Role of Sb in the superconducting kagome metal CsV$_3$Sb$_5$ revealed by its anisotropic compression

Abstract: Pressure evolution of the superconducting kagome metal CsV$_3$Sb$_5$ is studied with single-crystal x-ray diffraction and density-functional band-structure calculations. A highly anisotropic compression observed up to 5 GPa is ascribed to the fast shrinkage of the Cs-Sb distances and suppression of Cs rattling motion. This prevents Sb displacements required to stabilize the three-dimensional charge-density-wave (CDW) order and elucidates the disappearance of the CDW already at 2 GPa despite only minor changes in the electronic structure of the normal state. At higher pressures, vanadium bands still change only marginally, whereas antimony bands undergo a major reconstruction caused by the gradual formation of the interlayer Sb-Sb bonds. Our results exclude pressure tuning of vanadium kagome bands as the main mechanism for the non-trivial evolution of superconductivity in real-world kagome metals. Concurrently, we establish the central role of Sb atoms in the stabilization of a three-dimensional CDW and Fermi surface reconstruction.