Deviatoric stress-induced metallization, layer reconstruction and collapse of van der Waals bonded zirconium disulfide

In contrast to two-dimensional (2D) monolayer materials, van der Waals layered transition metal dichalcogenides exhibit rich polymorphism, making them promising candidates for novel superconductor, topological insulators and electrochemical catalysts. Here, we highlight the role of hydrostatic pressure on the evolution of electronic and crystal structures of layered ZrS2. Under deviatoric stress, our electrical experiments demonstrate a semiconductor-to-metal transition above 30.2 GPa, while quasi-hydrostatic compression postponed the metallization to 38.9 GPa. Both X-ray diffraction and Raman results reveal structural phase transitions different from those under hydrostatic pressure. Under deviatoric stress, ZrS2 rearranges the original ZrS6 octahedra into ZrS8 cuboids at 5.5 GPa, in which the unique cuboids coordination of Zr atoms is thermodynamically metastable. The structure collapses to a partially disordered phase at 17.4 GPa. These complex phase transitions present the importance of deviatoric stress on the highly tunable electronic properties of ZrS2 with possible implications for optoelectronic devices.. Authors: Yang, Linfei [Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China); Jingdezhen Ceramic University, Jiangxi (China); OSTI]; Li, Junwei [Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China)]; Zhang, Dongzhou [Univ. of Hawaii at Manoa, Honolulu, HI (United States)] (ORCID:000000026679892X); Liu, Yuegao [Chinese Academy of Sciences (CAS), Sanya (China). Institute of Deep-sea Science and Engineering]; Hu, Qingyang [Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China); Shanghai Advanced Research in Physical Sciences (SHARPS), Shanghai (China)] (ORCID:0000000227423017). DOE Contract: FG02-94ER14466. Subjects: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; electronic materials; solid-state chemistry; two-dimensional materials