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Recently, kagome lattice materials have emerged as a new model material platform for discovering and engineering novel quantum phases of matter. In this work, we elucidate the driving mechanism of the$$\sqrt{{{3}}}$$$\sqrt{3}$×$$\sqrt{{{3}}}$$$\sqrt{3}$charge order in a newly discovered kagome metal ScV₆Sn₆. Through multimodal investigations combining angle-resolved photoemission spectroscopy, phonon dispersion calculations, and phase diagram study, we identify the central role of unstable planar Sn and Sc phonon modes, while the electronic instability and van Hove singularities originating from the V kagome lattice have a marginal influence. Our results highlight that the$$\sqrt{{{3}}}$$$\sqrt{3}$×$$\sqrt{{{3}}}$$$\sqrt{3}$charge order in ScV₆Sn₆is fundamentally distinguished from the electronically driven 2 × 2 charge order in the canonical kagome system AV₃Sb₅, uncovering a new mechanism to induce symmetry-breaking phase transition in kagome lattice materials.

 

Electron-hole bound pairs, or excitons, are common excitations in semiconductors. They can spontaneously form and condense into a new insulating ground state—the so-called excitonic insulator—when the energy of electron-hole Coulomb attraction exceeds the band gap. In the presence of electron-phonon coupling, a periodic lattice distortion often concomitantly occurs. However, a similar structural transition can also be induced by electron-phonon coupling itself, therefore hindering the clean identification of bulk excitonic insulators (e.g., which instability is the driving force of the phase transition). Using high-resolution synchrotron x-ray diffraction and angle-resolved photoemission spectroscopy, we identify key electron-phonon coupling effects in a leading excitonic insulator candidate Ta 2 NiSe 5 . These include an extensive unidirectional lattice fluctuation and an electronic pseudogap in the normal state, as well as a negative electronic compressibility in the charge-doped broken-symmetry state. In combination with first principles and model calculations, we use the normal state electronic spectra to quantitatively determine the electron-phonon interaction vertex g and interband Coulomb interaction V in the minimal lattice model, the solution to which captures the experimental observations. Moreover, we show how the Coulomb and electron-phonon coupling effects can be unambiguously separated based on the solution to quantified microscopic models. Finally, we discuss how the strong lattice fluctuations enabled by low dimensionality relate to the unique electron-phonon interaction effects beyond the textbook Born-Oppenheimer approximation. 

During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators – an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta₂Ni(Se,S)₅. A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta₂NiSe₅, but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems.

 

Transition metal dichalcogenide heterostructures show strong interactions and can imprint a moiré potential to a separate layer.