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Although it is crucial to the formation of cirrus clouds and consequently the climate on Earth, the unambiguous effect of carbonaceous materials (CM) on ice nucleation remains to be unveiled as the chemical variation on the surface of CM is always complicated by the change in morphology. Here, we separately investigate the effects of the surface chemistry and morphology of CM on ice nucleation by studying ice nucleation on highly oriented pyrolytic graphite surfaces treated with different types of plasmas. We discover unambiguously that increasing the density of hydroxyl groups leads to an increased activity of ice nucleation on the surface of graphene, while no observable effects are found when carboxylic groups are introduced. Analysis based on the classical nucleation theory reveals that the increase in the density of hydroxyl groups on the graphene surface results in an increased binding energy between the …