Superconductivity in Te-deficient ZrTe$_2$

Abstract

We present structural, electrical, and thermoelectric potential measurements on high-quality single crystals of ZrTe$_{1.8}$ grown from isothermal chemical vapor transport. These measurements show that the Te-deficient ZrTe$_{1.8}$, which forms the same structure as the non-superconducting ZrTe$_2$, is superconducting below 3.2\,K. The temperature dependence of the upper critical field (H$_{c2}$) deviates from the behavior expected in conventional single-band superconductors, being best described by an electron-phonon two-gap superconducting model with strong intraband coupling. For the ZrTe$_{1.8}$ single crystals, the Seebeck potential measurements suggest that the charge carriers are predominantly negative, in agreement with the ab initio calculations. Through first-principles calculations within DFT, we show that the slight reduction of Te occupancy in ZrTe$_2$ unexpectedly gives origin to density of states peaks at the Fermi level due to the formation of localized Zr-$d$ bands, possibly promoting electronic instabilities at the Fermi level and an increase at the critical temperature according to the standard BCS theory. These findings highlight that the Te deficiency promotes the electronic conditions for the stability of the superconducting ground state, suggesting that defects can fine-tune the electronic structure to support superconductivity.