First-principles insights into hyperfine parameters in the pristine and Ta-probed monoclinic hafnia.
Saved in:
| Title: | First-principles insights into hyperfine parameters in the pristine and Ta-probed monoclinic hafnia. |
|---|---|
| Authors: | Pathak, Santanu1,2 (AUTHOR), Das, Parnika1,2 (AUTHOR) parnika@vecc.gov.in, Das, Tilak3 (AUTHOR) tilak.das@phy.iitkgp.ac.in |
| Source: | Applied Physics A: Materials Science & Processing. Aug2025, Vol. 131 Issue 8, p1-16. 16p. |
| Subjects: | Hyperfine interactions, Hafnium oxide, Spin-spin interactions, Tantalum, Oxygen vacancy, Point defects, Nuclear quadrupole resonance |
| Abstract: | Effect on Hyperfine Interactions (HFI) parameters in presence of point-defects made out of oxygen vacancies and or Tantalum (Ta) substitutions at the Hafnium (Hf) site in the monoclinic hafnia (m-HfO ) is proposed. The scope of the study is to better understand the microscopic origin of the nuclear quadrupole character (i.e., local crystal structure and dynamics of lattices) in m-HfO through the systematic computational study of HFI parameters. Thus, an attempt based on the first-principles electronic structure calculations and on-site Hubbard U (self-consistent, ) is proposed herein, to evaluate the correlation of dipolar effects (spin-spin and spin-nuclear interactions) on the estimated electric quadrupolar parameters, so called HFI parameters of the host and probe nuclei in m-HfO . The measure of quadropolar parameters through the calculations of electric-field gradient (EFG) and associated asymmetric, and quadrupole frequencies, are thus, undertaken in this study in the pristine and also point-defects (single Ta substitution at Hf-site and oxygen vacancy) included m-HfO . Charged () or neutral () point-defects induced additional dipole-dipole interactions, play a critical role in the estimation of the EFG component, at the metal sites pertaining to the singlet or triplet spin-centre in the host m-HfO . Our results are discussed in comparison with the known Time Differential Perturbed Angular Correlation (TDPAC) data. Observations from the spin-densities and electronic structure modulation due to point-defects are crucial to explain anomalies of the current estimated and earlier known at the Ta-probe site from TDPAC measurements in reference to the host lattice Hf-sites. Spin-orbital effects are marginal on the estimated HFI parameters. The observation of spin-spin and spin-nuclear interactions in current binary oxide through HFI parameters determination may provide a rational implication in structural dynamics for other similar oxides. [ABSTRACT FROM AUTHOR] |
| Copyright of Applied Physics A: Materials Science & Processing is the property of Springer Nature and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
| Database: | Engineering Source |
|
Full text is not displayed to guests.
Login for full access.
|
|
| Abstract: | Effect on Hyperfine Interactions (HFI) parameters in presence of point-defects made out of oxygen vacancies and or Tantalum (Ta) substitutions at the Hafnium (Hf) site in the monoclinic hafnia (m-HfO ) is proposed. The scope of the study is to better understand the microscopic origin of the nuclear quadrupole character (i.e., local crystal structure and dynamics of lattices) in m-HfO through the systematic computational study of HFI parameters. Thus, an attempt based on the first-principles electronic structure calculations and on-site Hubbard U (self-consistent, ) is proposed herein, to evaluate the correlation of dipolar effects (spin-spin and spin-nuclear interactions) on the estimated electric quadrupolar parameters, so called HFI parameters of the host and probe nuclei in m-HfO . The measure of quadropolar parameters through the calculations of electric-field gradient (EFG) and associated asymmetric, and quadrupole frequencies, are thus, undertaken in this study in the pristine and also point-defects (single Ta substitution at Hf-site and oxygen vacancy) included m-HfO . Charged () or neutral () point-defects induced additional dipole-dipole interactions, play a critical role in the estimation of the EFG component, at the metal sites pertaining to the singlet or triplet spin-centre in the host m-HfO . Our results are discussed in comparison with the known Time Differential Perturbed Angular Correlation (TDPAC) data. Observations from the spin-densities and electronic structure modulation due to point-defects are crucial to explain anomalies of the current estimated and earlier known at the Ta-probe site from TDPAC measurements in reference to the host lattice Hf-sites. Spin-orbital effects are marginal on the estimated HFI parameters. The observation of spin-spin and spin-nuclear interactions in current binary oxide through HFI parameters determination may provide a rational implication in structural dynamics for other similar oxides. [ABSTRACT FROM AUTHOR] |
|---|---|
| ISSN: | 09478396 |
| DOI: | 10.1007/s00339-025-08769-4 |
