CNT Parameterization Based on the Observed INP Concentration during Arctic Summer Campaigns in a Marine Environment

Aerosol–cloud interactions present a large source of uncertainties in atmospheric and climate models. One of the main challenges to simulate ice clouds is to reproduce the right ice nucleating particle concentration. In this study, we derive a parameterization for immersion freezing according to the classical nucleation theory. Our objective was to constrain this parameterization with observations taken over the Canadian Arctic during the Amundsen summer 2014 and 2016 campaigns. We found a linear dependence of contact angle and temperature. Using this approach, we were able to reproduce the scatter in ice nucleated particle concentrations within a factor 5 of observed values with a small negative bias. This parameterization would be easy to implement in climate and atmospheric models, but its representativeness has to first be validated against other datasets.Science, Faculty ofNon UBCChemistry, Department ofReviewedFacult

A new parameterization of ice heterogeneous nucleation coupled to aerosol chemistry in WRF-Chem model version 3.5.1: evaluation through ISDAC measurements

International audienceIn the Arctic, during polar night and early spring, ice clouds are separated into two leading types of ice clouds (TICs): (1) TIC1 clouds characterized by a large concentration of very small crystals and TIC2 clouds characterized by a low concentration of large ice crystals. Using a suitable parameterization of heterogeneous ice nucleation is essential for properly representing ice clouds in meteorological and climate models and subsequently understanding their interactions with aerosols and radiation. Here, we describe a new parameterization for ice crystal formation by heterogeneous nucleation in water-subsaturated conditions coupled to aerosol chemistry in the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). The parameterization is implemented in the Milbrandt and Yau (2005a, b) two-moment cloud microphysics scheme, and we assess how the WRF-Chem model responds to the run-time interaction between chemistry and the new parameterization. Well-documented reference cases provided us with in situ data from the spring 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) over Alaska. Our analysis reveals that the new parameterization clearly improves the representation of the ice water content (IWC) in polluted or unpolluted air masses and shows the poor performance of the reference parameterization in representing ice clouds with low IWC. The new parameterization is able to represent TIC1 and TIC2 microphysical characteristics at the top of the clouds, where heterogenous ice nucleation is most likely occurring, even with the known bias of simulated aerosols by WRF-Chem over the Arctic

Ice nucleating particles in the marine boundary layer in the Canadian Arctic during summer 2014

International audienceIce nucleating particles (INPs) in the Arctic can influence climate and precipitation in the region; yet our understanding of the concentrations and sources of INPs in this region remain uncertain. In the following, we (1) measured concentrations of INPs in the immersion mode in the Cana-dian Arctic marine boundary layer during summer 2014 on board the CCGS Amundsen, (2) determined ratios of surface areas of mineral dust aerosol to sea spray aerosol, and (3) investigated the source region of the INPs using particle dispersion modelling. Average concentrations of INPs at − 15, −20, and −25 • C were 0.005, 0.044, and 0.154 L −1 , respectively. These concentrations fall within the range of INP concentrations measured in other marine environments. For the samples investigated the ratio of mineral dust surface area to sea spray surface area ranged from 0.03 to 0.09. Based on these ratios and the ice active surface site densities of mineral dust and sea spray aerosol determined in previous laboratory studies, our results suggest that mineral dust is a more important contributor to the INP population than sea spray aerosol for the samples analysed. Based on particle dispersion modelling , the highest concentrations of INPs were often associated with lower-latitude source regions such as the Hudson Bay area, eastern Greenland, or northwestern continental Canada. On the other hand, the lowest concentrations were often associated with regions further north of the sampling sites and over Baffin Bay. A weak correlation was observed between INP concentrations and the time the air mass spent over bare land, and a weak negative correlation was observed between INP concentrations and the time the air mass spent over ice and open water. These combined results suggest that mineral dust from local sources is an important contributor to the INP population in the Canadian Arctic marine boundary layer during summer 2014

Balloon-borne match measurements of midlatitude cirrus clouds

Observations of high supersaturations with respect to ice inside cirrus clouds with high ice water content (> 0.01 g kg−1) and high crystal number densities (> 1 cm−3) are challenging our understanding of cloud microphysics and of climate feedback processes in the upper troposphere. However, single measurements of a cloudy air mass provide only a snapshot from which the persistence of ice supersaturation cannot be judged. We introduce here the "cirrus match technique" to obtain information about the evolution of clouds and their saturation ratio. The aim of these coordinated balloon soundings is to analyze the same air mass twice. To this end the standard radiosonde equipment is complemented by a frost point hygrometer, "SnowWhite", and a particle backscatter detector, "COBALD" (Compact Optical Backscatter AerosoL Detector). Extensive trajectory calculations based on regional weather model COSMO (Consortium for Small-Scale Modeling) forecasts are performed for flight planning, and COSMO analyses are used as a basis for comprehensive microphysical box modeling (with grid scale of 2 and 7 km, respectively). Here we present the results of matching a cirrus cloud to within 2–15 km, realized on 8 June 2010 over Payerne, Switzerland, and a location 120 km downstream close to Zurich. A thick cirrus cloud was detected over both measurement sites. We show that in order to quantitatively reproduce the measured particle backscatter ratios, the small-scale temperature fluctuations not resolved by COSMO must be superimposed on the trajectories. The stochastic nature of the fluctuations is captured by ensemble calculations. Possibilities for further improvements in the agreement with the measured backscatter data are investigated by assuming a very slow mass accommodation of water on ice, the presence of heterogeneous ice nuclei, or a wide span of (spheroidal) particle shapes. However, the resulting improvements from these microphysical refinements are moderate and comparable in magnitude with changes caused by assuming different regimes of temperature fluctuations for clear-sky or cloudy-sky conditions, highlighting the importance of proper treatment of subscale fluctuations. The model yields good agreement with the measured backscatter over both sites and reproduces the measured saturation ratios with respect to ice over Payerne. Conversely, the 30% in-cloud supersaturation measured in a massive 4 km thick cloud layer over Zurich cannot be reproduced, irrespective of the choice of meteorological or microphysical model parameters. The measured supersaturation can only be explained by either resorting to an unknown physical process, which prevents the ice particles from consuming the excess humidity, or – much more likely – by a measurement error, such as a contamination of the sensor housing of the SnowWhite hygrometer by a precipitation drop from a mixed-phase cloud just below the cirrus layer or from some very slight rain in the boundary layer. This uncertainty calls for in-flight checks or calibrations of hygrometers under the special humidity conditions in the upper troposphere.ISSN:1680-7375ISSN:1680-736

Overview paper: New insights into aerosol and climate in the Arctic

International audienceMotivated by the need to predict how the Arc-tic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an in-terdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Cana-dian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30-50 nm particle number density. DMS-oxidation-driven nucle-ation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface micro-layer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol-climate interactions under Arctic conditions. Aircraft-and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s −1)

New insights into aerosol and climate in the Arctic

Abstract. Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013 . (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water and the overlying atmosphere in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source. (2) Evidence was found of widespread particle nucleation and growth in the marine boundary layer in the CAA in the summertime. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from sea bird colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic material (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow