Magnetic Ni-N-Ni Centers in N-substituted NiO

Godin, Simon; Elfimov, Ilya S.; Li, Fengmiao; Davidson, Bruce A.; Sutarto, Ronny; Denlinger, Jonathan D.; Tjeng, Liu Hao; Sawatzky, George A.; Zou, Ke

doi:10.1103/mp1d-jg6c

Magnetic Ni-N-Ni Centers in N-substituted NiO

Journal Article · Thu Jul 24 00:00:00 EDT 2025 · Physical Review Letters

DOI:https://doi.org/10.1103/mp1d-jg6c· OSTI ID:3007108

^[1]; ^[1]; ^[1]; ^[1]; ^[2]; ^[3]; ^[4]; ^[1]; ^[1]

Univ. of British Columbia, Vancouver, BC (Canada)
Univ. of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Max Planck Institute for Chemical Physics of Solids, Dresden (Germany)

Here, to explore how anion substitution modifies the existing magnetism in strongly correlated oxides, we investigate local electronic states and magnetic ordering in nickel oxide (NiO) induced by substituting oxygen (O) with nitrogen (N). Each N introduces an additional N 2p hole and modifies the magnetic moment of a neighboring nickel (Ni) cation site, as the exchange interaction between this hole and the Ni $$e_{g}$$ electrons exceeds the Ni-O-Ni superexchange interaction. This leads to the formation of Ni-N-Ni centers consisting of five spins, without perturbing the antiferromagnetic NiO lattice. These centers are studied using density functional theory and confirmed through high-resolution spectroscopy on N-substituted NiO thin films grown by molecular beam epitaxy. This type of magnetic design may enable future advances in quantum technologies based on strongly correlated materials, such as quantum sensors and spin-based qubits.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 3007108

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 4 Vol. 135; ISSN 1079-7114; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (50)

