Indirect And Semi-Direct Aerosol Campaign Research Articles

Combined Effect of the Wegener–Bergeron–Findeisen Mechanism and Large Eddies on Microphysics of Mixed-Phase Stratiform Clouds

Abstract The process of glaciation in mixed-phase stratiform clouds was investigated by a novel Lagrangian–Eulerian model (LEM) in which thousands of adjoining Lagrangian parcels moved within a turbulent-like velocity field with statistical parameters typical of the Arctic boundary layer. We used detailed bin microphysics to describe the condensation/evaporation processes in each parcel, in which droplets, aerosols, and ice particles were described using size distributions of 500 mass bins. The model also calculated aerosol mass inside droplets and ice particles. Gravitational sedimentation of droplets and ice particles was also accounted for. Assuming that droplet freezing is the primary source of ice particles, the Arctic clouds observed in Indirect and Semi-Direct Aerosol Campaign (ISDAC) were successfully simulated. The model showed that at a low ice particle concentration typical of ISDAC, large vortices (eddies) led to a quasi-stationary regime, in which mixed-phase St existed for a long time. The large eddies controlled the water partitioning in the mixed-phase clouds. Droplets formed and grew in updrafts, typically reaching the cloud top, and evaporated in downdrafts. Ice particles grew in updrafts and downdrafts. The Wegener–Bergeron–Findeisen (WBF) mechanism was efficient in downdrafts and some parts of updrafts, depending on ice concentration and vertical velocity. At low ice concentrations, the effect of ice on the phase partitioning was negligible. In this regime, liquid droplets were found near the cloud top, whereas ice particles precipitated through the cloud base. When ice concentration exceeded about 10 L−1, the WBF mechanism led to glaciation of almost the entire cloud, with the exception of narrow cloud regions associated with strong updrafts. At ice particle concentrations of a few tens per liter, the oscillatory regime took place due to the ice–liquid interaction. The microphysical structure of mixed-phase St forms as a combined effect of cloud dynamics (large eddies) and the WBF mechanism.

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

Abstract. In 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.

Simulating Arctic Ice Clouds during Spring Using an Advanced Ice Cloud Microphysics in the WRF Model

Two Types of Ice Clouds (TICs) have been characterized in the Arctic during the polar night and early spring. TIC-1 are composed by non-precipitating small ice crystals of less than 30 µm in diameter. The second type, TIC-2, are characterized by a low concentration of large precipitating ice crystals (>30 µm). Here, we evaluate the Weather Research and Forecasting (WRF) model performance both in space and time after implementing a parameterization based on a stochastic approach dedicated to the simulation of ice clouds in the Arctic. Well documented reference cases provided us in situ data from the spring of 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) campaign over Alaska. Simulations of the microphysical properties of the TIC-2 clouds on 15 and 25 April 2008 (polluted or acidic cases) and TIC-1 clouds on non-polluted cases are compared to DARDAR (raDAR/liDAR) satellite products. Our results show that the stochastic approach based on the classical nucleation theory, with the appropriate contact angle, is better than the original scheme in WRF model to represent TIC-1 and TIC-2 properties (ice crystal concentration and size) in response to the IN acidification.

Potential of Higher-Order Moments and Slopes of the Radar Doppler Spectrum for Retrieving Microphysical and Kinematic Properties of Arctic Ice Clouds

AbstractRetrievals of ice-cloud properties from cloud-radar observations are challenging because the retrieval methods are typically underdetermined. Here, the authors investigate whether additional information can be obtained from higher-order moments and the slopes of the radar Doppler spectrum such as skewness and kurtosis as well as the slopes of the Doppler peak. To estimate quantitatively the additional information content, a generalized Bayesian retrieval framework that is based on optimal estimation is developed. Real and synthetic cloud-radar observations of the Indirect and Semi-Direct Aerosol Campaign (ISDAC) dataset obtained around Barrow, Alaska, are used in this study. The state vector consists of the microphysical (particle-size distribution, mass–size relation, and cross section–area relation) and kinematic (vertical wind and turbulence) quantities required to forward model the moments and slopes of the radar Doppler spectrum. It is found that, for a single radar frequency, more information can be retrieved when including higher-order moments and slopes than when using only reflectivity and mean Doppler velocity but two radar frequencies. When using all moments and slopes with two or even three frequencies, the uncertainties of all state variables, including the mass–size relation, can be considerably reduced with respect to the prior knowledge.

