The frustration in super‐ionic conductors enables their exceptionally high ionic conductivities, which are desired for many technological applications including batteries and fuel cells. A key challenge in the study of frustration is the difficulties in analyzing a large number of disordered atomistic configurations. Using lithium super‐ionic conductors as model systems, we propose and demonstrate the density of atomistic states (DOAS) analytics to quantitatively characterize the onset and degree of disordering, reveal the energetics of local disorder, and elucidate how the frustration enhances diffusion through the broadening and overlapping of the energy levels of atomistic states. Furthermore, material design strategies aided by the DOAS are devised and demonstrated for new super‐ionic conductors. The DOAS is generally applicable analytics for unraveling fundamental mechanisms in complex atomistic systems and guiding material design.
Architected materials design across orders of magnitude length scale intrigues exceptional mechanical responses nonexistent in their natural bulk state. However, the so‐termed mechanical metamaterials, when scaling bottom down to the atomistic or microparticle level, remain largely unexplored and conventionally fall out of their coarse‐resolution, ordered‐pattern design space. Here, combining high‐throughput molecular dynamics (MD) simulations and machine learning (ML) strategies, some intriguing atomistic families of disordered mechanical metamaterials are discovered, as fabricated by melt quenching and exemplified herein by lightweight‐yet‐stiff cellular materials featuring a theoretical limit of linear stiffness–density scaling, whose structural disorder—rather than order—is key to reduce the scaling exponent and is simply controlled by the bonding interactions and their directionality that enable flexible tunability experimentally. Importantly, a systematic navigation in the forcefield landscape reveals that, in‐between directional and non‐directional bonding such as covalent and ionic bonds, modest bond directionality is most likely to promotes disordered packing of polyhedral, stretching‐dominated structures responsible for the formation of metamaterials. This work pioneers a bottom‐down atomistic scheme to design mechanical metamaterials formatted disorderly, unlocking a largely untapped field in leveraging structural disorder in devising metamaterials atomistically and, potentially, generic to conventional upscaled designs.
more » « less- Award ID(s):
- 2119643
- PAR ID:
- 10489728
- Publisher / Repository:
- willey
- Date Published:
- Journal Name:
- Advanced Science
- ISSN:
- 2198-3844
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract -
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Abstract The frustration in super‐ionic conductors enables their exceptionally high ionic conductivities, which are desired for many technological applications including batteries and fuel cells. A key challenge in the study of frustration is the difficulties in analyzing a large number of disordered atomistic configurations. Using lithium super‐ionic conductors as model systems, we propose and demonstrate the density of atomistic states (DOAS) analytics to quantitatively characterize the onset and degree of disordering, reveal the energetics of local disorder, and elucidate how the frustration enhances diffusion through the broadening and overlapping of the energy levels of atomistic states. Furthermore, material design strategies aided by the DOAS are devised and demonstrated for new super‐ionic conductors. The DOAS is generally applicable analytics for unraveling fundamental mechanisms in complex atomistic systems and guiding material design.
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1002/advs.202304834
