based trace gas measurements in the Arctic from two NETCARE airborne field campaigns (July 2014 and April 2015) with the Alfred Wegener Insti- tute Polar 6 aircraft, covering an area from Spitsbergen to Alaska (134 to 17◦ W and 68 to 83◦ N). Using these data we characterized the transport regimes of midlatitude air masses traveling to the high Arctic based on CO and CO2 mea- surements as well as kinematic 10 d back trajectories. We found that dynamical isolation of the high Arctic lower tro- posphere leads to gradients of chemical tracers reflecting dif- ferent local chemical lifetimes, sources, and sinks. In par- ticular, gradients of CO and CO2 allowed for a trace-gas- based definition of the polar dome boundary for the two mea- surement periods, which showed pronounced seasonal differences. Rather than a sharp boundary, we derived a transi- tion zone from both campaigns. In July 2014 the polar dome boundary was at 73.5◦ N latitude and 299–303.5 K potential temperature. During April 2015 the polar dome boundary was on average located at 66–68.5◦ N and 283.5–287.5 K. Tracer–tracer scatter plots confirm different air mass prop- erties inside and outside the polar dome in both spring and summer. Further, we explored the processes controlling the recent transport history of air masses within and outside the polar dome. Air masses within the springtime polar dome mainly experienced diabatic cooling while traveling over cold sur- faces. In contrast, air masses in the summertime polar dome were diabatically heated due to insolation. During both sea- sons air masses outside the polar dome slowly descended into the Arctic lower troposphere from above through ra- diative cooling. Ascent to the middle and upper troposphere mainly took place outside the Arctic, followed by a north- ward motion. Air masses inside and outside the polar dome were also distinguished by different chemical compositions of both trace gases and aerosol particles. We found that the fraction of amine-containing particles, originating from Arc- tic marine biogenic sources, is enhanced inside the polar dome. In contrast, concentrations of refractory black carbon are highest outside the polar dome, indicating remote pollu- tion sources. Synoptic-scale weather systems frequently disturb the transport barrier formed by the polar dome and foster ex- change between air masses from midlatitudes and polar re- gions. During the second phase of the NETCARE 2014 measurements a pronounced low-pressure system south of Resolute Bay brought inflow from southern latitudes, which pushed the polar dome northward and significantly affected trace gas mixing ratios in the measurement region. Mean CO mixing ratios increased from 77.9 ± 2.5 to 84.9 ± 4.7 ppbv between these two regimes. At the same time CO2 mix- ing ratios significantly decreased from 398.16 ± 1.01 to 393.81 ± 2.25 ppmv. Our results demonstrate the utility of applying a tracer-based diagnostic to determine the polar dome boundary for interpreting observations of atmospheric composition in the context of transport history

Trans-Pacific Transport of Saharan Dust to Western North America: A Case Study

The first documented case of long range transport of Saharan dust over a pathway spanning Asia and the Pacific to Western North America is described. Crustal material generated by North African dust storms during the period 28 February - 3 March 2005 reached western Canada on 13-14 March 2005 and was observed by lidar and sunphotometer in the Vancouver region and by high altitude aerosol instrumentation at Whistler Peak. Global chemical models (GEOS-CHEM and NRL NAAPS) confirm the transport pathway and suggest source attribution was simplified in this case by the distinct, and somewhat unusual, lack of dust activity over Eurasia (Gobi and Takla Makan deserts) at this time. Over western North America, the dust layer, although subsiding close to the boundary layer, did not appear to contribute to boundary layer particulate matter concentrations. Furthermore, sunphotometer observations (and associated inversion products) suggest that the dust layer had only subtle optical impact (Aerosol Optical Thickness (Tau(sub a500)) and Angstrom exponent (Alpha(sub 440-870) were 0.1 and 1.2 respectively) and was dominated by fine particulate matter (modes in aerodynamic diameter at 0.3 and 2.5microns). High Altitude observations at Whistler BC, confirm the crustal origin of the layer (rich in Ca(++) ions) and the bi-modal size distribution. Although a weak event compared to the Asian Trans-Pacific dust events of 1998 and 2001, this novel case highlights the possibility that Saharan sources may contribute episodically to the aerosol burden in western North America

Arctic marine secondary organic aerosol contributes significantly to summertime particle size distributions in the Canadian Arctic Archipelago

