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<br />44 <br /> <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br />I <br /> <br />also too ambiguous in explaining the difference between condensation- <br /> <br />freezing and immersion-freezing. For this study, condensation-freezing <br />is distinguished from immersion-freezing by the requirement that ice <br /> <br />crystal formation occurs instantly in response to a given water <br /> <br />supersaturation and temperature, and the lack of requirement for the <br /> <br />activation of a macroscopic cloud droplet. In fact, nucleation that <br /> <br /> <br />follows from predicted cloud droplet activation is termed a form of <br /> <br /> <br />immersion-freezing. Nucleation due to water supersaturation in excess <br /> <br />of the immersion-freezing fraction is termed condensation-freezing. <br /> <br />These working definitions can be further clarified by considering the <br /> <br /> <br />history of a particle in a condensing environment, as is done next. <br /> <br /> <br />As the schematic in Fig. 4.1 shows, the four nucleation modes <br /> <br />actually present five different pathways by which ice can form when <br /> <br />heterogeneous ice nuclei are present or are introduced into ice <br /> <br />supersaturated or cloudy air below ooC. Deposition nucleation requires <br /> <br />only that the saturation ratio with respect to ice exceed 1. Then, at <br /> <br />any temperature (Tl) and time (tl), some fraction of the aerosol (F1) <br /> <br />will act to form ice (lowest path in Figure 4.1). At a constant <br /> <br />temperature and ice supersaturation (Si1)' the fraction Fl may vary <br /> <br />with time, expressing the kinetic rate of ice crystal formation. <br /> <br />When saturation with respect to water (Sw1) is approached and <br /> <br />exceeded, some fraction (F2) of the ice nucleating aerosol may hydrate, <br /> <br />form a liquid haze particle, or activate as a solution droplet (middle <br /> <br />pathway in Figure 4.1). This will depend primarily on the chemical <br /> <br />hygroscopic characteristics of the aerosol, and the peak Swl achieved, <br /> <br />At temperatures Tl below OOC, the instantaneous freezing of the <br /> <br />condensing liquid phase is referred to as condensation-freezing <br />