Importance of Chemical Composition of Ice Nuclei on the Formation of Arctic Ice Clouds

Ice clouds play an important role in the Arctic weather and climate system but interactions between aerosols, clouds and radiation remain poorly understood. Consequently, it is essential to fully understand their properties and especially their formation process. Extensive measurements from ground-based sites and satellite remote sensing reveal the existence of two Types of Ice Clouds (TICs) in the Arctic during the polar night and early spring. TICs-1 are composed by non-precipitating small (radar-unseen) ice crystals of less than 30 μm in diameter. The second type, TICs-2, are detected by radar and are characterized by a low concentration of large precipitating ice crystals ice crystals (>30 μm). To explain these differences, we hypothesized that TIC-2 formation is linked to the acidification of aerosols, which inhibits the ice nucleating properties of ice nuclei (IN). As a result, the IN concentration is reduced in these regions, resulting to a lower concentration of larger ice crystals. Water vapor available for deposition being the same, these crystals reach a larger size. Current weather and climate models cannot simulate these different types of ice clouds. This problem is partly due to the parameterizations implemented for ice nucleation. Over the past 10 years, several parameterizations of homogeneous and heterogeneous ice nucleation on IN of different chemical compositions have been developed. These parameterizations are based on two approaches: stochastic (that is nucleation is a probabilistic process, which is time dependent) and singular (that is nucleation occurs at fixed conditions of temperature and humidity and time-independent). The best approach remains unclear. This research aims to better understand the formation process of Arctic TICs using recently developed ice nucleation parameterizations. For this purpose, we have implemented these ice nucleation parameterizations into the Limited Area version of the Global Multiscale Environmental Model (GEM-LAM) and use them to simulate ice clouds observed during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in Alaska. Simulation results of the TICs-2 observed on April 15th and 25th (acidic cases) and TICs-1 observed on April 5th (non-acidic cases) are presented. Our results show that the stochastic approach based on the classical nucleation theory with the appropriate contact angle is better. Parameterizations of ice nucleation based on the singular approach tend to overestimate the ice crystal concentration in TICs-1 and TICs-2. The classical nucleation theory using the appropriate contact angle is the best approach to use to simulate the ice clouds investigated in this research.

Sensitivities in Large-Eddy Simulations of Mixed-Phase Arctic Stratocumulus Clouds Using a Simple Microphysics Approach*

Abstract Arctic mixed-phase stratocumulus clouds are maintained by feedbacks between microphysical and dynamical phenomena, but the details of these interactions are incompletely understood. Although large-eddy simulations are a promising means of elucidating microphysics–turbulence relationships, the use of sophisticated microphysical schemes complicates analysis of their results. Here, the ability of a simplified one-moment scheme to capture basic features of this cloud type is investigated through simulations based on Mixed-Phase Arctic Cloud Experiment (MPACE), SHEBA/FIRE-ACE, and Indirect and Semi-Direct Aerosol Campaign (ISDAC) intercomparison studies. The results of the simple scheme show reasonable agreement with liquid and ice water path predictions reported by models using schemes of similar or greater complexity. Additional tests are performed to evaluate the sensitivity of the results to three main parameters of the scheme: the snow and ice size distribution intercept parameters and the exponent appearing in the temperature-dependent phase-partition function, which is used to diagnose cloud condensate amounts. Sensitivities of the SHEBA and ISDAC cases, both of which have low surface heat fluxes and low precipitation rates, tend to be similar, while the MPACE case, with higher surface fluxes and precipitation rates, shows somewhat different trends. Results of all three cases are found to be sensitive to the snow size distribution intercept parameter, but this quantity can be adequately estimated using a recently developed diagnostic expression based on observations of Arctic clouds.

