Mechanisms for the Influence from Ice Nucleus Aerosols on Clouds and their Indirect Effects: Cloud Modelling

The role of multiple groups of primary biological aerosol particles (PBAPs) as ice nucleating particles (INPs), and of ice formation processes such as time-dependent freezing of various INPs, and various secondary ice production(SIP) mechanisms in overall ice concentration has been evaluated in a range of cloud systems by simulating them numerically with the state-of-the-art ‘Aerosol-Cloud’ (AC) model in a 3D mesoscale domain. Also, the mechanismsof aerosol indirect effects (AIEs) arising from anthropogenic INPs, and the responses to these AIEs from time-dependent INP freezing and SIP processes are investigated in the simulated clouds. The cloud systems simulated with AC are: events of summertime deep convection observed over Oklahoma, USA during the Midlatitude Continental Convective Cloud Experiment (MC3E) in 2011 on 1) 11 May, and 2) 20 May, and wintertime 3) orographic clouds observed during the Atmospheric Radiation Measurement Cloud Aerosol Precipitation Experiment (ACAPEX) on 07 February 2015 over North California, and 4) supercooled layer clouds observed over Larkhill, UK, during the Aerosol Properties, Processes And Influences on the Earth’s climate (APPRAISE) campaign on 18 February 2009.AC uses the dynamical core of the Weather Research and Forecasting (WRF) model, modified Geophysical Fluid Dynamic Laboratory (GFDL) radiation scheme, and hybrid bin-bulk microphysics scheme. AC is validated adequately with the coincident aircraft, ground-based, and satellite observations for all four cases. AC forms secondary ice through the Hallett-Mossop (HM) process of rime-splintering, and fragmentation during ice-ice collisions, raindrop freezing, and sublimation of dendritic snow and graupel. A measure of SIP is defined using theterm ‘ice enhancement’ (IE) ratio which is the ratio between the number concentration of total ice particles and active INPs at cloud tops. For both cases in MC3E, overall, PBAPs have little effect (+1-6%) on the cloud-liquid (droplet mean sizes, number concentrations, and their water contents) properties, overall ice concentration, and on precipitation. AC predicts the activity of various INPs with an empirical parameterization (EP). The EP is modified to represent the time-dependent approach of INP freezing in light of our published laboratory observations. It is predicted that the time dependence of INP freezing is not the main cause for continuous ice nucleation and precipitation in all simulated cases. Rather, the main mechanism of precipitation formation is the combination of various SIP mechanisms (in convection) and recirculation-reactivation of dust particles (in APPRAISE layer cloud episode). Also, for all cases, the inclusion oftime dependence of INP freezing causes little increase (about 10-20%) in the total ice concentration and ice from all SIP.Regarding SIP, in young developing convective clouds of MC3E (11 May), with tops > −15oC, the initial explosive growth is from the fast HM process, creating IE ratios as high as 103. By contrast, in mature convective clouds (tops < −20oC), fragmentation in ice-ice collisions prevails, creating IE ratios of up to about 102-103. Regarding AIEs from INPs, increasing anthropogenic pollution is predicted to exert a net cooling in APPRAISE, and a strong net warmingin MC3E (11 May). Furthermore, these net AIEs are mainly from glaciated clouds. Overall, the contribution to the AIEs from ice formation processes, such as time-dependent INP freezing and SIP, shows a high sensitivity with respect to anthropogenic INPs (about 20-60% increase in net AIEs). Also, two new indirect effects associated with ice initiation mechanisms are proposed here. These are, 1) the ‘SIP’ indirect effect, and 2) the ‘time-dependent INP’ indirect effect. It is predicted that in APPRAISE and MC3E, both SIP and time-dependent INP indirect effects form less than 30%, and more than 50% of the net AIE, respectively

