Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo5 Systems

Lamichhane, Tej N.; Onyszczak, Michael T.; Palasyuk, Olena; Sharikadze, Saba; Kim, Tae -Hoon; Lin, Qisheng; Kramer, Matthew J.; McCallum, R. W.; Wysocki, Aleksander L.; Nguyen, Manh Cuong; Antropov, Vladimir P.; Pandey, Tribhuwan; Parker, David; Bud’ko, Sergey L.; Canfield, Paul C.; Palasyuk, Andriy

doi:10.1103/PhysRevApplied.11.014052

Title: Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo₅ Systems

Journal Article · Fri Jan 25 00:00:00 EST 2019 · Physical Review Applied

DOI:https://doi.org/10.1103/PhysRevApplied.11.014052· OSTI ID:1494934

Lamichhane, Tej N. ^[1]; Onyszczak, Michael T. ^[2]; Palasyuk, Olena ^[1]; Sharikadze, Saba ^[2]; Kim, Tae -Hoon ^[1]; Lin, Qisheng ^[1]; Kramer, Matthew J. ^[1]; McCallum, R. W. ^[1]; Wysocki, Aleksander L. ^[1]; Nguyen, Manh Cuong ^[1]; Antropov, Vladimir P. ^[1]; Pandey, Tribhuwan ^[3]; Parker, David ^[3]; Bud’ko, Sergey L. ^[1]; Canfield, Paul C. ^[1]; Palasyuk, Andriy ^[1]

Ames Lab. and Iowa State Univ., Ames, IA (United States)
Iowa State Univ., Ames, IA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

To reduce material and processing costs of commercial permanent magnets and to attempt to fill the empty niche of energy products, 10–20 MGOe, between low-flux (ferrites, alnico) and high-flux (Nd₂Fe₁₄B- and SmCo₅-type) magnets, we report the synthesis, structure, magnetic properties, and modeling of Ta-, Cu-, and Fe-substituted CeCo₅. Using a self-flux technique, we grow single crystals of Ce_15.1Ta_1.0Co_74.4Cu_9.5, Ce_16.3Ta_0.6Co_68.9Cu_14.2, Ce_15.7Ta_0.6Co_67.8Cu_15.9, Ce_16.3Ta_0.3Co_61.7Cu_21.7, and Ce_14.3Ta_1.0Co_62.0Fe_12.3Cu_10.4. X-ray-diffraction analysis shows that these materials retain a CaCu₅ substructure and incorporate small amounts of Ta in the form of “dumbbells,” filling the 2e crystallographic sites within the one-dimensional hexagonal channel with the 1a Ce site, whereas Co, Cu, and Fe are statistically distributed among the 2c and 3g crystallographic sites. Scanning-electron-microscopy, energy-dispersive-x-ray-spectroscopy, and scanning-transmission-electron-microscopy examinations provide strong evidence of the single-phase nature of the as-grown crystals, even though they readily exhibit significant magnetic coercivities of approximately 1.6 kOe to approximately 1.8 kOe caused by Co-enriched, nanosized structural defects and faults that can serve as pinning sites. Heat treatments at 1040°C for 10 h and hardening at 400°C for 4 h lead to the formation of a so-called composite crystal with a bimodal microstructure that consists of a Ta-poor matrix and Ta-rich laminal precipitates. Formation of the composite crystal during the heat treatment creates a three-dimensional array of extended defects within a primarily single-grain single crystal, which greatly improves its magnetic characteristics. Possible causes for the formation of the composite crystal may be associated with Ta atoms leaving matrix interstices at lower temperatures and/or matrix degradation induced by decreased miscibility at lower temperatures. Furthermore Fe strongly increases both the Curie temperature and magnetization of the system resulting, in (BH)_max ≈ 13 MGOe at room temperature.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Ames Lab., Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1494934

Alternate ID(s):: OSTI ID: 1492120

Report Number(s):: IS-J-9882; PRAHB2

Journal Information:: Physical Review Applied, Vol. 11, Issue 1; ISSN 2331-7019

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (59)

