Atomistic Origin of Diverse Charge Density Wave States in CsV3Sb5

Kagome metals AV₃Sb₅ (A=K, Rb, or Cs) exhibit intriguing charge density wave (CDW) instabilities, which interplay with superconductivity and band topology. However, despite firm observations, the atomistic origins of the CDW phases, as well as hidden instabilities, remain elusive. Here, we adopt our newly developed symmetry-adapted cluster expansion method to construct a first-principles-based effective Hamiltonian of CsV₃Sb₅, which not only reproduces the established inverse star of David (ISD) phase, but also predict a series of D₃ₕ-n states under mild tensile strains. With such atomistic Hamiltonians, the microscopic origins of different CDW states are revealed as the competition of the second-nearest neighbor V-V pairs versus the first-nearest neighbor V-V and V-Sb couplings. Interestingly, the effective Hamiltonians also reveal the existence of ionic Dzyaloshinskii-Moriya interaction in the high-symmetry phase of CsV₃Sb₅ and drives the formation of noncollinear CDW patterns. Our work thus not only deepens the understanding of the CDW formation in AV₃Sb₅, but also demonstrates that the effective Hamiltonian is a suitable approach for investigating CDW mechanisms, which can be extended to various CDW systems.