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Title: Defect energetics of cubic hafnia from quantum Monte Carlo simulations

Journal Article · · Physical Review Materials
 [1];  [1];  [1];  [2]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern-Argonne Institute for Science and Engineering, Evanston, IL (United States)

Cubic hafnia (HfO2) is of great interest for a number of applications in electronics because of its high dielectric constant. However, common defects in such applications degrade the properties of hafina. We have investigated the electronic properties of oxygen vacancies and nitrogen substitution in cubic HfO2 using first-principles calculations based on density functional theory (DFT) and many-body diffusion Monte Carlo (DMC) methods. We investigate five different charge defect states of oxygen vacancies, as well as substitutional N defects which can lead to local magnetic moments. Both DMC and DFT calculations shows that an oxygen vacancy induces strong lattice relaxations around the defect. Finally, we compare defect formation energies, charge and spin densities obtained from DMC with results obtained using DFT. While the obtained formation energies from DMC are 0.6–1.5 eV larger than those from GGA+U, the agreement for the most important defects, neutral and positively charged oxygen vacancies, and nitrogen substitutional defect, under oxygen-poor conditions are in reasonably good agreement. Lastly, our work confirms that nitrogen can act to passivate cubic hafnia for applications in electronics.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1545380
Alternate ID(s):
OSTI ID: 1545423; OSTI ID: 1558516
Journal Information:
Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 7 Vol. 3; ISSN PRMHAR; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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