Role of on-site Coulomb energy and negative-charge transfer in a Dirac semi-metal NiTe${}_2$

Abstract

Angle-resolved photoemission spectroscopy (ARPES) combined with band structure calculations have shown that the layered transition metal dichalcogenide(TMD) NiTe${}_2$ is a type-II Dirac semimetal. However, conflicting conclusions were reported regarding the role of electron correlations in NiTe${}_2$. We study core-levels and valence band electronic structure of single crystal NiTe${}_2$ using soft and hard x-ray photoemission spectroscopy(SXPES, HAXPES), X-ray absorption spectroscopy(XAS) and Ni $2p-3d$ Resonant-PES to quantify electronic parameters in NiTe${}_2$. The Ni $3d$ on-site Coulomb energy ($U_{dd}$) is quantified from measurements of the Ni $3d$ single particle density of states(DOS) and the two-hole correlation satellite. The Ni $2p$ core level and $L$-edge XAS spectra are analyzed by charge-transfer (CT) cluster model calculations using the experimental $U_{dd}$, and it shows that NiTe${}_2$ exhibits a negative CT energy $\hat{I}”$. A comparative analysis of NiO $L$-edge XAS confirms its well-known strongly correlated CT insulator character, with a larger $U_{dd}$ and positive $\hat{I}”$. The $d$-$p$ hybridization strength $T_{eg}$ for NiTe${}_2$$<$NiO, and shows that $T_{eg}$ is not responsible for reducing $U_{dd}$ in NiTe\textsubscript{2} compared to NiO. The negative-$\hat{I}”$ and a reduced $U_{dd}$ leads to the increase in $d^n$ count on the Ni site in NiTe${}_2$ by nearly one electron. However, importantly, since $U_{dd}$$>$$|\hat{I}”|$, a finite repulsive $U_{dd}$ results in pushing $d$-states away from Fermi level and this is required to make NiTe${}_2$ a moderately correlated Dirac semi-metal with band inversion in the $p$-$p$ type lowest energy excitations.

13 pages, 13 figures (Revised version submitted to Physical Review B);typos corrected