Large‐eddy simulation of three mixed‐phase cloud events during ISDAC: Conditions for persistent heterogeneous ice formation

AbstractA Classical‐Nucleation‐Theory‐based parameterization for heterogenous ice nucleation, including explicit dependencies of the nucleation rates on the number concentration, size, and composition of the ambient aerosol population, is implemented in a cloud‐scale, large‐eddy simulation model and evaluated against Arctic mixed‐phase cloud events observed during Indirect and Semi‐Direct Aerosol Campaign (ISDAC). An important feature of the parameterization is that the ice nucleation efficiency of each considered aerosol type is described using a contact angle distribution which evolves with time so that the model accounts for the inhibition of ice nucleation as the most efficient ice‐forming particles are nucleated and scavenged. The model gives a reasonable representation of first‐order (ice water paths) and second‐order (ice crystal size distributions) ice microphysical properties. The production of new ice crystals in the upper part of the cloud, essential to guarantee sustained mixed‐phase conditions, is found to be controlled mostly by the competition between radiative cooling (resulting in more aerosol particles becoming efficient ice nuclei as the temperature decreases), cloud‐top entrainment (entraining fresh particles into the cloud), and nucleation scavenging of the ice+forming aerosol particles. The relative contribution of each process is mostly determined by the cloud‐top temperature and the entrainment rates. Accounting for the evolution of the contact angle probability density function with time seems to be essential to capture the persistence of in‐cloud ice production without having to, for example, increase the free tropospheric aerosol concentration. Although limited to only three cases and despite important limitations of the parameterization (e.g., the present version only considers dust and black carbon as potential ice nuclei), the results suggest that modeling the time evolution of the ice nuclei population ability to form ice is required to accurately model Arctic mixed‐phase cloud processes.

Developing and Evaluating Ice Cloud Parameterizations for Forward Modeling of Radar Moments Using in situ Aircraft Observations

AbstractObserving ice clouds using zenith pointing millimeter cloud radars is challenging because the transfer functions relating the observables to meteorological quantities are not uniquely defined. Here, the authors use a spectral radar simulator to develop a consistent dataset containing particle mass, area, and size distribution as functions of size. This is an essential prerequisite for radar sensitivity studies and retrieval development. The data are obtained from aircraft in situ and ground-based radar observations during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) campaign in Alaska. The two main results of this study are as follows: 1) An improved method to estimate the particle mass–size relation as a function of temperature is developed and successfully evaluated by combining aircraft in situ and radar observations. The method relies on a functional relation between reflectivity and Doppler velocity. 2) The impact on the Doppler spectrum by replacing measurements of particle area and size distribution by recent analytical expressions is investigated. For this, higher-order moments such as skewness and kurtosis as well as the slopes of the Doppler spectrum are also used as a proxy for the Doppler spectrum. For the area–size relation, it is found that a power law is not sufficient to describe particle area and small deviations from a power law are essential for obtaining consistent higher moments. For particle size distributions, the normalization approach for the gamma distribution of Testud et al., adapted to maximum diameter as size descriptor, is preferred.

Dimensions and aspect ratios of natural ice crystals

Abstract. During the 2006 Tropical Warm Pool International Cloud Experiment (TWP-ICE) in the tropics, the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) in the Arctic, and the 2010 Small PARTicles In CirrUS (SPARTICUS) campaign at mid-latitudes, high-resolution images of ice crystals were recorded by a Cloud Particle Imager at temperatures (T) between −87 and 0 °C. The projected maximum dimension (D'), length (L'), and width (W') of pristine columns, plates, and component bullets of bullet rosettes were measured using newly developed software, the Ice Crystal Ruler. The number of bullets in each bullet rosette was also measured. Column crystals were further distinguished as either horizontally oriented columns or columns with other orientations to eliminate any orientation effect on the measured dimensions. The dimensions and aspect ratios (AR, the dimension of the major axis divided by the dimension of the minor axis) of crystals were determined as functions of temperature, geophysical location, and type of cirrus. Dimensions of crystals generally increased with temperature. Columns and bullets had larger dimensions (i.e., W') of the minor axis (i.e., a axis) for a given dimension (i.e., D' orL') of the major axis (i.e., c axis), and thus smaller AR, as T increased, whereas this trend did not occur for plate crystals. The average number of branches in bullet rosettes was 5.50 ± 1.35 during three campaigns and 6.32 ± 1.34 (5.46 ± 1.34; 4.95 ± 1.01) during TWP-ICE (SPARTICUS; ISDAC). The AR of bullets increased with the number of branches in bullet rosettes. Most dimensions of crystals and ARs of columnar crystals measured during SPARTICUS were larger than those measured during TWP-ICE and ISDAC at −67 < T < -35 °C and at −40 < T < −15 °C, respectively. The relative occurrence of varying pristine habits depended strongly on cirrus type (i.e., anvil or non-anvil clouds), with plates especially occurring more frequently in anvils. The L–W relationships of columns derived using current data exhibited a strong dependence on temperature; similar relationships determined in previous studies were within the range of the current data.

