Multiscale Optical Imaging Unveils the Distinct Roles of Supersaturation and Substrate in Interfacial Crystallization

invariably follows a homogeneous nucleation-bulk solution deposition pathway. Quantitative analysis of this homogeneous nucleation pathway reveals that hydrophilic surfaces capture a greater density of nascent nuclei, limiting their final size through spatial confinement and growth competition. LRISM-based three-dimensional orientation analysis further confirms that hydrophilic surfaces preferentially induce horizontal crystal alignment. These results establish quantitative observables and a general methodology for designing scale-mitigation surfaces by controlling postnucleation capture and orientation rather than nucleation inhibition alone.