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Bismuth compounds; Charge density; Charge density waves; Chemical bonds; Crystal structure; Degrees of freedom (mechanics); Density functional theory; Scaffolds; Selenium compounds; 1-D models; Bulk compounds; Bulk crystals; Bulk single crystals; Chemical bondings; Chemical concepts; One-dimensional (1D) system; One-dimensional physics; Peierls distortion; Property; article; charge density; chemical binding; controlled study; crystal structure; density functional theory; dimerization; environmental temperature; nonhuman; structure analysis; X ray diffraction; Iridium compounds
Abstract:
One-dimensional (1D) systems persist as some of the most interesting because of the rich physics that emerges from constrained degrees of freedom. A desirable route to harness the properties therein is to grow bulk single crystals of a physically three-dimensional (3D) but electronically 1D compound. Most bulk compounds which approach the electronic 1D limit still field interactions across the other two crystallographic directions and, consequently, deviate from the 1D models. In this paper, we lay out chemical concepts to realize the physics of 1D models in 3D crystals. These are based on both structural and electronic arguments. We present BiIr4Se8, a bulk crystal consisting of linear Bi2+ chains within a scaffolding of IrSe6 octahedra, as a prime example. Through crystal structure analysis, density functional theory calculations, X-ray diffraction, and physical property measurements, we demonstrate the unique 1D electronic configuration in BiIr4Se8. This configuration at ambient temperature is a gapped Su-Schriefer-Heeger system, generated by way of a canonical Peierls distortion involving Bi dimerization that relieves instabilities in a 1D metallic state. At 190 K, an additional 1D charge density wave distortion emerges, which affects the Peierls distortion. The experimental evidence validates our design principles and distinguishes BiIr4Se8 among other quasi-1D bulk compounds. We thus show that it is possible to realize unique electronically 1D materials applying chemical concepts. © 2024 American Chemical Society.