The Characterization of Ice Hydrometeor Gamma Size Distributions as Volumes in N0–λ–μ Phase Space: Implications for Microphysical Process Modeling

Abstract Gamma distributions represent particle size distributions (SDs) in mesoscale and cloud-resolving models that predict one, two, or three moments of hydrometeor species. They are characterized by intercept (N0), slope (λ), and shape (μ) parameters prognosed by such schemes or diagnosed based on fits to SDs measured in situ in clouds. Here, ice crystal SDs acquired in arctic cirrus during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) and in hurricanes during the National Aeronautic and Space Administration (NASA) African Monsoon Multidisciplinary Analyses (NAMMA) are fit to gamma distributions using multiple algorithms. It is shown that N0, λ, and μ are not independent parameters but rather exhibit mutual dependence. Although N0, λ, and μ are not highly dependent on choice of fitting routine, they are sensitive to the tolerance permitted by fitting algorithms, meaning a three-dimensional volume in N0–λ–μ phase space is required to represent a single SD. Depending on the uncertainty in the measured SD and on how well a gamma distribution matches the SD, parameters within this volume of equally realizable solutions can vary substantially, with N0, in particular, spanning several orders of magnitude. A method to characterize a family of SDs as an ellipsoid in N0–λ–μ phase space is described, with the associated scatter in N0–λ–μ for such families comparable to scatter in N0, λ, and μ observed in prior field campaigns conducted in different conditions. Ramifications for the development of cloud parameterization schemes and associated calculations of microphysical process rates are discussed.

An Assessment of the Impact of Antishattering Tips and Artifact Removal Techniques on Cloud Ice Size Distributions Measured by the 2D Cloud Probe

AbstractPrior estimates of ice crystal size distributions derived from 2D cloud probes (2DCs) have been artificially amplified by small ice crystals generated from the shattering of large ice crystals on the probe tips. Although antishatter tips and algorithms exist, there is considerable uncertainty in their effectiveness. This paper examines differences in ice crystal size distributions from adjacent 2DCs with standard and antishatter tips, and processed with and without antishattering algorithms. The measurements were obtained from the National Research Council of Canada Convair-580 during the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) and the National Center for Atmospheric Research C-130 during the 2011 Instrumentation Development and Education in Airborne Science (IDEAS-2011). The 2DC size distributions are compared with those from the Holographic Detector for Clouds (HOLODEC), which has antishatter tips and allows for identification of shattering through spatial statistics.The ratio of the number concentration N of particles with maximum dimensions 125–500 μm from the 2DC with standard tips to that from the 2DC with modified tips was correlated with median mass diameter and perimeter divided by area, but not with airspeed, attack, and attitude angles. Antishatter tips and algorithms reduced N by up to a factor of 10 for IDEAS-2011 and ISDAC, but neither alone removed all artifacts. For the period with coincident data, both N from the HOLODEC and 2DC with modified tips are around 5 × 10−3 L−1 μm−1, suggesting that antishatter tips and algorithms combined remove artifacts from the 2DC for the conditions sampled during IDEAS-2011.

An Assessment of the Impact of Antishattering Tips and Artifact Removal Techniques on Bulk Cloud Ice Microphysical and Optical Properties Measured by the 2D Cloud Probe

Abstract A recent study showed that the ratio of the number of distribution functions derived from 2D cloud probes (2DCs) with standard tips to those with antishatter tips used during the 2008 Indirect and Semidirect Aerosol Campaign (ISDAC) and Instrumentation Development and Education in Airborne Science 2011 (IDEAS-2011) was greater than 1 for ice crystals with maximum dimension D < 500 μm. To assess the applicability of 2DC data obtained without antishatter tips previously used in parameterization schemes for numerical models and remote sensing retrievals, the impacts of artifacts on bulk microphysical and scattering properties were examined by quantifying differences between such properties derived from 2DCs with standard and antishatter tips, and with and without the use of shatter detection algorithms using the ISDAC and IDEAS-2011 data. Using either modified tips or algorithms changed the quantities dominated by higher-order moments, such as ice water content, bulk extinction, effective radius, mass-weighted terminal velocity, median mass diameter, asymmetry parameter, and single-scatter albedo, at wavenumbers from 5 to 100 cm−1 and wavelengths of 0.5–5 μm by less than 20%. This is significantly less than the fractional changes quantities dominated by lower-order moments, such as number concentration. The results suggest that model parameterizations and remote sensing techniques based on higher-order moments of ice particle size distributions obtained in conditions similar to those sampled during IDEAS-2011 and ISDAC derived from 2DCs are not substantially biased by shattered remnants.

