Role of topotactic hydrogen in Superconductivity of Infinite-layer Nickelate NdNiO$_{2}$: A first-principles and variational Monte Carlo study

TL;DR

This study combines first-principles calculations and variational Monte Carlo methods to investigate how hydrogenation affects the electronic structure and superconductivity in NdNiO₂, revealing that hydrogen influences interstitial orbitals and the two-gap superconductivity.

Contribution

It provides a detailed first-principles and many-body analysis of hydrogen's role in modifying the electronic and superconducting properties of NdNiO₂, highlighting the impact on interstitial orbitals and superconducting gaps.

Findings

Hydrogen alters the Wannier functions and suppresses the electron pocket at the $k_z$ = $\pi$ Fermi surface.

Superconductivity involves two overlapping domes from different orbitals, with hydrogen strengthening the interstitial orbital contribution.

The two-band model remains valid even with hydrogenation, indicating robustness of the electronic structure features.

Abstract

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.