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Isolated hydrogen configurations in zirconia as seen by muon spin spectroscopy and ab initio calculations

Authors: R. B. L. Vieira; R. C. Vilão; A. G. Marinopoulos; P. M. Gordo; J. A. Paixão; H. V. Alberto; J. M. Gil; A. Weidinger; R. L. Lichti; B. Baker; P. W. Mengyan: J. S. Lord

Ref.: Phys. Rev. B 94, 115207(1)-115207(11) (2016)

Abstract: We present a systematic study of isolated hydrogen in diverse forms of ZrO2 (zirconia), both undoped and stabilized in the cubic phase by additions of transition-metal oxides (Y2O3, Sc2O3, MgO, CaO). Hydrogen is modeled by using muonium as a pseudoisotope in muon-spin spectroscopy experiments. The muon study is also supplemented with first-principles calculations of the hydrogen states in scandia-stabilized zirconia by conventional density-functional theory (DFT) as well as a hybrid-functional approach which admixes a portion of exact exchange to the semilocal DFT exchange. The experimentally observable metastable states accessible by means of the muon implantation allowed us to probe two distinct hydrogen configurations predicted theoretically: an oxygen-bound configuration and a quasiatomic interstitial one with a large isotropic hyperfine constant. The neutral-oxygen-bound configuration is characterized by an electron spreading over the neighboring zirconium cations, forming a polaronic state with a vanishingly small hyperfine interaction at the muon. The atom-like interstitial muonium is observed also in all samples but with different fractions. The hyperfine interaction is isotropic in calcia-doped zirconia [Aiso = 3.02(8) GHz], but slightly anisotropic in the nanograin yttria-doped zirconia [Aiso = 2.1(1) GHz, D = 0.13(2) GHz] probably due to muons stopping close to the interface regions between the nanograins in the latter case.

DOI: 10.1103/PhysRevB.94.115207

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