Optical, physical, and chemical properties of springtime aerosol over Barrow Alaska in 2008

Airborne observations from four flights during the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) are used to examine some cloud-free optical, physical, and chemical properties of aerosol particles in the springtime Arctic troposphere. The number concentrations of particles larger than 0.12 µm (Na>120), important for light extinction and cloud droplet formation, ranged from 15 to 2260 cm−3, with the higher Na>120 cases dominated by measurements from two flights of long-range transported biomass burning (BB) aerosols. The two other flights examined here document a relatively clean aerosol and an Arctic Haze aerosol impacted by larger particles largely composed of dust. For observations from the cleaner case and the BB cases, the particle light scattering coefficients at low relative humidity (RH<20%) increased nonlinearly with increasing Na>120, driven mostly by an increase in mean sizes of particles with increasing Na>120 (BB cases). For those three cases, particle light absorption coefficients also increased nonlinearly with increasing Na>120 and linearly with increasing submicron particle volume concentration. In addition to black carbon, brown carbon was estimated to have increased light absorption coefficients by 27% (450 nm wavelength) and 14% (550 nm) in the BB cases. For the case with strong dust influence, the absorption relative to submicron particle volume was small compared with the other cases. There was a slight gradient of Passive Cavity Aerosol Spectrometer Probe (PCASP) mean volume diameter (MVD) towards smaller sizes with increasing height, which suggests more scavenging of the more elevated particles, consistent with a typically longer lifetime of particles higher in the atmosphere. However, in approximately 10% of the cases, the MVD increased (>0.4 µm) with increasing altitude, suggesting transport of larger fine particle mass (possibly coarse particle mass) at high levels over the Arctic. This may be because of transport of larger particles at higher elevations and relatively slow deposition to the surface.

Intercomparison of large‐eddy simulations of Arctic mixed‐phase clouds: Importance of ice size distribution assumptions

AbstractLarge‐eddy simulations of mixed‐phase Arctic clouds by 11 different models are analyzed with the goal of improving understanding and model representation of processes controlling the evolution of these clouds. In a case based on observations from the Indirect and Semi‐Direct Aerosol Campaign (ISDAC), it is found that ice number concentration, Ni, exerts significant influence on the cloud structure. Increasing Ni leads to a substantial reduction in liquid water path (LWP), in agreement with earlier studies. In contrast to previous intercomparison studies, all models here use the same ice particle properties (i.e., mass‐size, mass‐fall speed, and mass‐capacitance relationships) and a common radiation parameterization. The constrained setup exposes the importance of ice particle size distributions (PSDs) in influencing cloud evolution. A clear separation in LWP and IWP predicted by models with bin and bulk microphysical treatments is documented and attributed primarily to the assumed shape of ice PSD used in bulk schemes. Compared to the bin schemes that explicitly predict the PSD, schemes assuming exponential ice PSD underestimate ice growth by vapor deposition and overestimate mass‐weighted fall speed leading to an underprediction of IWP by a factor of two in the considered case. Sensitivity tests indicate LWP and IWP are much closer to the bin model simulations when a modified shape factor which is similar to that predicted by bin model simulation is used in bulk scheme. These results demonstrate the importance of representation of ice PSD in determining the partitioning of liquid and ice and the longevity of mixed‐phase clouds.

On the relationship between Arctic ice clouds and polluted air masses over the North Slope of Alaska in April 2008