Effects from Time Dependence of Ice Nucleus Activity for Contrasting Cloud Types

The role of time-dependent freezing of ice nucleating particles (INPs) is evaluated with the “Aerosol–Cloud” (AC) model in 1) deep convection observed over Oklahoma during the Midlatitude Continental Convective Cloud Experiment (MC3E), 2) orographic clouds observed over North California during the Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX), and 3) supercooled, stratiform clouds over the United Kingdom, observed during the Aerosol Properties, Processes And Influences on the Earth’s climate (APPRAISE) campaign. AC uses the dynamical core of the WRF Model and has hybrid bin–bulk microphysics and a 3D mesoscale domain. AC is validated against coincident aircraft, ground-based, and satellite observations for all three cases. Filtered concentrations of ice (.0.1–0.2 mm) agree with those observed at all sampled levels. AC predicts the INP activity of various types of aerosol particles with an empirical parameterization (EP), which follows a singular approach (no time dependence). Here, the EP is modified to represent time-dependent INP activity by a purely empirical approach, using our published laboratory observations of time-dependent INP activity. In all simulated clouds, the inclusion of time dependence increases the predicted INP activity of mineral dust particles by 0.5–1 order of magnitude. However, there is little impact on the cloud glaciation because the total ice is mostly (80%–90%) from secondary ice production (SIP) at levels warmer than about 2368C. The Hallett–Mossop process and fragmentation in ice–ice collisions together initiate about 70% of the total ice, whereas fragmentation during both raindrop freezing and sublimation contributes ,10%. Overall, total ice concentrations and SIP are unaffected by time-dependent INP activity. In the simulated APPRAISE case, the main causes of persistence of long-lived clouds and precipitation are predicted to be SIP in weak embedded convection and reactivation following recirculation of dust particles in supercooled layer cloud

New Empirical Formulation for the Sublimational Breakup of Graupel and Dendritic Snow

Ice fragments are generated by sublimation of ice particles in subsaturated conditions in natural clouds. Conceivably, such sublimational breakup would be expected to cause ice multiplication in natural clouds. Any fragment that survives will grow to become ice precipitation that may sublimate and fragment further. As a first step toward assessing this overlooked process, a formulation is proposed for the number of ice fragments from sublimation of ice particles for an atmospheric model. This is done by amalgamating laboratory observations from previously published studies. The concept of a “sublimated mass activity spectrum” for the breakup is applied to the dataset. The number of ice fragments is determined by the relative humidity over ice and the initial size of the parent ice particles. The new formulation applies to dendritic crystals and heavily rimed particles only. Finally, a thought experiment is performed for an idealized scenario of subsaturation with in-cloud descent. Scaling analysis yields an estimate of an ice enhancement ratio of about 5 (10) within a weak deep convective downdraft of about 2 m s−1, for an initial monodisperse population of dendritic snow (graupel) particles of 3 L−1 and 2 mm. During descent, there is a dynamic equilibrium between continual emission of fragments and their depletion by sublimation. A simplified bin microphysics parcel model exhibits this dynamical quasi equilibrium, consistent with the thought experiment. The fragments have average lifetimes of around 90 and 70 s for dendrites and graupel, respectively. Sublimational breakup is predicted to cause significant secondary ice production

Comment on "Review of Experimental Studies of Secondary Ice Production" by Korolev and Leisner (2020)

International audienc

Time dependence of heterogeneous ice nucleation by ambient aerosols : laboratory observations and a formulation for models

The time dependence of ice-nucleating particle (INP) activity is known to exist, yet for simplicity it is often omitted in atmospheric models as an approximation. Hitherto, only limited experimental work has been done to quantify this time dependency, for which published data are especially scarce regarding ambient aerosol samples and longer timescales. In this study, the time dependence of INP activity is quantified experimentally for six ambient environmental samples. The experimental approach includes a series of hybrid experiments with alternating constant cooling and isothermal experiments using a recently developed cold-stage setup called the Lund University Cold-Stage (LUCS). This approach of observing ambient aerosol samples provides the optimum realism for representing their time dependence in any model. Six ambient aerosol samples were collected at a station in rural Sweden representing aerosol conditions likely influenced by various types of INPs: marine, mineral dust, continental pristine, continental-polluted, combustion-related and rural continental aerosol. Active INP concentrations were seen to be augmented by about 40% to 100% (or 70% to 200%), depending on the sample, over 2h (or 10h). Mineral dust and rural continental samples displayed the most time dependence. This degree of time dependence observed was comparable to, but weaker than, that seen in previous published works. A general tendency was observed for the natural timescale of the freezing to dilate increasingly with time. The fractional freezing rate was observed to decline steadily with the time since the start of isothermal conditions following a power law. A representation of time dependence for incorporation into schemes of heterogeneous ice nucleation that currently omit it is proposed. Our measurements are inconsistent with the simplest purely stochastic model of INP activity, which assumes that the fractional freezing rate of all unfrozen drops is somehow constant and would eventually overpredict active INPs. In reality, the variability of efficiencies among INPs must be treated with any stochastic theory

