The present work combines remote sensing observations and detailed cloud modeling to investigate two altocumulus cloud cases observed over Leipzig, Germany. A suite of remote sensing instruments was ...able to detect primary ice at rather high temperatures of -6 °C. For comparison, a second mixed phase case at about -25 °C is introduced. To further look into the details of cloud microphysical processes, a simple dynamics model of the Asai-Kasahara (AK) type is combined with detailed spectral microphysics (SPECS) forming the model system AK-SPECS. Vertical velocities are prescribed to force the dynamics, as well as main cloud features, to be close to the observations. Subsequently, sensitivity studies with respect to ice microphysical parameters are carried out with the aim to quantify the most important sensitivities for the cases investigated. For the cases selected, the liquid phase is mainly determined by the model dynamics (location and strength of vertical velocity), whereas the ice phase is much more sensitive to the microphysical parameters (ice nucleating particle (INP) number, ice particle shape). The choice of ice particle shape may induce large uncertainties that are on the same order as those for the temperature-dependent INP number distribution.
In model studies of aerosol‐dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. In contrast, the ...immersion freezing of larger drops—“rain”—is usually represented by a liquid volume‐dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop‐drop‐collisions. Here we introduce an extension to a two‐moment microphysical scheme in order to account explicitly for particle accumulation in raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust‐based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol‐dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.
Key Points
A parameterization scheme of aerosol‐dependent raindrop freezing is presented
Particle accumulation due to drop‐drop collisions is considered explicitly
Cloud glaciation with dust‐mediated freezing is less efficient than with Bigg's approach
This work presents a unique combination of aerosol, cloud microphysical, thermodynamic and turbulence variables to characterize supersaturation fluctuations in a turbulent marine stratocumulus (SC) ...layer. The analysis is based on observations with the helicopter-borne measurement platform ACTOS and a detailed cloud microphysical parcel model following three different approaches: (1) From the comparison of aerosol number size distributions inside and below the SC layer, the number of activated particles is calculated as 435±87 cm−3 and compares well with the observed median droplet number concentration of Nd = 464 cm−3. Furthermore, a 50% activation diameter of Dp50≈115 nm was derived, which was linked to a critical supersaturation Scrit of 0.16% via Köhler theory. From the shape of the fraction of activated particles, we estimated a standard deviation of supersaturation fluctuations of σS' = 0.09%. (2) These estimates are compared to more direct thermodynamic observations at cloud base. Therefore, supersaturation fluctuations (S') are calculated based on highly-resolved thermodynamic data showing a standard deviation of S' ranging within 0.1%≤σS'≤0.3 %. (3) The sensitivity of the supersaturation on observed vertical wind velocity fluctuations is investigated with the help of a detailed cloud microphysical model. These results show highest fluctuations of S' with σS'=0.1% at cloud base and a decreasing σS' with increasing liquid water content and droplet number concentration. All three approaches are independent of each other and vary only within a factor of about two.
Numerical simulations were performed to investigate the effects of drop freezing in immersion and contact modes for a convective situation. For the description of heterogeneous drop freezing, new ...approaches were used considering the significantly different ice nucleating efficiencies of various ice nuclei. An air parcel model with a sectional two‐dimensional description of the cloud microphysics was employed. Sensitivity studies were undertaken by varying the insoluble particle types as well as the soluble fraction of the aerosol particles showing the effects of these parameters on drop freezing and their possible impact on the vertical cloud dynamics. The soluble fraction ɛ decides whether immersion or contact freezing will be the major process. For high ɛ values, immersion freezing is the dominant process. In such cases the freezing process is strongly temperature‐dependent, and the ice nucleation efficiency of the insoluble particle types becomes important for efficient freezing. The freezing point depression can be neglected because of the preferential freezing of large drops. Contact freezing is the major process in cases of lower ɛ values. In these cases the freezing process is less dependent on temperature and aerosol particle type. For conditions of efficient freezing, cold, high‐altitude, completely glaciated clouds could form. The presented approaches for immersion and contact freezing can be incorporated further into mesoscale and global models to estimate the effects of specific ice nuclei on ice formation.
Clear experimental evidence of the Twomey effect for shallow trade wind cumuli near Barbados is presented. Effective droplet radius (reff) and cloud optical thickness (τ), retrieved from ...helicopter‐borne spectral cloud‐reflected radiance measurements, and spectral cloud reflectivity (γλ) are correlated with collocated in situ observations of the number concentration of aerosol particles from the subcloud layer (N). N denotes the concentration of particles larger than 80 nm in diameter and represents particles in the activation mode. In situ cloud microphysical and aerosol parameters were sampled by the Airborne Cloud Turbulence Observation System (ACTOS). Spectral cloud‐reflected radiance data were collected by the Spectral Modular Airborne Radiation measurement sysTem (SMART‐HELIOS). With increasing N a shift in the probability density functions of τ and γλ toward larger values is observed, while the mean values and observed ranges of retrieved reff decrease. The relative susceptibilities (RS) of reff, τ, and γλ to N are derived for bins of constant liquid water path. The resulting values of RS are in the range of 0.35 for reff and τ, and 0.27 for γλ. These results are close to the maximum susceptibility possible from theory. Overall, the shallow cumuli sampled near Barbados show characteristics of homogeneous, plane‐parallel clouds. Comparisons of RS derived from in situ measured reff and from a microphysical parcel model are in close agreement.
