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arxiv 2506.13399 v1 pith:3EXT55XJ submitted 2025-06-16 cond-mat.supr-con cond-mat.mtrl-scicond-mat.str-el

Role of topotactic hydrogen in Superconductivity of Infinite-layer Nickelate NdNiO₂: A first-principles and variational Monte Carlo study

classification cond-mat.supr-con cond-mat.mtrl-scicond-mat.str-el
keywords arisinghydrogenmodelcarlofirst-principleshydrogenationinfinite-layerinterstitial
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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Employing combination of first-principles calculations, low-energy model construction, and variational Monte Carlo solution of the ab-initio derived Hubbard model, we study the effect of hydrogenation in the electronic structure and superconducting properties of infinite-layer nickelate, NdNiO$_2$. We find that the introduction of hydrogen at the apical oxygen vacancy position strongly influences the Wannier function corresponding to the effective interstitial orbital at the Ni site bound to the hydrogen. This results in the near disappearance of the electron pocket at the $k_z$ = $\pi$ Fermi surface, keeping that of $k_z$ = 0 unchanged, compared to the dehydrogenated case. The two-band model thus remains valid even in the presence of H. The calculated superconducting order parameters both in absence and presence of H, show a two-hump superconductivity arising the two overlapping domes, one arising from $d_{x^{2}-y^{2}}$ and another arising from interstitial orbital degree of freedom. Hydrogenation strengthens the latter, marginally affecting the former.

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