A single habit parameterization for the shortwave optical properties of cirrus is presented. The parameterization utilizes a hollow particle geometry, with stepped internal cavities as identified in laboratory and field studies. This particular habit was chosen as both experimental and theoretical results show that the particle exhibits lower asymmetry parameters when compared to solid crystals of the same aspect ratio. The aspect ratio of the particle was varied as a function of maximum dimension, D, in order to adhere to the same physical relationships assumed in the microphysical scheme in a configuration of the Met Office atmosphere-only global model, concerning particle mass, size and effective density. Single scattering properties were then computed using T-Matrix, Ray Tracing with Diffraction on Facets (RTDF) and Ray Tracing (RT) for small, medium, and large size parameters respectively. The scattering properties were integrated over 28 particle size distributions as used in the microphysical scheme. The fits were then parameterized as simple functions of Ice Water Content (IWC) for 6 shortwave bands. The parameterization was implemented into the GA6 configuration of the Met Office Unified Model along with the current operational long-wave parameterization. The GA6 configuration is used to simulate the annual twenty-year short-wave (SW) fluxes at top-of-atmosphere (TOA) and also the temperature and humidity structure of the atmosphere. The parameterization presented here is compared against the current operational model and a more recent habit mixture model.
Abstract. The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (droplets and ice particles) as well as interstitial (unactivated) aerosol particles; an interstitial inlet which collected only interstitial aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the condensed phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~5–10% in mixed-phase clouds with IMF>0.2. This can be explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.
Abstract. Large-scale subsidence, associated with high-pressure systems, is often imposed in large-eddy simulation (LES) models to maintain the height of boundary layer (BL) clouds. Previous studies have considered the influence of subsidence on warm liquid clouds in subtropical regions; however, the relationship between subsidence and mixed-phase cloud microphysics has not specifically been studied. For the first time, we investigate how widespread subsidence associated with synoptic-scale meteorological features can affect the microphysics of Arctic mixed-phase marine stratocumulus (Sc) clouds. Modelled with LES, four idealised scenarios – a stable Sc, varied droplet (Ndrop) or ice (Nice) number concentrations, and a warming surface (representing motion southwards) – were subjected to different levels of subsidence to investigate the cloud microphysical response. We find strong sensitivities to large-scale subsidence, indicating that high-pressure systems in the ocean-exposed Arctic regions have the potential to generate turbulence and changes in cloud microphysics in any resident BL mixed-phase clouds.Increased cloud convection is modelled with increased subsidence, driven by longwave radiative cooling at cloud top and rain evaporative cooling and latent heating from snow growth below cloud. Subsidence strengthens the BL temperature inversion, thus reducing entrainment and allowing the liquid- and ice-water paths (LWPs, IWPs) to increase. Through increased cloud-top radiative cooling and subsequent convective overturning, precipitation production is enhanced: rain particle number concentrations (Nrain), in-cloud rain mass production rates, and below-cloud evaporation rates increase with increased subsidence.Ice number concentrations (Nice) play an important role, as greater concentrations suppress the liquid phase; therefore, Nice acts to mediate the strength of turbulent overturning promoted by increased subsidence. With a warming surface, a lack of – or low – subsidence allows for rapid BL turbulent kinetic energy (TKE) coupling, leading to a heterogeneous cloud layer, cloud-top ascent, and cumuli formation below the Sc cloud. In these scenarios, higher levels of subsidence act to stabilise the Sc layer, where the combination of these two forcings counteract one another to produce a stable, yet dynamic, cloud layer.
Abstract In situ measurements associated with the passage of a kata cold front over the United Kingdom on 29 November 2011 are used to initialize a Lagrangian parcel model for the purpose of calculating rates of diabatic heating and cooling associated with the phase changes of water within the cloud system. The parcel model calculations are performed with both bin-resolved and bulk treatments of microphysical processes. The in situ data from this case study reveal droplet number concentrations up to 100 cm −3 , with planar ice crystals detected at cloud top, as well as columnar crystals produced by rime splinter ejection within the prefrontal warm sector. The results show that in terms of magnitude, the most significant rates of diabatic heating and cooling are produced by condensation growth of liquid water within the convective updrafts at the leading edge of the front. The peak temperature tendencies associated with condensation are typically found to be at least an order of magnitude larger than those associated with the ice phase, although the cooling effect from sublimation and melting occurs over a wide region. The parcel model framework is used in conjunction with the observations to assess the suitability of existing bulk microphysical treatments, of the kind used in operational weather forecast models. It is found that the assumption of spherical ice crystals (with diameters equal to the maximum dimension of those sampled), along with the use of negative exponential functions to describe ice particle size distributions, can lead to an overestimation of local diabatic heating and cooling rates by a factor of 2 or more.
