Natural materials exhibit emergent mechanical properties as a result of their nanoarchitected, nanocomposite structures with optimized hierarchy, anisotropy, and nanoporosity. Fabrication of such complex systems is currently challenging because high-quality three-dimensional (3D) nanoprinting is mostly limited to simple, homogeneous materials. We report a strategy for the rapid nanoprinting of complex structural nanocomposites using metal nanoclusters. These ultrasmall, quantum-confined nanoclusters function as highly sensitive two-photon activators and simultaneously serve as precursors for mechanical reinforcements and nanoscale porogens. Nanocomposites with complex 3D architectures are printed, as well as structures with tunable, hierarchical, and anisotropic nanoporosity. Nanocluster-polymer nanolattices exhibit high specific strength, energy absorption, deformability, and recoverability. This framework provides a generalizable, versatile approach for the use of photoactive nanomaterials in additive manufacturing of complex systems with emergent mechanical properties.
The ability to gradually modify the atomic structures of nanomaterials and directly identify such structural variation is important in nanoscience research. Here, we present the first example of a high-pressure single-crystal X-ray diffraction analysis of atomically precise metal nanoclusters. The pressure-dependent, subangstrom structural evolution of an ultrasmall gold nanoparticle, Au25S18, has been directly identified. We found that a 0.1 Å decrease of the Au–Au bond length could induce a blue-shift of 30 nm in the photoluminescence spectra of gold nanoclusters. From theoretical calculations, the origins of the blue-shift and enhanced photoluminescence under pressure are investigated, which are ascribed to molecular orbital symmetry and conformational locking, respectively. The combination of the high-pressure in situ X-ray results with both theoretical and experimental optical spectra provides a direct and generalizable avenue to unveil the underlying structure–property relations for nanoclusters and nanoparticles which cannot be obtained through traditional physical chemistry measurements.
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