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Orbital and spin character of doped carriers in infinite-layer nickelates

M. Rossi1, H. Lu1,2, A. Nag3, D. Li1,4, M. Osada1,5, K. Lee1,2, B. Y. Wang1,2, S. Agrestini3, M. Garcia-Fernandez3 et al.

J. J. Kas6,1, Y.-D. Chuang7, Z. X. Shen1,2,4,8, H. Y. Hwang1,4,8, B. Moritz1, Ke-Jin Zhou3, T. P. Devereaux1,5,8,*, and W. S. Lee1,†

  • 1Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA
  • 2Department of Physics, Stanford University, Stanford, California 94305, USA
  • 3Diamond Light Source, Harwell Campus, Didcot OX11 0DE, United Kingdom
  • 4Department of Applied Physics, Stanford University, Stanford, California 94305, USA
  • 5Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, USA
  • 6Department of Physics, University of Washington, Seattle, Washington 98195, USA
  • 7Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, MS 6-2100, Berkeley, California 94720, USA
  • 8Geballe Laboratory for Advanced Materials, Stanford University, Stanford, California 94305, USA

  • *Corresponding author: tpd@stanford.edu
  • †Corresponding author: leews@stanford.edu

Phys. Rev. B 104, L220505 – Published 8 December, 2021

DOI: https://doi.org/10.1103/PhysRevB.104.L220505

Abstract

The recent discovery of superconductivity in Nd1−xSrxNiO2 has drawn significant attention in the field. A key open question regards the evolution of the electronic structure with respect to hole doping. Here we exploit x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) to probe the doping-dependent electronic structure of Nd1−xSrxNiO2. Upon doping, a high-energy feature in Ni L3-edge XAS develops in addition to the main absorption peak, while XAS at the O K-, Nd M3- and Nd M5-edge exhibits a much weaker response. This implies that doped holes are mainly introduced into Ni 3d states. By comparing our data to atomic multiplet calculations including D4h crystal field, the doping-induced feature in Ni L3-edge XAS is consistent with a d8 spin-singlet state in which doped holes reside in the 3dx2−y2 orbitals. This is further supported by the softening of RIXS orbital excitations due to doping, corroborating with the Fermi level shift associated with increasing holes in the Ni 3dx2−y2 orbital.

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