The search for intrinsic excitonic insulators (EI) has long been confounded by coexisting electron-phonon coupling in bulk materials. Although the ground state of an EI may be difficult to differentiate from density-wave orders or other structural instabilities, excited states offer distinctive signatures. One way to provide clarity is to directly inspect the phonon spectral function for long wavelength broadening due to phonon interaction with the high velocity EI phason. Here, we report that the quasi-one-dimensional (quasi-1D) EI candidate Ta2NiSe5 shows extremely anisotropic phonon broadening and softening in the semimetallic normal state. In contrast, such a behavior is completely absent in the broken symmetry state of Ta2NiSe5 and in the isostructural Ta2NiS5, where the latter has a fully gapped normal state. By contrasting the expected phonon lifetimes in the BCS and BEC limits of a putative EI, our results suggest that the phase transition in Ta2Ni(Se,S)5 family is closely related to strong interband electron-phonon coupling. We experimentally determine the dimensionless coupling ω0g∼10, showing Ta2Ni(Se,S)5 as a rare "ultra-strong coupling" material.
@article{arxiv.2509.09620,
title = {Strong long-wavelength electron-phonon coupling in Ta$_2$Ni(Se,S)$_5$},
author = {Zhibo Kang and Burak Gurlek and Weichen Tang and Xiang Chen and Jacob P. C. Ruff and Ahmet Alatas and Ayman Said and Robert J. Birgeneau and Steven G. Louie and Angel Rubio and Simone Latini and Yu He},
journal= {arXiv preprint arXiv:2509.09620},
year = {2026}
}