Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds

Two-dimensional (2D) materials have emerged as promising candidates for next-generation electronic and optoelectronic applications. Yet, only a few dozens of 2D materials have been successfully synthesized or exfoliated. Here, we search for novel 2D materials that can be easily exfoliated from their parent compounds. Starting from 108423 unique, experimentally known three-dimensional compounds we identify a subset of 5619 that appear layered according to robust geometric and bonding criteria. High-throughput calculations using van-der-Waals density-functional theory, validated against experimental structural data and calculated random-phase-approximation binding energies, allow to identify 1825 compounds that are either easily or potentially exfoliable. In particular, the subset of 1036 easily exfoliable cases provides novel structural prototypes and simple ternary compounds as well as a large portfolio of materials to search from for optimal properties. For a subset of 258 compounds we explore vibrational, electronic, magnetic, and topological properties, identifying 56 ferromagnetic and antiferromagnetic systems, including half-metals and half-semiconductors. This archive entry contains the database of 2D materials (structural parameters, band structures, binding energies, phonons for the subset of the 258 easily exfoliable materials with less than 6 atoms, structures and binding energies for the remaining 1567 materials) together with the provenance of all data and calculations as stored by AiiDA.

二维（2D）材料已成为下一代电子与光电子应用领域极具潜力的候选材料。然而目前仅成功合成或剥离出数十种二维材料。本研究旨在筛选可从母体化合物中轻松剥离的新型二维材料：我们从108423种经实验确证的独特三维化合物出发，通过严谨的几何与成键判据筛选出5619种具有层状结构的候选体系。基于范德瓦尔斯密度泛函理论（van-der-Waals density-functional theory）开展高通量计算，并以实验结构数据与随机相位近似（random-phase-approximation）结合能计算结果进行验证，最终筛选出1825种可轻松剥离或具备潜在剥离可行性的化合物。其中，1036种可轻松剥离的化合物不仅提供了新型结构原型与简单三元化合物体系，还为筛选最优性能材料提供了丰富的候选库。我们对其中258种化合物开展了振动、电子、磁学与拓扑性质研究，共识别出56种铁磁与反铁磁体系，涵盖半金属与半半导体材料。本归档条目包含二维材料数据库（其中原子数少于6的258种易剥离材料附带结构参数、能带结构、结合能与声子谱数据，其余1567种材料附带结构与结合能数据），同时收录了由AiiDA存储的全部数据与计算过程溯源信息。