Abstract. Recently, two types of ice clouds (TICs) properties have been characterized using the Indirect and Semi-Direct Aerosol Campaign (ISDAC) airborne measurements (Alaska, April 2008). TIC-2B were characterized by fewer (&lt; 10 L−1) and larger (&gt; 110 μm) ice crystals, and a larger ice supersaturation (&gt; 15%) compared to TIC-1/2A. It has been hypothesized that emissions of SO2 may reduce the ice nucleating properties of ice nuclei (IN) through acidification, resulting in a smaller concentration of larger ice crystals and leading to precipitation (e.g., cloud regime TIC-2B). Here, the origin of air masses forming the ISDAC TIC-1/2A (1 April 2008) and TIC-2B (15 April 2008) is investigated using trajectory tools and satellite data. Results show that the synoptic conditions favor air masses transport from three potential SO2 emission sources into Alaska: eastern China and Siberia where anthropogenic and biomass burning emissions, respectively, are produced, and the volcanic region of the Kamchatka/Aleutians. Weather conditions allow the accumulation of pollutants from eastern China and Siberia over Alaska, most probably with the contribution of acidic volcanic aerosol during the TIC-2B period. Observation Monitoring Instrument (OMI) satellite observations reveal that SO2 concentrations in air masses forming the TIC-2B were larger than in air masses forming the TIC-1/2A. Airborne measurements show high acidity near the TIC-2B flight where humidity was low. These results support the hypothesis that acidic coating on IN could be at the origin of the formation of TIC-2B.

Chemical characterization of individual particles and residuals of cloud droplets and ice crystals collected on board research aircraft in the ISDAC 2008 study

Ambient particles and the dry residuals of mixed‐phase cloud droplets and ice crystals were collected during the Indirect and Semi‐Direct Aerosol Campaign (ISDAC) near Barrow, Alaska, in spring of 2008. The collected particles were analyzed using Computer Controlled Scanning Electron Microscopy with Energy Dispersive X‐ray analysis and Scanning Transmission X‐ray Microscopy coupled with Near Edge X‐ray Absorption Fine Structure spectroscopy to identify physico‐chemical properties that differentiate cloud‐nucleating particles from the total aerosol population. A wide range of individually mixed components was identified in the ambient particles and residuals including organic carbon compounds, inorganics, carbonates, and black carbon. Our results show that cloud droplet residuals differ from the ambient particles in both size and composition, suggesting that both properties may impact the cloud‐nucleating ability of aerosols in mixed‐phase clouds. The percentage of residual particles which contained carbonates (47%) was almost four times higher than those in ambient samples. Residual populations were also enhanced in sea salt and black carbon and reduced in organic compounds relative to the ambient particles. Further, our measurements suggest that chemical processing of aerosols may improve their cloud‐nucleating ability. Comparison of results for various time periods within ISDAC suggests that the number and composition of cloud‐nucleating particles over Alaska can be influenced by episodic events bringing aerosols from both the local vicinity and as far away as Siberia.

Small Cloud Particle Shapes in Mixed-Phase Clouds

AbstractThe shapes of cloud particles with maximum dimensions Dmax between 35 and 60 μm in mixed-phase clouds were studied using high-resolution particle images collected by a cloud particle imager (CPI) during the Mixed-Phase Arctic Cloud Experiment (M-PACE) and the Indirect and Semi-Direct Aerosol Campaign (ISDAC). The area ratio α, the projected area of a particle divided by the area of a circle with diameter Dmax, quantified particle shape. The differing optical characteristics of CPIs used in M-PACE and ISDAC had no effect on derived α provided that Dmax &gt; 35 μm and CPI focus &gt; 45. The fraction of particles with 35 &lt; Dmax &lt; 60 μm with α &gt; 0.8 increased with the ratio of liquid water content (LWC) to total water content (TWC). The average αmean of small particles in each 10-s interval in mixed-phase clouds was correlated with LWC/TWC with a correlation coefficient of 0.60 for M-PACE and 0.43 for ISDAC. The stronger correlation seen during M-PACE was most likely associated with the presence of more liquid droplets that were larger than the CPI detection threshold contributing to αmean; the modal effective radius was larger (11 vs 6 μm), and drops with D &gt; 35 μm had concentrations during M-PACE that were 6 times as large as those of ISDAC. This study hence suggests that area ratio can be used to identify the phase of particles with 35 &lt; Dmax &lt; 60 μm and questions the assumption used in previous studies that all particles in this size range are supercooled droplets.