Permanent magnets: Plugging the gap Coey, J. M. D. Scripta Materialia, Vol. 67, Issue 6 https://doi.org/10.1016/j.scriptamat.2012.04.036	journal	September 2012
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
Microstructure of a Cerium, Cobalt and Copper Alloy with a High Coercivity Senno, Harufumi; Tawara, Yoshio Japanese Journal of Applied Physics, Vol. 8, Issue 1 https://doi.org/10.1143/JJAP.8.118	journal	January 1969
Effect of Processing on Permanent Magnet Materials Containing Rare‐Earth Metals Nesbitt, E. A.; Chin, G. Y.; Sherwood, R. C. Journal of Applied Physics, Vol. 40, Issue 10 https://doi.org/10.1063/1.1657135	journal	September 1969
An empirical correction for absorption anisotropy Blessing, R. H. Acta Crystallographica Section A Foundations of Crystallography, Vol. 51, Issue 1 https://doi.org/10.1107/S0108767394005726	journal	January 1995
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
Local spin density functional approach to the theory of exchange interactions in ferromagnetic metals and alloys Liechtenstein, A. I.; Katsnelson, M. I.; Antropov, V. P. Journal of Magnetism and Magnetic Materials, Vol. 67, Issue 1 https://doi.org/10.1016/0304-8853(87)90721-9	journal	May 1987
Magnetocrystalline anisotropy in cobalt based magnets: a choice of correlation parameters and the relativistic effects Nguyen, Manh Cuong; Yao, Yongxin; Wang, Cai-Zhuang Journal of Physics: Condensed Matter, Vol. 30, Issue 19 https://doi.org/10.1088/1361-648X/aab9fa	journal	April 2018
Structural and magnetic properties of Nd ₂ Fe ₁ ₄ B (invited) Herbst, J. F.; Croat, J. J.; Yelon, W. B. Journal of Applied Physics, Vol. 57, Issue 8 https://doi.org/10.1063/1.334680	journal	April 1985
Influence of cerium content on the structure and magnetic behavior of Co-Fe-Cu-Ce permanent magnets Nesbitt, E.; Chin, G.; Sherwood, R. IEEE Transactions on Magnetics, Vol. 9, Issue 3 https://doi.org/10.1109/TMAG.1973.1067641	journal	September 1973
X-ray and neutron determination of a so-called Th2Ni17-type structure in the lutetium-iron system Givord, D.; Lemaire, R.; Moreau, J. M. Journal of the Less Common Metals, Vol. 29, Issue 4 https://doi.org/10.1016/0022-5088(72)90200-7	journal	December 1972
The structure of Co-Cu-Fe-Ce permanent magnets Leamy, H.; Green, M. IEEE Transactions on Magnetics, Vol. 9, Issue 3 https://doi.org/10.1109/TMAG.1973.1067642	journal	September 1973
Structural and magnetic properties of iron-rich compounds in the Yb–Fe–Ga system Tokaychuk, Ya. O.; Bodak, O. I.; Gorelenko, Yu. K. Journal of Alloys and Compounds, Vol. 415, Issue 1-2 https://doi.org/10.1016/j.jallcom.2005.07.044	journal	May 2006
Spin-Fluctuation Mechanism of Anomalous Temperature Dependence of Magnetocrystalline Anisotropy in Itinerant Magnets Zhuravlev, I. A.; Antropov, V. P.; Belashchenko, K. D. Physical Review Letters, Vol. 115, Issue 21 https://doi.org/10.1103/PhysRevLett.115.217201	journal	November 2015
Recent advances in magnetic structure determination by neutron powder diffraction Rodríguez-Carvajal, Juan Physica B: Condensed Matter, Vol. 192, Issue 1-2 https://doi.org/10.1016/0921-4526(93)90108-I	journal	October 1993
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
A critical review on solvent extraction of rare earths from aqueous solutions Xie, Feng; Zhang, Ting An; Dreisinger, David Minerals Engineering, Vol. 56 https://doi.org/10.1016/j.mineng.2013.10.021	journal	February 2014
Directional solidification of Co-Cu-R permanent-magnet alloys Chin, G.; Green, M.; Nesbitt, E. IEEE Transactions on Magnetics, Vol. 8, Issue 1 https://doi.org/10.1109/TMAG.1972.1067257	journal	March 1972
Intermetallic compounds in the cobalt-rich part of the R-cobalt systems (R = Ce, La, CeLa) Khan, Y. Journal of the Less Common Metals, Vol. 34, Issue 2 https://doi.org/10.1016/0022-5088(74)90159-3	journal	February 1974
Oxidation study of monocrystalline CeCo5−xCux by X-ray diffraction methods Labulle, B.; Petipas, C. Journal of the Less Common Metals, Vol. 71, Issue 2 https://doi.org/10.1016/0022-5088(80)90203-9	journal	June 1980
Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators Liechtenstein, A. I.; Anisimov, V. I.; Zaanen, J. Physical Review B, Vol. 52, Issue 8 https://doi.org/10.1103/PhysRevB.52.R5467	journal	August 1995
${Ce}_{3 - x} {Mg}_{x} {Co}_{9}$ : Transformation of a Pauli Paramagnet into a Strong Permanent Magnet Lamichhane, Tej N.; Taufour, Valentin; Palasyuk, Andriy Physical Review Applied, Vol. 9, Issue 2 https://doi.org/10.1103/PhysRevApplied.9.024023	journal	February 2018
Growth of single crystals from metallic fluxes Canfield, P. C.; Fisk, Z. Philosophical Magazine B, Vol. 65, Issue 6 https://doi.org/10.1080/13642819208215073	journal	June 1992
Prospects for Non-Rare Earth Permanent Magnets for Traction Motors and Generators Kramer, M. J.; McCallum, R. W.; Anderson, I. A. JOM, Vol. 64, Issue 7 https://doi.org/10.1007/s11837-012-0351-z	journal	June 2012
New Permanent Magnet Materials Nesbitt, E. A.; Willens, R. H.; Sherwood, R. C. Applied Physics Letters, Vol. 12, Issue 11 https://doi.org/10.1063/1.1651855	journal	June 1968
Cerium, Cobalt and Copper Alloy as a Permanent Magnet Material Tawara, Yoshio; Senno, Harufumi Japanese Journal of Applied Physics, Vol. 7, Issue 8 https://doi.org/10.1143/JJAP.7.966	journal	August 1968
Aspects of spin dynamics and magnetic interactions Antropov, V. P.; Harmon, B. N.; Smirnov, A. N. Journal of Magnetism and Magnetic Materials, Vol. 200, Issue 1-3 https://doi.org/10.1016/S0304-8853(99)00425-4	journal	October 1999
X-ray study of monocrystalline alloys near the composition CeCo3.5Cu1.5 Labulle, B.; Petipas, C. Journal of the Less Common Metals, Vol. 66, Issue 2 https://doi.org/10.1016/0022-5088(79)90228-5	journal	August 1979
Formation of TbCu7-type CeFe10Zr0.8 by rapid solidification Zhou, Chen; Pinkerton, Frederick E.; Herbst, Jan F. Journal of Alloys and Compounds, Vol. 569 https://doi.org/10.1016/j.jallcom.2013.03.175	journal	August 2013
Micromagnetic simulations with periodic boundary conditions: Hard-soft nanocomposites Wysocki, Aleksander L.; Antropov, Vladimir P. Journal of Magnetism and Magnetic Materials, Vol. 428 https://doi.org/10.1016/j.jmmm.2016.11.128	journal	April 2017
Rare earth-cobalt permanent magnets Strnat, Karl J.; Strnat, Reinhold M. W. Journal of Magnetism and Magnetic Materials, Vol. 100, Issue 1-3 https://doi.org/10.1016/0304-8853(91)90811-N	journal	November 1991
Phase equilibria in the CeCo5-CeCu5 system and structural characterization of the Ce(Co1−xCux)5 phases Girodin, D.; Allibert, C. H.; Givord, F. Journal of the Less Common Metals, Vol. 110, Issue 1-2 https://doi.org/10.1016/0022-5088(85)90316-9	journal	August 1985
Magnetic anisotropy and high-field magnetization process of CeCo5 Bartashevich, M. I.; Goto, T.; Radwanski, R. J. Journal of Magnetism and Magnetic Materials, Vol. 131, Issue 1-2 https://doi.org/10.1016/0304-8853(94)90010-8	journal	March 1994
Structural and magnetic properties of iron-rich compounds in the Yb–Fe–Al system Bodak, O.; Tokaychuk, Ya.; Manyako, M. Journal of Alloys and Compounds, Vol. 354, Issue 1-2 https://doi.org/10.1016/S0925-8388(02)01353-1	journal	May 2003
A study of the physical properties of single crystalline Fe5B2P Lamichhane, Tej N.; Taufour, Valentin; Thimmaiah, Srinivasa Journal of Magnetism and Magnetic Materials, Vol. 401 https://doi.org/10.1016/j.jmmm.2015.10.088	journal	March 2016
Permanent-magnet properties of Sm-Ce-Co-Fe-Cu alloys with compositions between 1-5 and 2-17 Senno, H.; Tawara, Y. IEEE Transactions on Magnetics, Vol. 10, Issue 2 https://doi.org/10.1109/TMAG.1974.1058334	journal	June 1974
Local atomic order in the vicinity of Cu2 dumbbells in TbCu7-type YCu6.576 studied by Bragg and total scattering techniques Černý, Radovan; Filinchuk, Yaroslav; Brühne, Stefan Intermetallics, Vol. 17, Issue 10 https://doi.org/10.1016/j.intermet.2009.03.010	journal	October 2009
2Flux growth and characterization of Ce-substituted ${Nd}_{2} {Fe}_{14} B$ single crystals Susner, Michael A.; Conner, Benjamin S.; Saparov, Bayrammurad I. Journal of Magnetism and Magnetic Materials, Vol. 434 https://doi.org/10.1016/j.jmmm.2016.10.127	journal	July 2017
