Datenpaket: Soft Mode Origin of Charge Ordering in Superconducting Kagome CsV₃Sb₅

Charge-density-wave (CDW) order and superconductivity coexist in the kagome metals AV₃Sb₅~(A=K, Cs, Rb), raising fundamental questions about the mechanisms driving their intertwined phases. Here we combine high-resolution inelastic X-ray scattering with first-principles calculations to uncover the origin of CDW formation in CsV₃Sb₅. Guided by structure factor analysis, we identify a soft phonon mode along the reciprocal $\textit{M}-\textit{L}$ direction, with the strongest effect at the $\textit{L}$ point, where the elastic scattering intensity also grows most rapidly upon cooling. First-principles calculations incorporating lattice anharmonicity and electron-phonon coupling reproduce these observations and establish a soft-mode instability at the $\textit{L}$ point as the driving mechanism of CDW formation. Despite the weakly first-order character of the transition, our results unambiguously demonstrate that the CDW in CsV₃Sb₅ originates from a softened phonon, clarifying its microscopic origin and highlighting the central role of lattice dynamics in kagome metals.

Charge-density-wave (CDW) order and superconductivity coexist in the kagome metals AV₃Sb₅~(A=K, Cs, Rb), raising fundamental questions about the mechanisms driving their intertwined phases. Here we combine high-resolution inelastic X-ray scattering with first-principles calculations to uncover the origin of CDW formation in CsV₃Sb₅. Guided by structure factor analysis, we identify a soft phonon mode along the reciprocal $\textit{M}-\textit{L}$ direction, with the strongest effect at the $\textit{L}$ point, where the elastic scattering intensity also grows most rapidly upon cooling. First-principles calculations incorporating lattice anharmonicity and electron-phonon coupling reproduce these observations and establish a soft-mode instability at the $\textit{L}$ point as the driving mechanism of CDW formation. Despite the weakly first-order character of the transition, our results unambiguously demonstrate that the CDW in CsV₃Sb₅ originates from a softened phonon, clarifying its microscopic origin and highlighting the central role of lattice dynamics in kagome metals.

Figure 1:
Calculation results on reasonable request
Figure 2:
Find the raw data in ESRF DS
Figure 3:
Find the raw data in RIKEN IXS: a,b,d,f --> A06; c,e --> A38
Figure 4:
Find the raw data in RIKEN IXS (A06)
Calculation results on reasonable request
Figure 5:
Find the raw data in RIKEN IXS (A06)
Calculation results on reasonable request
Figure S1:
Calculation results on reasonable request
Figure S2:
Calculation results on reasonable request
Figure S3:
Calculation results on reasonable request
Figure S4:
Find the raw data in ESRF IXS --> timescan in spec document, a cryostream was used
Figure S5:
Find the raw data in RIKEN IXS (A06)
Figure S6:
Find the raw data in RIKEN IXS (A06)
Figure S7:
Find the raw data in RIKEN IXS (A06)
Figure S8:
Find the raw data in ESRF DS
Figure S9:
Find the raw data in ESRF IXS (A2)
Figure S10:
Calculation results on reasonable request