Data-driven quest for two-dimensional non-van der Waals materials

Abstract

Two-dimensional (2D) materials are frequently associated with the sheets which form bulk layered compounds bonded by van der Waals (vdW) forces. The anisotropy and weak interaction between the sheets have also been the main criteria in the computational search for new 2D systems, which predicted about 2000 exfoliable compounds. However, several representatives of a new type of non-vdW 2D systems, such as hematene or ilmenene, which have no layered 3D analogues, and which, unlike, e.g. silicene, do not need to strongly interact with the substrate to be stable, were recently manufactured. The family of non-vdW 2D materials is an attractive playground for data-driven high-throughput approaches as computational design principles are still missing. Here, we outline a new set of 8 binary and 20 ternary candidates by filtering the AFLOW-ICSD database according to the structural prototype of the first two template systems realized in experiment. All materials show a strong structural relaxation upon confinement to 2D which is essential to correctly estimate the bonding strength between facets. The oxidation state of the cations at the surface of the sheets is demonstrated to regulate the inter-facet binding energy with low oxidation states leading to weak bonding. We anticipate this descriptor to be highly useful to obtain novel 2D materials, providing clear guidelines for experiments. Our calculations further indicate that the materials exhibit a vast range of appealing electronic, optical and magnetic properties, which is expected to also make them attractive for potential applications particularly in spintronics.

26 pages, 6 figures

References in corpus (8)

• Electric Field Effect in Atomically Thin Carbon Films
• Two Dimensional Atomic Crystals
• Magnetic 2D materials and heterostructures
• Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
• Van der Waals bonding in layered compounds from advanced first-principles calculations
• A RESTful API for exchanging Materials Data in the AFLOWLIB.org consortium
• Equipartition of Energy Defines the Size-Thickness Relationship in Liquid-Exfoliated Nanosheets
• Automated coordination corrected enthalpies with AFLOW-CCE

Cited by in corpus (14)

• Step-edge epitaxy for borophene growth on insulators
• A New Group of Two-Dimensional Non-van der Waals Materials with Ultra Low Exfoliation Energies
• High-refractive index and mechanically cleavable non-van der Waals InGaS3
• Screening 0D materials for 2D nanoelectronics applications
• Magnetic State Control of Non-van der Waals 2D Materials by Hydrogenation
• Prediction and Characterization of Two-Dimensional Zn2VN3
• Two-dimensional non-van der Waals niobium nitride nanosheets with high-temperature two-gap superconductivity
• A Framework for Identifying Non-van der Waals 2D Materials
• Massive Discovery of Low-Dimensional Materials from Universal Computational Strategy
• Effect of molecular and electronic geometries on the electronic density in FLO-SIC
• Enhanced Magnetism and Phase Transitions in Ultrathin Quantum Spin Liquid Na2IrO3 Flakes
• Non-van der Waals Heterostructures
• Magnetic ground state and strain-mediated chiral-like atomic distortions behavior in two-dimensional rectangular spin lattice
• High-Throughput Prediction of Exfoliable Non-van der Waals Materials from a Universal Potential