Practical methods for background subtraction in photoemission spectra: Practical methods for background subtraction in photoemission spectra Herrera-Gomez, A.; Bravo-Sanchez, M.; Ceballos-Sanchez, O. Surface and Interface Analysis, Vol. 46, Issue 10-11 https://doi.org/10.1002/sia.5453	journal	March 2014
Differences between L3 and L2 X-ray absorption spectra de Groot, F. M. F. Physica B: Condensed Matter, Vol. 208-209 https://doi.org/10.1016/0921-4526(94)00817-F	journal	March 1995
Comparison of the superexchange interaction in NiO and in a NiO[100] surface de Graaf, C.; Broer, R.; Nieuwpoort, W. C. Chemical Physics Letters, Vol. 271, Issue 4-6 https://doi.org/10.1016/S0009-2614(97)00457-0	journal	June 1997
Study of reactively sputtered nickel nitride thin films Pandey, Nidhi; Gupta, Mukul; Stahn, Jochen Journal of Alloys and Compounds, Vol. 851 https://doi.org/10.1016/j.jallcom.2020.156299	journal	January 2021
Magnetic linear dichroism studies of in situ grown NiO thin films Krishnakumar, S. R.; Liberati, M.; Grazioli, C. Journal of Magnetism and Magnetic Materials, Vol. 310, Issue 1 https://doi.org/10.1016/j.jmmm.2006.07.020	journal	March 2007
High performance of Co-doped NiO nanoparticle anode material for rechargeable lithium ion batteries Thi, Trang Vu; Rai, Alok Kumar; Gim, Jihyeon Journal of Power Sources, Vol. 292 https://doi.org/10.1016/j.jpowsour.2015.05.029	journal	October 2015
Nitrogen-doped nickel oxide thin films for enhanced electrochromic applications Lin, Feng; Gillaspie, Dane T.; Dillon, Anne C. Thin Solid Films, Vol. 527 https://doi.org/10.1016/j.tsf.2012.12.031	journal	January 2013
Heteroatom-Doped Transition Metal Electrocatalysts for Hydrogen Evolution Reaction Jin, Huanyu; Liu, Xin; Chen, Shuangming ACS Energy Letters, Vol. 4, Issue 4 https://doi.org/10.1021/acsenergylett.9b00348	journal	February 2019
Universal Surface Engineering of Transition Metals for Superior Electrocatalytic Hydrogen Evolution in Neutral Water You, Bo; Liu, Xuan; Hu, Guoxiang Journal of the American Chemical Society, Vol. 139, Issue 35 https://doi.org/10.1021/jacs.7b06434	journal	August 2017
High-sensitivity diamond magnetometer with nanoscale resolution Taylor, J. M.; Cappellaro, P.; Childress, L. Nature Physics, Vol. 4, Issue 10 https://doi.org/10.1038/nphys1075	journal	September 2008
Ultrafast coupled charge and spin dynamics in strongly correlated NiO Gillmeister, Konrad; Golež, Denis; Chiang, Cheng-Tien Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-17925-8	journal	August 2020
Spectroscopic capture of a low-spin Mn(IV)-oxo species in Ni–Mn3O4 nanoparticles during water oxidation catalysis Park, Sunghak; Jin, Kyoungsuk; Lim, Hyung Kyu Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19133-w	journal	October 2020
A quantum coherent spin in hexagonal boron nitride at ambient conditions Stern, Hannah L.; M. Gilardoni, Carmem; Gu, Qiushi Nature Materials, Vol. 23, Issue 10 https://doi.org/10.1038/s41563-024-01887-z	journal	May 2024
Optical observation of single spins in silicon Higginbottom, Daniel B.; Kurkjian, Alexander T. K.; Chartrand, Camille Nature, Vol. 607, Issue 7918 https://doi.org/10.1038/s41586-022-04821-y	journal	July 2022
Determination of total x-ray absorption coefficient using non-resonant x-ray emission Achkar, A. J.; Regier, T. Z.; Monkman, E. J. Scientific Reports, Vol. 1, Issue 1 https://doi.org/10.1038/srep00182	journal	December 2011
Number of Single, Double, and Triple Clusters in a System Containing Two Types of Atoms Behringer, Robert E. The Journal of Chemical Physics, Vol. 29, Issue 3 https://doi.org/10.1063/1.1744537	journal	September 1958
NO-assisted molecular-beam epitaxial growth of nitrogen substituted EuO Wicks, R.; Altendorf, S. G.; Caspers, C. Applied Physics Letters, Vol. 100, Issue 16 https://doi.org/10.1063/1.3701589	journal	April 2012
Structural and magnetic properties of N doped ZnO thin films Jindal, Kajal; Tomar, Monika; Katiyar, R. S. Journal of Applied Physics, Vol. 111, Issue 10 https://doi.org/10.1063/1.4714686	journal	May 2012
A method to stabilize the unreconstructed MgO (111) polar surface Godin, Simon; Davidson, Bruce A.; Sutarto, Ronny Applied Physics Letters, Vol. 121, Issue 6 https://doi.org/10.1063/5.0096334	journal	August 2022
Quantum computing with defects Weber, J. R.; Koehl, W. F.; Varley, J. B. Proceedings of the National Academy of Sciences, Vol. 107, Issue 19 https://doi.org/10.1073/pnas.1003052107	journal	April 2010
Magnon-mediated qubit coupling determined via dissipation measurements Fukami, Masaya; Marcks, Jonathan C.; Candido, Denis R. Proceedings of the National Academy of Sciences, Vol. 121, Issue 2 https://doi.org/10.1073/pnas.2313754120	journal	January 2024
Diamond quantum sensors: from physics to applications on condensed matter research Ho, Kin On; Shen, Yang; Pang, Yiu Yung Functional Diamond, Vol. 1, Issue 1 https://doi.org/10.1080/26941112.2021.1964926	journal	January 2021
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Advanced capabilities for materials modelling with Quantum ESPRESSO Giannozzi, P.; Andreussi, O.; Brumme, T. Journal of Physics: Condensed Matter, Vol. 29, Issue 46 https://doi.org/10.1088/1361-648X/aa8f79	journal	October 2017
Silicon-Integrated Telecommunications Photon-Spin Interface Bergeron, L.; Chartrand, C.; Kurkjian, A. T. K. PRX Quantum, Vol. 1, Issue 2 https://doi.org/10.1103/PRXQuantum.1.020301	journal	October 2020
Band theory of insulating transition-metal monoxides: Band-structure calculations Terakura, K.; Oguchi, T.; Williams, A. R. Physical Review B, Vol. 30, Issue 8 https://doi.org/10.1103/PhysRevB.30.4734	journal	October 1984