Cast Permanent Magnets of Cobalt, Copper, and Cerium: Process and Performance Characteristics Cullen, Thomas J. Journal of Applied Physics, Vol. 42, Issue 4 https://doi.org/10.1063/1.1660328	journal	March 1971
Preparation and properties of sintered CoCuFeCe permanent magnets Sherwood, R. C.; Nesbitt, E. A.; Chin, G. Y. Materials Research Bulletin, Vol. 7, Issue 5 https://doi.org/10.1016/0025-5408(72)90151-1	journal	May 1972
Sintered Ce‐Co‐Cu‐Fe‐Ti magnets Inomata, Koichiro; Oshima, Teruo; Ido, Tadashi Applied Physics Letters, Vol. 30, Issue 12 https://doi.org/10.1063/1.89280	journal	June 1977
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Sintered magnets of copper- and iron-modified cerium cobalt Tawara, Y.; Senno, H. IEEE Transactions on Magnetics, Vol. 8, Issue 3 https://doi.org/10.1109/TMAG.1972.1067360	journal	September 1972
High performance Nd-Fe-B permanent magnets without critical elements Pathak, Arjun K.; Gschneidner, K. A.; Khan, M. Journal of Alloys and Compounds, Vol. 668 https://doi.org/10.1016/j.jallcom.2016.01.194	journal	May 2016
Practical Aspects of Modern and Future Permanent Magnets McCallum, R. W.; Lewis, L.; Skomski, R. Annual Review of Materials Research, Vol. 44, Issue 1 https://doi.org/10.1146/annurev-matsci-070813-113457	journal	July 2014
The crystal structures of the rare-earth compounds of the form R2Ni17, R2Co17 and R2Fe17 Buschow, K. H. J. Journal of the Less Common Metals, Vol. 11, Issue 3 https://doi.org/10.1016/0022-5088(66)90006-3	journal	September 1966
Structural and Ferromagnetic Properties of an Orthorhombic Phase of MnBi Stabilized with Rh Additions Taufour, Valentin; Thimmaiah, Srinivasa; March, Stephen Physical Review Applied, Vol. 4, Issue 1 https://doi.org/10.1103/PhysRevApplied.4.014021	journal	July 2015
Composition and crystal structure of hexagonal Cu-rich rare earth–copper compounds Buschow, K. H. J.; van der Goot, A. S. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 27, Issue 6 https://doi.org/10.1107/S0567740871003558	journal	June 1971
Cerium: An Unlikely Replacement of Dysprosium in High Performance Nd-Fe-B Permanent Magnets Pathak, Arjun K.; Khan, Mahmud; Gschneidner, Karl A. Advanced Materials, Vol. 27, Issue 16 https://doi.org/10.1002/adma.201404892	journal	March 2015
Permanent magnets based on (Ce,Sm)(Co,Fe,Cu) _z Tawara, Yoshio; Chino, Tetsuichi; Matsui, Yukihiro Applied Physics Letters, Vol. 33, Issue 7 https://doi.org/10.1063/1.90460	journal	October 1978
Theory of ferromagnetism in ${CeCo}_{5}$ Nordström, Lars; Eriksson, Olle; Brooks, M. S. S. Physical Review B, Vol. 41, Issue 13 https://doi.org/10.1103/PhysRevB.41.9111	journal	May 1990
What determines the demagnetization in Nd-Fe-B magnets? Blank, R. Journal of Magnetism and Magnetic Materials, Vol. 101, Issue 1-3 https://doi.org/10.1016/0304-8853(91)90765-3	journal	October 1991
New Permanent Magnet Materials Containing Rare‐Earth Metals Nesbitt, E. A. Journal of Applied Physics, Vol. 40, Issue 3 https://doi.org/10.1063/1.1657619	journal	March 1969
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets Chen, Ruyi; Cui, Qirui; Liao, Liyang Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23414-3	journal	May 2021
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-58835-5	journal	February 2020
Structural and Magnetic Properties of Iron-Rich Compounds in the Yb—Fe—Ga System. Tokaychuk, Ya. O.; Bodak, O. I.; Gorelenko, Yu. K. ChemInform, Vol. 37, Issue 30 https://doi.org/10.1002/chin.200630010	journal	July 2006
Structural and ferromagnetic properties of an orthorhombic phase of MnBi stabilized with Rh additions Taufour, Valentin; Thimmaiah, Srinivasa; March, Stephen arXiv https://doi.org/10.48550/arxiv.1508.00473	text	January 2015
Micromagnetic simulations with periodic boundary conditions: Hard-soft nanocomposites Wysocki, Aleksander L.; Antropov, Vladimir P. arXiv https://doi.org/10.48550/arxiv.1510.08543	preprint	January 2015

