Pre-activation of aerosol particles by ice preserved in pores

Abstract

Abstract. Pre-activation denotes the capability of particles or materials to nucleate ice at lower relative humidities or higher temperatures compared to their intrinsic ice nucleation efficiency after having experienced an ice nucleation event or low temperature before. This review presumes that ice preserved in pores is responsible for pre-activation and analyses pre-activation under this presumption. Idealized trajectories of air parcels are used to discuss the pore characteristics needed for ice to persist in pores and to induce macroscopic ice growth out of the pores. The pore width needed to keep pores filled with water decreases with decreasing relative humidity as described by the inverse Kelvin equation. Thus, narrow pores remain filled with ice well below ice saturation. However, the smaller the pore width, the larger the melting and freezing point depressions within the pores. Therefore, pre-activation due to pore ice is constrained by the melting of ice in narrow pores and the sublimation of ice from wide pores imposing restrictions on the temperature and relative humidity range of pre-activation for cylindrical pores. Ice is better protected in ink-bottle-shaped pores with a narrow opening leading to a large cavity. However, whether pre-activation is efficient also depends on the capability of ice to grow macroscopically, i.e. out of the pore. A strong effect of pre-activation is expected for swelling pores, because at low relative humidity (RH) their openings narrow and protect the ice within them against sublimation. At high relative humidities, they open up and the ice can grow to macroscopic size and form an ice crystal. Similarly, ice protected in pockets is perfectly sheltered against sublimation but needs the dissolution of the surrounding matrix to be effective. Pores partially filled with condensable material may also show preactivation. In this case, complete filling occurs at lower RH than for empty pores and freezing shifts to lower temperatures.Pre-activation experiments confirm that materials susceptible to pre-activation are indeed porous. Pre-activation was observed for clay minerals like illite, kaolinite, and montmorillonite with inherent porosity. The largest effect was observed for the swelling clay mineral montmorillonite. Some materials may acquire porosity, depending on the formation and processing conditions. Particles of CaCO 3 , meteoritic material, and volcanic ash showed pre-activation for some samples or in some studies but not in other ones. Quartz and silver iodide were not susceptible to pre-activation.Atmospheric relevance of pre-activation by ice preserved in pores may not be generally given but depend on the atmospheric scenario. Lower-level cloud seeding by pre-activated particles released from high-level clouds crucially depends on the ability of pores to retain ice at the relative humidities and temperatures of the air masses they pass through. Porous particles that are recycled in wave clouds may show pre-activation with subsequent ice growth as soon as ice sat...

The Impact of Cloud Processing on the Ice Nucleation Abilities of Soot Particles at Cirrus Temperatures

“…While narrower pores can remain filled with ice well below ice saturation (conditions satisfied at the exit of HINC1) due to the inverse Kelvin effect, melting and freezing point depression increase with decreasing pore size. Hence, preactivation due to ice pockets is constrained by the melting of ice in narrow pores and the sublimation of ice from larger pores (Marcolli, ). Using the example of T CATZ =233 K along with the contrail processing conditions in HINC1, the relative humidity within CATZ would be RH i,CATZ ( T =233 K)=56% (equivalent to RH w,CATZ ( T =233 K)=38%).…”

“…Here, M w =18.015 g/mol is the molar mass of water, ρ w ( T =298 K)=996.23 kg/m 3 denotes the density of liquid water, evaluated using the parameterization given by Marcolli (), and n a denotes the moles of water molecules that are added per unit mass to the adsorbent. The gravimetrically measured change in sample mass, Δ m , can directly be used to derive n a …”

Elucidating ice formation pathways in the aerosol-climate model ECHAM6-HAM2

“…Beyond the theoretical and experimental uncertainties of the freezing mechanisms (Welti et al, 2014;Ickes et al, 2015;Marcolli, 2017), a realistic representation of cloud glaciation is further complicated by uncertainties in the parameterization of subsequent ice growth. Due to the lower saturation water vapor pressure over an ice crystal compared to a liquid droplet surface, cloud ice can grow below water saturation, leading to evaporation of the cloud droplets.…”

Prognostic parameterization of cloud ice with a single category in the aerosol-climate model ECHAM(v6.3.0)-HAM(v2.3)

“…In this study we focus on the pathways subsequent to ice initiation by a more physically-based description of cloud ice but acknowledge the importance of ongoing research to understand freezing mechanisms (Welti et al, 2014;Ickes et al, 2015;Marcolli, 2017) and resulting parameterization development (Phillips et al, 2013;Ickes et al, 2017). We will use the microphysical properties of ice described in Morrison and Milbrandt (2015) (hereafter MM15) and embed them in the ECHAM6-HAM2 microphysics scheme.…”