Electronic structure of NiO: Correlation and band effects Shen, Z. -X.; List, R. S.; Dessau, D. S. Physical Review B, Vol. 44, Issue 8 https://doi.org/10.1103/PhysRevB.44.3604	journal	August 1991
Band theory and Mott insulators: Hubbard U instead of Stoner I Anisimov, Vladimir I.; Zaanen, Jan; Andersen, Ole K. Physical Review B, Vol. 44, Issue 3, p. 943-954 https://doi.org/10.1103/PhysRevB.44.943	journal	July 1991
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Temperature and thickness dependence of magnetic moments in NiO epitaxial films Alders, D.; Tjeng, L. H.; Voogt, F. C. Physical Review B, Vol. 57, Issue 18 https://doi.org/10.1103/PhysRevB.57.11623	journal	May 1998
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
Measurement of Spin-Wave Dispersion in NiO by Inelastic Neutron Scattering and Its Relation to Magnetic Properties Hutchings, M. T.; Samuelsen, E. J. Physical Review B, Vol. 6, Issue 9 https://doi.org/10.1103/PhysRevB.6.3447	journal	November 1972
NO2-assisted molecular-beam epitaxy of wustitelike and magnetitelike Fe oxynitride films on MgO(100) Voogt, F. C.; Smulders, P. J. M.; Wijnja, G. H. Physical Review B, Vol. 63, Issue 12 https://doi.org/10.1103/PhysRevB.63.125409	journal	March 2001
Magnetic versus crystal-field linear dichroism in NiO thin films Haverkort, M. W.; Csiszar, S. I.; Hu, Z. Physical Review B, Vol. 69, Issue 2 https://doi.org/10.1103/PhysRevB.69.020408	journal	January 2004
Mechanism of ferromagnetism in nitrogen-doped ZnO: First-principle calculations Shen, L.; Wu, R. Q.; Pan, H. Physical Review B, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevB.78.073306	journal	August 2008
Intrinsic charge transfer gap in NiO from Ni K -edge x-ray absorption spectroscopy Gougoussis, C.; Calandra, M.; Seitsonen, A. Physical Review B, Vol. 79, Issue 4 https://doi.org/10.1103/PhysRevB.79.045118	journal	January 2009
Antiferromagnetic phase transition and spin correlations in NiO Chatterji, Tapan; McIntyre, G. J.; Lindgard, P. -A. Physical Review B, Vol. 79, Issue 17 https://doi.org/10.1103/PhysRevB.79.172403	journal	May 2009
First-principles calculations of x-ray absorption in a scheme based on ultrasoft pseudopotentials: From α -quartz to high- T c compounds Gougoussis, Christos; Calandra, Matteo; Seitsonen, Ari P. Physical Review B, Vol. 80, Issue 7 https://doi.org/10.1103/PhysRevB.80.075102	journal	August 2009
Three-dimensional spin orientation in antiferromagnetic domain walls of NiO studied by x-ray magnetic linear dichroism photoemission electron microscopy Arai, Kuniaki; Okuda, Taichi; Tanaka, Arata Physical Review B, Vol. 85, Issue 10 https://doi.org/10.1103/PhysRevB.85.104418	journal	March 2012
Band gaps and electronic structure of transition-metal compounds Zaanen, J.; Sawatzky, G. A.; Allen, J. W. Physical Review Letters, Vol. 55, Issue 4 https://doi.org/10.1103/PhysRevLett.55.418	journal	July 1985
Nonlocal screening effects in 2 p x-ray photoemission spectroscopy core-level line shapes of transition metal compounds van Veenendaal, M. A.; Sawatzky, G. A. Physical Review Letters, Vol. 70, Issue 16 https://doi.org/10.1103/PhysRevLett.70.2459	journal	April 1993
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Magnetic Dichroism and Spin Structure of Antiferromagnetic NiO(001) Films Altieri, S.; Finazzi, M.; Hsieh, H. H. Physical Review Letters, Vol. 91, Issue 13 https://doi.org/10.1103/PhysRevLett.91.137201	journal	September 2003
Magnetostrictive Domain Walls in Antiferromagnetic NiO Weber, N. B.; Ohldag, H.; Gomonaj, H. Physical Review Letters, Vol. 91, Issue 23 https://doi.org/10.1103/PhysRevLett.91.237205	journal	December 2003
Magnetizing Oxides by Substituting Nitrogen for Oxygen Elfimov, I. S.; Rusydi, A.; Csiszar, S. I. Physical Review Letters, Vol. 98, Issue 13 https://doi.org/10.1103/PhysRevLett.98.137202	journal	March 2007
NiO: Correlated Band Structure of a Charge-Transfer Insulator Kuneš, J.; Anisimov, V. I.; Skornyakov, S. L. Physical Review Letters, Vol. 99, Issue 15 https://doi.org/10.1103/PhysRevLett.99.156404	journal	October 2007
GenX : an extensible X-ray reflectivity refinement program utilizing differential evolution Björck, Matts; Andersson, Gabriella Journal of Applied Crystallography, Vol. 40, Issue 6 https://doi.org/10.1107/S0021889807045086	journal	November 2007
Vanadium spin qubits as telecom quantum emitters in silicon carbide Wolfowicz, Gary; Anderson, Christopher P.; Diler, Berk Science Advances, Vol. 6, Issue 18 https://doi.org/10.1126/sciadv.aaz1192	journal	May 2020
Influence of nitrogen doping on properties of NiO films Sriram, S.; Thayumanavan, A.; Ravichandran, K. Surface Engineering, Vol. 32, Issue 3 https://doi.org/10.1179/1743294414Y.0000000380	journal	March 2016
Importance of the Spin-Orbit Coupling for 3d-Ion Compounds: the Case of NiO Radwański, R. J.; Ropka, Z. Acta Physica Polonica A, Vol. 97, Issue 5 https://doi.org/10.12693/APhysPolA.97.963	journal	May 2000

Similar Records

Signatures of stripe phases in hole-doped La{sub 2}NiO{sub 4}

Journal Article · Wed Jul 01 00:00:00 EDT 1998 · Physical Review, B: Condensed Matter · OSTI ID:636186

Imaging Chemical Aggregation of Ni/NiO Particles from Reduced NiO-YSZ

Journal Article · Wed Jul 20 00:00:00 EDT 2011 · Electrochemical and Solid-State Letters · OSTI ID:1029067

Magnetic properties of La{sub 2}NiO{sub 4.16} and La{sub 2{minus}x}Pr{sub x}NiO{sub 4+{delta}}

Journal Article · Wed Jul 01 00:00:00 EDT 1998 · Journal of Solid State Chemistry · OSTI ID:651120

Magnetic Ni-N-Ni Centers in N-substituted NiO

Citation Formats

References (50)

Similar Records

Related Subjects