Summertime Arctic aerosol size distributions are strongly controlled by natural regional emissions. Within this context, we use a chemical transport model with sizeresolved aerosol microphysics (GEOS-Chem-TOMAS) to interpret measurements of aerosol size distributions from the Canadian Arctic Archipelago during the summer of 2016, as part of the "NETwork on Climate and Aerosols: Addressing key uncertainties in Remote Canadian Environments" (NETCARE) project. Our simulations suggest that condensation of secondary organic aerosol (SOA) from precursor vapors emitted in the Arctic and near Arctic marine (ice-free seawater) regions plays a key role in particle growth events that shape the aerosol size distributions observed at Alert (82.5° N, 62.3° W), Eureka (80.1° N, 86.4° W), and along a NETCARE ship track within the Archipelago. We refer to this SOA as Arctic marine SOA (AMSOA) to reflect the Arctic marine-based and likely biogenic sources for the precursors of the condensing organic vapors. AMSOA from a simulated flux (500 μgm-2 day-1, north of 50° N) of precursor vapors (with an assumed yield of unity) reduces the summertime particle size distribution model-observation mean fractional error 2- to 4-fold, relative to a simulation without this AMSOA. Particle growth due to the condensable organic vapor flux contributes strongly (30 %-50 %) to the simulated summertime-mean number of particles with diameters larger than 20 nm in the study region. This growth couples with ternary particle nucleation (sulfuric acid, ammonia, and water vapor) and biogenic sulfate condensation to account for more than 90% of this simulated particle number, which represents a strong biogenic influence. The simulated fit to summertime size-distribution observations is further improved at Eureka and for the ship track by scaling up the nucleation rate by a factor of 100 to account for other particle precursors such as gas-phase iodine and/or amines and/or fragmenting primary particles that could be missing from our simulations. Additionally, the fits to the observed size distributions and total aerosol number concentrations for particles larger than 4 nm improve with the assumption that the AMSOA contains semivolatile species: the model-observation mean fractional error is reduced 2- to 3-fold for the Alert and ship track size distributions. AMSOA accounts for about half of the simulated particle surface area and volume distributions in the summertime Canadian Arctic Archipelago, with climaterelevant simulated summertime pan-Arctic-mean top-of-theatmosphere aerosol direct (-0:04Wm-2) and cloud-albedo indirect (-0:4Wm-2) radiative effects, which due to uncertainties are viewed as an order of magnitude estimate. Future work should focus on further understanding summertime Arctic sources of AMSOA

Aircraft-based measurements of High Arctic springtime aerosol show evidence for vertically varying sources, transport and composition

The sources, chemical transformations and re- moval mechanisms of aerosol transported to the Arctic are key factors that control Arctic aerosol–climate interactions. Our understanding of sources and processes is limited by a lack of vertically resolved observations in remote Arctic re- gions. We present vertically resolved observations of trace gases and aerosol composition in High Arctic springtime, made largely north of 80◦ N, during the NETCARE cam- paign. Trace gas gradients observed on these flights defined the polar dome as north of 66–68◦ 30′ N and below poten- tial temperatures of 283.5–287.5 K. In the polar dome, we observe evidence for vertically varying source regions and chemical processing. These vertical changes in sources and chemistry lead to systematic variation in aerosol composition as a function of potential temperature. We show evidence for sources of aerosol with higher organic aerosol (OA), ammo- nium and refractory black carbon (rBC) content in the upper polar dome. Based on FLEXPART-ECMWF calculations, air masses sampled at all levels inside the polar dome (i.e., po- tential temperature 10 days) in the Arc- tic, while air masses in the upper polar dome had entered the Arctic more recently. Variations in aerosol composition were closely related to transport history. In the lower polar dome, the measured sub-micron aerosol mass was dominated by sulfate (mean 74 %), with lower contributions from rBC (1 %), ammonium (4 %) and OA (20 %). At higher altitudes and higher potential temperatures, OA, ammonium and rBC contributed 42 %, 8 % and 2 % of aerosol mass, respectively. A qualitative indication for the presence of sea salt showed that sodium chloride contributed to sub-micron aerosol in the lower polar dome, but was not detectable in the upper po- lar dome. Our observations highlight the differences in Arc- tic aerosol chemistry observed at surface-based sites and the aerosol transported throughout the depth of the Arctic tropo- sphere in spring

