4.8 Article

Active sites for ice nucleation differ depending on nucleation mode

出版社

NATL ACAD SCIENCES
DOI: 10.1073/pnas.2022859118

关键词

nucleation; crystallization; ice; pores; active sites

资金

  1. Engineering and Physical Sciences Research Council (EPSRC) [EP/M003027/1, EP/N002423/1, EP/R018820/1]
  2. European Research Council [648661]
  3. Leverhulme Trust [RPG-2014-306]

向作者/读者索取更多资源

The nucleation of ice crystals in clouds is influenced by different meteorological conditions, leading to distinct pathways of immersion freezing and deposition nucleation. Experimental results on two atmospheric minerals show little correlation between active sites in these two modes, suggesting different properties determine the activity of nucleation sites for each mode. Therefore, the ability to nucleate is pathway dependent, and mode of nucleation must be considered when applying experimental data in cloud models.
The nucleation of ice crystals in clouds is poorly understood, despite being of critical importance for our planet?s climate. Nucleation occurs largely at rare ?active sites? present on airborne particles such as mineral dust, but the nucleation pathway is distinct under different meteorological conditions. These give rise to two key nucleation pathways where a particle is either immersed in a supercooled liquid water droplet (immersion freezing mode) or suspended in a supersaturated vapor (deposition mode). However, it is unclear if the same active sites are responsible for nucleation in these two modes. Here, we directly compare the sites that are active in these two modes by performing immersion freezing and deposition experiments on the same thin sections of two atmospherically important minerals (feldspar and quartz). For both substrates, we confirm that nucleation is dominated by a limited number of sites and show that there is little correlation between the two sets of sites operating in each experimental method: across both materials, only six out of 73 sites active for immersion freezing nucleation were also active for deposition nucleation. Clearly, different properties determine the activity of nucleation sites for each mode, and we use the pore condensation and freezing concept to argue that effective deposition sites have size and/or geometry requirements not of relevance to effective immersion freezing sites. Hence, the ability to nucleate is pathway dependent, and the mode of nucleation has to be explicitly considered when applying experimental data in cloud models.

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