Origin of competing charge density waves in kagome metal ScV<sub>6</sub>Sn<sub>6</sub>.

Wang, Kang; Chen, Siyu; Kim, Sun-Woo; Monserrat, Bartomeu · Nat Commun · 2024

basic_science · Level V

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Abstract

Understanding competing charge density wave (CDW) orders in the bilayer kagome metal ScV<sub>6</sub>Sn<sub>6</sub> remains challenging. Experimentally, upon cooling, short-range order with wave vector <math xmlns="http://www.w3.org/1998/Math/MathML"> <msub><mrow><mi>q</mi></mrow> <mrow><mn>2</mn></mrow> </msub> <mo>=</mo> <mrow><mo>(</mo> <mrow> <mfrac><mrow><mn>1</mn></mrow> <mrow><mn>3</mn></mrow> </mfrac> <mo>,</mo> <mfrac><mrow><mn>1</mn></mrow> <mrow><mn>3</mn></mrow> </mfrac> <mo>,</mo> <mfrac><mrow><mn>1</mn></mrow> <mrow><mn>2</mn></mrow> </mfrac> </mrow> <mo>)</mo></mrow> </math> forms, which is subsequently suppressed by the condensation of long-range <math xmlns="http://www.w3.org/1998/Math/MathML"> <msub><mrow><mi>q</mi></mrow> <mrow><mn>3</mn></mrow> </msub> <mo>=</mo> <mrow><mo>(</mo> <mrow> <mfrac><mrow><mn>1</mn></mrow> <mrow><mn>3</mn></mrow> </mfrac> <mo>,</mo> <mfrac><mrow><mn>1</mn></mrow> <mrow><mn>3</mn></mrow> </mfrac> <mo>,</mo> <mfrac><mrow><mn>1</mn></mrow> <mrow><mn>3</mn></mrow> </mfrac> </mrow> <mo>)</mo></mrow> </math> CDW order at lower temperature. Theoretically, however, the q<sub>2</sub> CDW is predicted as the ground state, leaving the CDW mechanism elusive. Here, using anharmonic phonon-phonon calculations combined with density functional theory, we predict a temperature-driven structural phase transitions from the high-temperature pristine phase to the q<sub>2</sub> CDW, followed by the low-temperature q<sub>3</sub> CDW, explaining experimental observations. We demonstrate that semi-core electron states stabilize the q<sub>3</sub> CDW over the q<sub>2</sub> CDW. Furthermore, we find that the out-of-plane lattice parameter controls the competing CDWs, motivating us to propose compressive bi-axial strain as an experimental protocol to stabilize the q<sub>2</sub> CDW. Finally, we suggest Ge or Pb doping at the Sn site as another potential avenue to control CDW instabilities. Our work provides a full theory of CDWs in ScV<sub>6</sub>Sn<sub>6</sub>, rationalizing experimental observations and resolving earlier discrepancies between theory and experiment.