A Large Family of Synthetic Two-Dimensional Metal Hydrides

Abstract

Synthetic two-dimensional (2D) materials without layered bulk allotropes are approaching a new frontier of materials flatland, one with properties richer than those of graphene-like materials. This is the case even as only a few chemical elements and blends have shown synthetic 2D forms. While hydrogen and metals are earth-abundant and form numerous compounds, rarely are 2D materials with only robust metal−hydrogen bonds. Here, a large new family of 2D materials is found from metal hydrides by high-throughput computational search augmented with first-principles calculations. There are 110 thermally and dynamically stable 2D materials that range from metallic materials to wide-gap semiconductors. A subgroup of these materials even varies from topological insulators to nodal-loop semimetals as well as from antiferromagnetic semiconductors to ferromagnetic halfmetals. Unexpectedly, these monolayers resemble graphene in an ability to form weak interlayer interaction due to the variable multicenter bonding of hydrogen that eliminates the otherwise prevalent dangling bonds, rather than the covalent bonds between stacked layers as in previously reported synthetic 2D materials. This feature will favor potential experimental synthesis of these metal hydride monolayers.

Coupling a Crystal Graph Multilayer Descriptor to Active Learning for Rapid Discovery of 2D Ferromagnetic Semiconductors/Half‐Metals/Metals

“…Theoretical simulation provides a more efficient way for 2D ferromagnetic material discovery, [ 1a,5 ] which offers a large number of novel candidates with great performance for experiments. [ 6 ] Recently, the emergence of first‐principle high‐throughput calculations greatly accelerates the discovery, [ 7 ] while such strategy is restricted by the complexity of 2D magnetic materials and limitation of computational resources as well, causing the search throughout the whole chemical space to be unrealistic. In order to speed up the research and develop (R&D) cycle of new 2D magnetic materials, more efficient methods should be developed.…”

“…The optimized crystal structures and considered AFM configurations are presented in Figures S9 and S10, Supporting Information, as well. Among them, 11 candidates, Cr 2 Ge 2 Te 6 , [ 3 ] Fe 3 GeTe 2 , [ 4a ] CrWI 6 , [ 6c ] VO 2 , [ 24 ] VAg(PSe 3 ) 2 , [ 7b ] CrO 2 , [ 25 ] CrPTe 3 , [ 7b ] YCl, [ 14 ] CrSiTe 3 , [ 26 ] CrOF, [ 27 ] and CrPS 4 [ 28 ] have been successfully synthesized experimentally or predicted by previous first‐principles calculations. These prove the reliability of our ML method.…”

Structure Prototype Outperforming MXenes in Stability and Performance in Metal‐Ion Batteries: A High Throughput Study

“…The high throughput approach usually starts from a known structure prototype and varies the elements involved, which has led to extensive databases. [ 30,31 ] However, this procedure limits the structural diversity. For example, more than half of the materials in the database of ref.…”

Ising ferromagnetism and robust half-metallicity in two-dimensional honeycomb-kagome Cr2O3 layer

“…In contrast to the current research, which is mainly focused on the 2D graphene and transition metal dichalcogenide-like structures [10][11][12][13][14] , very few atomically thin metal oxides [15][16][17] and hydroxides 18 have been synthesized to date. Experimental study of 2D magnetic layers shows the Cr-based layers have FM state with large spin magnetic moment (≥3 μ B ) 19 .…”