Cited By (2)

Computational screening of Fe-Ta hard magnetic phases Arapan, S.; Nieves, P.; Herper, H. C. Physical Review B, Vol. 101, Issue 1 https://doi.org/10.1103/physrevb.101.014426	journal	January 2020
Computational screening of Fe-Ta hard magnetic phases Arapan, Sergiu; Nieves, Pablo; Herper, Heike C. arXiv https://doi.org/10.48550/arxiv.1910.10531	text	January 2019

Similar Records

Effect of the Ce Content on the Magnetic Properties and Microstructure of CeCo{sub 5}-based Sintered Bulk Magnets

Journal Article · Fri Jun 15 00:00:00 EDT 2018 · Journal of Superconductivity and Novel Magnetism · OSTI ID:1494934

Sun, Wei; Song, Kui-kui; Zhu, Ming-gang; +4 more

Atomic cooperation in enhancing magnetism: (Fe, Cu)-doped CeCo₅

Journal Article · Mon May 11 00:00:00 EDT 2020 · Journal of Alloys and Compounds · OSTI ID:1494934

Choudhary, Renu; Palasyuk, Andriy; Nlebedim, Ikenna C.; +2 more

Ternary and quaternary rare earth cobalt magnetic materials with low reversible temperature coefficients

Journal Article · Thu Mar 01 00:00:00 EST 1979 · J. Appl. Phys.; (United States) · OSTI ID:1494934

Gupta, N; Martis, R J.J.; Sankar, S G; +1 more

Related Subjects

36 MATERIALS SCIENCE

Title: Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo5 Systems

Citation Formats

References (59)

Cited By (2)

Similar Records

Related Subjects

Title: Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo₅ Systems