Characterization of Arctic ice cloud properties observed during ISDAC

Extensive measurements from ground‐based sites and satellite remote sensing (CloudSat and CALIPSO) reveal the existence of two types of ice clouds (TICs) in the Arctic during the polar night and early spring. The first type (TIC‐2A), being topped by a cover of nonprecipitating very small (radar unseen) ice crystals (TIC‐1), is found more frequently in pristine environment, whereas the second type (TIC‐2B), detected by both sensors, is associated preferentially with a high concentration of aerosols. To further investigate the microphysical properties of TIC‐1/2A and TIC‐2B, airborne in situ and satellite measurements of specific cases observed during Indirect and Semi‐Direct Aerosol Campaign (ISDAC) have been analyzed. For the first time, Arctic TIC‐1/2A and TIC‐2B microstructures are compared using in situ cloud observations. Results show that the differences between them are confined in the upper part of the clouds where ice nucleation occurs. TIC‐2B clouds are characterized by fewer (by more than 1 order of magnitude) and larger (by a factor of 2 to 3) ice crystals and a larger ice supersaturation (of 15–20%) compared to TIC‐1/2A. Ice crystal growth in TIC‐2B clouds seems explosive, whereas it seems more gradual in TIC‐1/2A. It is hypothesized that these differences are linked to the number concentration and the chemical composition of aerosols. The ice crystal growth rate in very cold conditions impinges on the precipitation efficiency, dehydration and radiation balance. These results represent an essential and important first step to relate previous modeling, remote sensing and laboratory studies with TICs cloud in situ observations.

The dependence of ice microphysics on aerosol concentration in arctic mixed‐phase stratus clouds during ISDAC and M‐PACE

Cloud and aerosol data acquired by the National Research Council of Canada (NRC) Convair‐580 aircraft in, above, and below single‐layer arctic stratocumulus cloud during the Indirect and Semi‐Direct Aerosol Campaign (ISDAC) in April 2008 were used to test three aerosol indirect effects hypothesized to act in mixed‐phase clouds: the riming indirect effect, the glaciation indirect effect, and the thermodynamic indirect effect. The data showed a correlation of R = 0.78 between liquid drop number concentration, Nliq inside cloud and ambient aerosol number concentration NPCASP below cloud. This, combined with increasing liquid water content LWC with height above cloud base and the nearly constant vertical profile of Nliq, suggested that liquid drops nucleated from aerosol at cloud base. No evidence of a riming indirect effect was observed, but a strong correlation of R = 0.69 between ice crystal number concentration Ni and NPCASP above cloud was noted. Increases in ice nuclei (IN) concentration with NPCASP above cloud for 2 flight dates combined with the subadiabatic LWC profiles suggest possible mixing of IN from cloud top consistent with the glaciation indirect effect. The lower Nice and lower effective radius rel for the more polluted ISDAC cases compared to data collected in cleaner single‐layer stratocumulus conditions during the Mixed‐Phase Arctic Cloud Experiment is consistent with the operation of the thermodynamic indirect effect. However, more data in a wider variety of meteorological and surface conditions, with greater variations in aerosol forcing, are required to identify the dominant aerosol forcing mechanisms in mixed‐phase arctic clouds.

Spatial and temporal variability of aerosol particles in Arctic spring

AbstractThe objective of this work is to investigate the variability in the aerosol particle number concentration in Arctic spring. The Indirect and Semi‐Direct Aerosol Campaign (ISDAC) was conducted during April 2008 in the vicinities of Fairbanks and Barrow, Alaska. Aircraft‐based measurements of total aerosol particle number concentration (Na) in the size range of 0.12–3 µm diameter were obtained using a passive cavity aerosol spectrometer probe (PCASP‐100X). The analysis considers Na during cloud‐free periods in biomass burning (BB) and non‐BB aerosol loading scenarios, the latter including background cases and cases with elevated concentration in layers. The BB cases had air masses originating mainly from Russian and Asian forest and crop fires, whereas the non‐BB cases originated predominantly from Arctic or oceanic regions. The average Na for all non‐BB cases was 127 cm−3, while that for all BB cases was Na = 720 cm−3. These estimates do not, however, capture the details of aerosol particle layers encountered during most flights. Variability in Na was considered for constant altitude (horizontal) flight legs ranging from 50 to 650 km in length, as well as for vertical flight profiles up to 7 km above sea level. When aerosol particle layers were encountered, Na rapidly increased from 20 to 550 cm−3, and reached up to 2200 cm−3 within air masses dominated by BB plumes. The observed variability in Na may have important implications for estimating cloud microphysical properties as well as estimates of particle properties used in global climate model simulations, because averaging over large space‐ or time‐scales may not represent real atmospheric conditions. The analysis demonstrates the difficulty in interpreting average aerosol particle characteristics along longer flight legs, particularly during cases with higher particle loading that varies over shorter distance scales and time periods. Copyright © 2012 Royal Meteorological Society and Crown in the right of Canada.