Key Points
Experimental evidence of Twomey effect
Susceptibility is quantified
Susceptibility of shallow cumuli shows characteristics of homogeneous clouds
The room-temperature phosphorescence behavior of erythrosine B (ER) and rose bengal (RB) in aerobic aqueous solution at pH 10 (10
−4
M NaOH) is investigated. The samples were excited with sliced ...second harmonic pulses of a Q-switched Nd:glass laser. A gated photomultiplier tube was used for instantaneous fluorescence signal discrimination and a digital oscilloscope was used for signal recording. For phosphorescence lifetime measurement the oscilloscope response time was adjusted to appropriate time resolution and sensitivity by the ohmic input resistance. In the case of phosphorescence quantum yield determination the gated photomultiplier – oscilloscope arrangement was operated in integration mode using 10
MΩ input resistance. Phosphorescence quantum yield calibration was achieved with erythrosine B and rose bengal doped starch films of known quantum yields. The determined phosphorescence lifetimes (quantum yields) of ER and RB in 0.1
mM NaOH are
τ
P
=1.92±0.1
μs (
ϕ
P=(1.5±0.3)×10
−5) and 2.40±0.1
μs ((5.7±0.9)×10
−5), respectively. The results are discussed in terms of triplet state deactivation by dissolved molecular oxygen.
► Phosphorescence lifetime of fluorone dyes in aerobe aqueous solution is measured. ► Phosphorescence quantum yield of fluorone dyes in aerobe solution is determined. ► Experimental setup with Q-switched laser and gated PMT detection is described. ► Phosphorescence quenching by dissolved molecular oxygen is analyzed. ► Absorption and fluorescence behavior of fluorones in aqueous solution is studied.
The novel model system LM-SPECS is presented combining a spectral bin microphysics scheme and the three-dimensional Lokalmodell (LM, today called COSMO) of the German Weather Service (“Deutscher ...Wetterdienst”). The model is designed to investigate in detail the interaction of atmospheric aerosol particles, clouds and precipitation. The microphysics scheme includes a combined spectrum of wetted aerosols, cloud droplets and rain drops. As a first application of the model, sensitivity studies on an artificial deep convective cloud were done. The results produced by LM-SPECS are satisfying. The studies show, e.g., that a diminished initial particle number leads to larger cloud droplets and thus to a higher efficiency of coalescence. This results in a larger amount of precipitation. Furthermore, studies on mixed phase clouds show the influence of varying ice nuclei, such as bacteria, kaolinite and soot, on cloud properties. Here, a more effective freezing leads to an increased number of ice particles with smaller radii. The results point to the importance of a detailed knowledge of the underlying microphysical processes in order to understand the formation of clouds and precipitation more accurately. Though to date the model was applied to artificial cases only, the use of the mesoscale weather model allows for more complex realistic cases which are subject to further studies.
Multiphase processes, such as the uptake of gases by clouds or the production of gas phase halogens from particulate halides are of increasing importance for the understanding of the tropospheric ...system. Mass transfer and chemical reactions modify the concentrations of stable compounds and oxidants in either phase. The parcel model SPACCIM is presented which combines a complex multiphase chemical model with a detailed microphysical model. For this purpose, a new coupling scheme is implemented. The description of both components is given for a fine-resolved particle/drop spectrum. The SPACCIM approach allows the coupling of multiphase chemical models with microphysical codes of various types. An efficient numerical solution of such systems is only possible utilizing the special structure. An implicit time-integration scheme with an adapted sparse solver for the linear systems is applied. Its numerical efficiency and robustness is analyzed for two scenarios and versions of different complexity of the multiphase chemistry mechanism CAPRAM. The sensitivity of simulation results against variations in the particle/droplet size resolution, the coupling time step and numerical control parameters is discussed. Guidelines for an “optimal” choice of control parameters are derived from this sensitivity study. The coupling scheme operation is always robust and reliable. Model simulations are compared with several measurements from the FEBUKO field campaign. Simulated and measured results show a reasonable agreement.
There is some evidence that the initiation of warm rain is suppressed in clouds over regions with vegetation fires. Thus, the ice phase becomes important as another possibility to initiate ...precipitation. Numerical simulations were performed to investigate heterogeneous drop freezing for a biomass-burning situation. An air parcel model with a sectional two-dimensional description of the cloud microphysics was employed with parameterizations for immersion and contact freezing which consider the different ice nucleating efficiencies of various ice nuclei. Three scenarios were simulated resulting to mixed-phase or completely glaciated clouds. According to the high insoluble fraction of the biomass-burning particles drop freezing via immersion and contact modes was very efficient. The preferential freezing of large drops followed by riming (i.e. the deposition of liquid drops on ice particles) and the evaporation of the liquid drops (Bergeron–Findeisen process) caused a further decrease of the liquid drops’ effective radius in higher altitudes. In turn ice particle sizes increased so that they could serve as germs for graupel or hailstone formation. The effects of ice initiation on the vertical cloud dynamics were fairly significant leading to a development of the cloud to much higher altitudes than in a warm cloud without ice formation.
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