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First-principles study of the electronic and optical properties of Ho$_{\rm W}$ impurities in tungsten disulfide

The electronic and optical properties of single-layer (SL) tungsten disulfide (WS$_2$) in the presence of substitutional Holmium impurities (Ho$_{\rm W}$) are studied. Although Ho is much larger than W, density functional theory (DFT) including spin-orbit coupling is used to show that Ho:SL WS$_2$ is stable. The magnetic moment of the Ho impurity is found to be 4.75$μ_B$ using spin-dependent DFT. The optical selection rules identified in the optical spectrum match exactly the optical selection rules derived by means of group theory. The presence of neutral Ho$_W$ impurities gives rise to localized impurity states (LIS) with f-orbital character in the band structure. Using the Kubo-Greenwood formula and Kohn-Sham orbitals we obtain atom-like sharp transitions in the in-plane and out-of-plane components of the susceptibility tensor, Im$χ_{\parallel}$ and Im$χ_{\perp}$. The optical resonances are in good agreement with experimental data.