Dependencies of Four Mechanisms of Secondary Ice Production on Cloud-Top Temperature in a Continental Convective Storm

Various mechanisms of secondary ice production (SIP) cause multiplication of numbers of ice particle, after the onset of primary ice. A measure of SIP is the ice enhancement ratio (“IE ratio”) defined here as the ratio between number concentrations of total ice (excluding homogeneously nucleated ice) and active ice-nucleating particles (INPs). A convective line observed on 11 May 2011 over the Southern Great Plains in the Mesoscale Continental Convective Cloud Experiment (MC3E) campaign was simulated with the “Aerosol–Cloud” (AC) model. AC is validated against coincident MC3E observations by aircraft, ground-based instruments, and satellite. Four SIP mechanisms are represented in AC: the Hallett–Mossop (HM) process of rime splintering, and fragmentation during ice–ice collisions, raindrop freezing, and sublimation. The vertical profile of the IE ratio, averaged over the entire simulation, is almost uniform (102 to 103) because fragmentation in ice–ice collisions dominates at long time scales, driving the ice concentration toward a theoretical maximum. The IE ratio increases with both the updraft (HM process, fragmentation during raindrop freezing, and ice–ice collisions) and downdraft speed (fragmentation during ice–ice collisions and sublimation). As reported historically in aircraft sampling, IE ratios were predicted to peak near 103 for cloud-top temperatures close to the −12°C level, mostly due to the HM process in typically young clouds with their age less than 15 min. At higher altitudes with temperatures of −20° to −30°C, the predicted IE ratios were smaller, ranging from 10 to 102, and mainly resulted from fragmentation in ice–ice collisions

The influence of multiple groups of biological ice nucleating particles on microphysical properties of mixed-phase clouds observed during MC3E

A new empirical parameterization (EP) for multiple groups of primary biological aerosol particles (PBAPs) is implemented in the aerosol-cloud model (AC) to investigate their roles as ice nucleating particles (INPs). The EP describes the heterogeneous ice nucleation by (1) fungal spores, (2) bacteria, (3) pollen, (4) detritus of plants, animals, and viruses, and (5) algae. Each group includes fragments from the originally emitted particles. A high-resolution simulation of a midlatitude mesoscale squall line by AC is validated against airborne and ground observations. Sensitivity tests are carried out by varying the initial vertical profiles of the loadings of individual PBAP groups. The resulting changes in warm and ice cloud microphysical parameters are investigated. The changes in warm microphysical parameters, including liquid water content and cloud droplet number concentration, are minimal (<10 %). Overall, PBAPs have little effect on the ice number concentration (<6 %) in the convective region. In the stratiform region, increasing the initial PBAP loadings by a factor of 1000 resulted in less than 40 % change in ice number concentrations. The total ice concentration is mostly controlled by various mechanisms of secondary ice production (SIP). However, when SIP is intentionally shut down in sensitivity tests, increasing the PBAP loading by a factor of 100 has an effect of less than 3 % on the ice phase. Further sensitivity tests revealed that PBAPs have little effect on surface precipitation and on the shortwave and longwave flux (<4 %) for a 100-fold perturbation in PBAPs

The microphysics of the warm-rain and ice crystal processes of precipitation in simulated continental convective storms

Precipitation in clouds can form by either warm-rain or ice crystal processes, referred to as warm and cold formation pathways, respectively. Here, we investigate the warm and cold pathway contributions to surface precipitation in simulated continental convective storms. We analyze three contrasting convective storms that are cold-based, slightly warm-based and very warm-based. We apply tracer-tagging techniques in our aerosol-cloud model to determine simulated microphysical pathways that lead to precipitation. We find cold components of graupel and rain mass were higher than warm components in cold- and slightly warm-based clouds. By contrast, in very warm-based clouds nearly 80% of surface precipitation was formed via warm-rain processes. Lowering of cloud base altitude to levels about 10–20 K warmer switched surface precipitation to being mostly warm, due to enhanced moisture content in the planetary boundary layer and larger cloud droplets aloft intensifying raindrop freezing. Our simulations indicate that warm and cold processes co-exist in any storm and the balance between them is determined by cloud base temperature and solute aerosol conditions