Low-density materials with tailorable properties have attracted attention for decades, yet stiff materials that can resiliently tolerate extreme forces and deformation while being manufactured at large scales have remained a rare find. Designs inspired by nature, such as hierarchical composites and atomic lattice-mimicking architectures, have achieved optimal combinations of mechanical properties but suffer from limited mechanical tunability, limited long-term stability, and low-throughput volumes that stem from limitations in additive manufacturing techniques. Based on natural self-assembly of polymeric emulsions via spinodal decomposition, here we demonstrate a concept for the scalable fabrication of nonperiodic, shell-based ceramic materials with ultralow densities, possessing features on the order of tens of nanometers and sample volumes on the order of cubic centimeters. Guided by simulations of separation processes, we numerically show that the curvature of self-assembled shells can produce close to optimal stiffness scaling with density, and we experimentally demonstrate that a carefully chosen combination of topology, geometry, and base material results in superior mechanical resilience in the architected product. Our approach provides a pathway to harnessing self-assembly methods in the design and scalable fabrication of beyond-periodic and nonbeam-based nano-architected materials with simultaneous directional tunability, high stiffness, and unsurpassed recoverability with marginal deterioration.

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Complex microstructural patterns arise as energy-minimizers in systems having non-convex energy landscapes such as those associated with phase transformations, deformation twinning, or finite-strain crystal plasticity. The prediction of such patterns at the microscale along with the resulting, effective material response at the macroscale is key to understanding a wide range of mechanical phenomena and has classically been dealt with by simplifying energy relaxation theory or by expensive finite element calculations. Here, we discuss a stabilized Fourier spectral technique for the homogenized response at the level of a representative volume element (RVE). We show that the FFT-based method admits sufficiently high resolution suitable to predict the emergence of energy-minimizing microstructures and the resulting effective response by computing the approximated quasiconvex energy hull. We test the method in the classical single-slip problem in single-and bicrystals. Especially the latter goes beyond the scope of traditional finite element and analytical relaxation treatments and hints at mechanisms of pattern formation in polycrystals. We also demonstrate that the chosen spectral finite-difference approximation, important for removing ringing artifacts in the presence of high contrasts, adds a natural regularization to the non-convex minimization. Finally, the technique is applied to polycrystalline pure magnesium, where we account for the competition between dislocation-mediated plasticity and deformation twinning. These inelastic deformation mechanisms result in complex texture evolution paths at the polycrystalline mesoscale and are simulated within RVEs of varying grain size and texture by a constitutive crystal plasticity model with an effective, volume fraction-based description of twinning.