GeSn on Si has attracted much research interest due to its tunable direct bandgap for mid‐infrared applications. Recently, short‐range order (SRO) in GeSn alloys has been theoretically predicted, which profoundly impacts the band structure. However, characterizing SRO in GeSn is challenging. Guided by physics‐informed Poisson statistical analyses of k‐nearest neighbors (KNN) in atom probe tomography (APT), a new approach is demonstrated here for 3D nanoscale SRO mapping and semi‐quantitative strain mapping in GeSn. For GeSn with ≈14 at. % Sn, the SRO parameters of Sn–Sn 1NN in 10 × 10 × 10 nm3 nanocubes can deviate from that of the random alloys by ±15 %. The relatively large fluctuation of the SRO parameters contributes to band‐edge softening observed optically. Sn–Sn 1NN also tends to be more favored toward the surface, less favored under strain relaxation or tensile strain, while almost independent of local Sn composition. An algorithm based on least square fit of atomic positions further verifies this Poisson‐KNN statistical method. Compared to existing macroscopic spectroscopy or electron microscopy techniques, this new APT statistical analysis uniquely offers 3D SRO mapping at nanoscale resolution in a relatively large volume with millions of atoms. It can also be extended to investigate SRO in other alloy systems.

Control of heterogeneous ice nucleation (HIN) is critical for applications that range from iceophobic surfaces to ice-templated materials. HIN on 2D materials is a particular interesting topic that still lacks extensive experimental investigations. Here, we focus on the HIN on single-layer graphene (SLG) transferred onto different substrates, including silicon, silica, and thermal oxide on silicon. Complemented by other samples without SLG, we obtain a large range of wetting contact angles (WCAs) from 2° to 95°. All pristine SLG samples exhibit a large contact angle of ∼95°, which is close to the theoretical value of 96° for free-standing SLG, irrespective of the substrate and even in the presence of nanoscale wrinkles on SLG, which are due to the transfer process, indicating that the topographical features have little impact on the wetting behavior. Interestingly, SLG displays changes in hydrophobicity upon repeated water droplet freezing–melting–drying cycles due to a shift in Fermi level and/or enhanced water–substrate polar molecular interactions, likely induced by residual adsorption of H2O molecules. We found that a 0.04 eV decrease in SLG Fermi level reduces the SLG/water interface energy by ∼6 mJ/m2, thereby making SLG less hydrophobic. Counterintuitively, the reduction in SLG/water interface energy and the enhanced hydrophilicity after repeated freezing–melting–evaporation cycles actually decreases the freezing temperature by ∼3–4 °C, thereby slightly retarding rather than enhancing HIN. We also found that the water droplet freezing temperature differed by only ∼1 °C on different substrates with WCAs from 2° to 95°, an intriguing and yet reasonable result that confirms that wettability alone is not a good indicator of HIN capability. The HIN rate is rather determined by the difference between substrate/water and substrate/ice interface energies, which was found to stay almost constant for substrates weakly interacting with water/ice via van der Waals or hydrogen bonds, irrespective of hydrophilicity.