High Arctic aircraft measurements characterising black carbon vertical variability in spring and summer

The vertical distribution of black carbon (BC) par- ticles in the Arctic atmosphere is one of the key parameters controlling their radiative forcing and thus role in Arctic cli- mate change. This work investigates the presence and prop- erties of these light-absorbing aerosols over the High Cana- dian Arctic ( > 70 degree N). Airborne campaigns were performed as part of the NETCARE project (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) and provided insights into the variability of the vertical distributions of BC particles in summer 2014 and spring 2015. The observation periods covered evolutions of cyclonic disturbances at the polar front, which favoured the transport of air pollution into the High Canadian Arctic, as otherwise this boundary between the air masses largely im- pedes entrainment of pollution from lower latitudes. A total of 48 vertical profiles of refractory BC (rBC) mass concen- tration and particle size, extending from 0.1 to 5.5 km altitude were obtained with a Single-Particle Soot Photometer (SP2). Generally, the rBC mass concentration decreased from spring to summer by a factor of 10. Such depletion was as- sociated with a decrease in the mean rBC particle diameter, from approximately 200 to 130 nm at low altitude. Due to the very low number fraction, rBC particles did not substantially contribute to the total aerosol population in summer. The analysis of profiles with potential temperature as ver- tical coordinate revealed characteristic variability patterns within specific levels of the cold and stably stratified, dome- like, atmosphere over the polar region. The associated his- tory of transport trajectories into each of these levels showed that the variability was induced by changing rates and effi- ciencies of rBC import. Generally, the source areas affecting the polar dome extended southward with increasing potential temperature (i.e. altitude) level in the dome. While the lower dome was mostly only influenced by low-level transport from sources within the cold central and marginal Arctic, for the mid-dome and upper dome during spring it was found that a cold air outbreak over eastern Europe caused intensified northward transport of air from a corridor over western Rus- sia to central Asia. This sector was affected by emissions from gas flaring, industrial activity and wildfires. The devel- opment of transport caused rBC concentrations in the second lowest level to gradually increase from 32 to 49 ng

Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79◦ N

Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, ver- tically resolved measurements of the particle light scatter- ing coefficient (σsp ) and light absorption coefficient (σap ) in the springtime Arctic atmosphere are infrequent, espe- cially measurements at latitudes at or above 80◦ N. Here, re- lationships among vertically distributed aerosol optical prop- erties (σap, σsp and single scattering albedo or SSA), par- ticle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4◦ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground- based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing Sys- tem (GEOS) model, GEOS-Chem, coupled with the TwO- Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, be- cause the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass ab- sorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two aver- aged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the obser- vations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap/2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Me- dian values of the measured σap, rBC and the organic com- ponent of particles all increase by a factor of 1.8 ± 0.1, going from near-surface to 750 hPa, and values higher than the sur- face persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The dif- ferences between modelled and observed optical properties follow the same trend as the differences between the mod- elled and observed concentrations of the carbonaceous com- ponents (black and organic). Model-observation discrepan- cies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp < 15 Mm−1. The large uncertainties in measuring optical properties and BC, and the large differ- ences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic

Size-resolved mixing state of black carbon in the Canadian high Arctic and implications for simulated direct radiative effect

Transport of anthropogenic aerosol into the Arc- tic in the spring months has the potential to affect regional climate; however, modeling estimates of the aerosol direct radiative effect (DRE) are sensitive to uncertainties in the mixing state of black carbon (BC). A common approach in previous modeling studies is to assume an entirely exter- nal mixture (all primarily scattering species are in separate particles from BC) or internal mixture (all primarily scat- tering species are mixed in the same particles as BC). To provide constraints on the size-resolved mixing state of BC, we use airborne single-particle soot photometer (SP2) and ultrahigh-sensitivity aerosol spectrometer (UHSAS) mea- surements from the Alfred Wegener Institute (AWI) Polar 6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter and the fraction of particles contain- ing rBC in the springtime Canadian high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find av- erage coating thicknesses of approximately 45 to 40 nm, re- spectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total par- ticle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16% to 3%, respec- tively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number dis- tributions from GEOS-Chem–TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely external or internal mixture. We find that the pan-Arctic average springtime DRE ranges fro