Abstract

Summary The intricate three-dimensional (3D) conformations of two-dimensional (2D) macromolecules play fundamental roles in biology and materials. Diverse conformational phases of 2D macromolecules have been predicted in theory but remain unclear in experimental validation. We established a conformational phase map of 2D macromolecules in solution using single-layer graphene oxide as the experimental model. The map covers not only predictable intramolecular phases but also intermolecular behaviors beyond theoretical prediction. We identified a symmetry-selection rule that discriminates anisotropic one-dimensional folding and isotropic 3D crumpling phases determined by the surface interaction. These symmetry-selective behaviors indicate a strong path-dependent competition between the elastic distortion and surface adhesion. The phase map offers a unified description of the conformational behaviors of 2D macromolecules that bridges the gap between theories and experiments, as well as a general guidance to precisely control multiscale condensed conformations of 2D nanomaterials.

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