Abstract. The composition of atmospheric aerosol particles has been found to influence their micro-physical properties and their interaction with water vapour in the atmosphere. Core-shell models have been used to investigate the relationship between composition, viscosity and equilibration time-scales. These models have traditionally relied on the Fickian laws of diffusion with no explicit account of non-ideal interactions. We introduce the Maxwell-Stefan diffusion framework as an alternative method, which explicitly accounts for non-ideal interactions through activity coefficients. E-folding time is the time it takes for the difference in surface and bulk concentration to change by an exponential factor and was used to investigate the interplay between viscosity and solubility and the effect this has on equilibration time-scales within individual aerosol particles. The e-folding time was estimated after instantaneous increases in relative humidity to binary systems of water and an organic component. At low water mole fractions, viscous effects were found to dominate mixing. However, at high water mole fractions, equilibration times were more sensitive to a range in solubility, shown through the greater variation in e-folding times. This is the first time the Maxwell-Stefan framework has been applied to an atmospheric aerosol core-shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition that requires further investigation.
Abstract. Cloud microphysical processes involving the ice phase in tropospheric clouds are among the major uncertainties in cloud formation, weather, and general circulation models. The detection of aerosol particles, liquid droplets, and ice crystals, especially in the small cloud particle-size range below 50 μm, remains challenging in mixed phase, often unstable environments. The Cloud Aerosol Spectrometer with Polarization (CASPOL) is an airborne instrument that has the ability to detect such small cloud particles and measure the variability in polarization state of their backscattered light. Here we operate the versatile Cosmics Leaving OUtdoor Droplets (CLOUD) chamber facility at the European Organization for Nuclear Research (CERN) to produce controlled mixed phase and other clouds by adiabatic expansions in an ultraclean environment, and use the CASPOL to discriminate between different aerosols, water, and ice particles. In this paper, optical property measurements of mixed-phase clouds and viscous secondary organic aerosol (SOA) are presented. We report observations of significant liquid–viscous SOA particle polarization transitions under dry conditions using CASPOL. Cluster analysis techniques were subsequently used to classify different types of particles according to their polarization ratios during phase transition. A classification map is presented for water droplets, organic aerosol (e.g., SOA and oxalic acid), crystalline substances such as ammonium sulfate, and volcanic ash. Finally, we discuss the benefits and limitations of this classification approach for atmospherically relevant concentrations and mixtures with respect to the CLOUD 8–9 campaigns and its potential contribution to tropical troposphere layer analysis.
Abstract. We present results of experiments at the aerosol interactions and dynamics in the atmosphere (AIDA) chamber facility looking at the freezing of water by three different types of mineral particles at temperatures between −12°C and −33°C. The three different dusts are Asia Dust-1 (AD1), Sahara Dust-2 (SD2) and Arizona test Dust (ATD). The dust samples used had particle concentrations of sizes that were log-normally distributed with mode diameters between 0.3 and 0.5 μm and standard deviations, σg, of 1.6–1.9. The results from the freezing experiments are consistent with the singular hypothesis of ice nucleation. The dusts showed different nucleation abilities, with ATD showing a rather sharp increase in ice-active surface site density at temperatures less than −24°C. AD1 was the next most efficient freezing nuclei and showed a more gradual increase in activity than the ATD sample. SD2 was the least active freezing nuclei. We used data taken with particle counting probes to derive the ice-active surface site density forming on the dust as a function of temperature for each of the three samples and polynomial curves are fitted to this data. The curve fits are then used independently within a bin microphysical model to simulate the ice formation rates from the experiments in order to test the validity of parameterising the data with smooth curves. Good agreement is found between the measurements and the model for AD1 and SD2; however, the curve for ATD does not yield results that agree well with the observations. The reason for this is that more experiments between −20 and −24°C are needed to quantify the rather sharp increase in ice-active surface site density on ATD in this temperature regime. The curves presented can be used as parameterisations in atmospheric cloud models where cooling rates of approximately 1°C min−1 or more are present to predict the concentration of ice crystals forming by the condensation-freezing mode of ice nucleation. Finally a polynomial is fitted to all three samples together in order to have a parameterisation describing the average ice-active surface site density vs. temperature for an equal mixture of the three dust samples.
Abstract. The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere). The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies). The organic carbon content (OC) of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI) to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2) to examine the mixing state of the BC containing ice residuals. Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content) where deposition freezing occurred at an ice saturation ratio Sice ~ 1.22 at a temperature T = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content) showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments) than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating. The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the onset of freezing occurred at colder temperatures and required a greater ice saturation ratio; for the medium and maximum OC flame soot, the addition of a sulphuric acid significantly reduced the freezing threshold.
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