Holden Mark A, Whale Thomas F, Tarn Mark D, O'Sullivan Daniel, Walshaw Richard D, Murray Benjamin J, Meldrum Fiona C, Christenson Hugo K
School of Earth and Environment, University of Leeds, Leeds LS2 9JT, UK.
School of Chemistry, University of Leeds, Leeds LS2 9JT, UK.
Sci Adv. 2019 Feb 1;5(2):eaav4316. doi: 10.1126/sciadv.aav4316. eCollection 2019 Feb.
Understanding how surfaces direct nucleation is a complex problem that limits our ability to predict and control crystal formation. We here address this challenge using high-speed imaging to identify and quantify the sites at which ice nucleates in water droplets on the two natural cleavage faces of macroscopic feldspar substrates. Our data show that ice nucleation only occurs at a few locations, all of which are associated with micron-size surface pits. Similar behavior is observed on α-quartz substrates that lack cleavage planes. These results demonstrate that substrate heterogeneities are the salient factor in promoting nucleation and therefore prove the existence of active sites. We also provide strong evidence that the activity of these sites derives from a combination of surface chemistry and nanoscale topography. Our results have implications for the nucleation of many materials and suggest new strategies for promoting or inhibiting nucleation across a wide range of applications.
理解表面如何引导成核是一个复杂的问题,它限制了我们预测和控制晶体形成的能力。我们在此通过高速成像来应对这一挑战,以识别和量化在宏观长石基底的两个天然解理面上的水滴中冰核形成的位置。我们的数据表明,冰核形成仅发生在少数几个位置,所有这些位置都与微米级的表面凹坑有关。在没有解理面的α-石英基底上也观察到了类似的行为。这些结果表明,基底的不均匀性是促进成核的显著因素,因此证明了活性位点的存在。我们还提供了有力证据,表明这些位点的活性源自表面化学和纳米级形貌的结合。我们的结果对许多材料的成核具有启示意义,并为在广泛应用中促进或抑制成核提出了新策略。