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

Abstract

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 themore »« less

Authors:

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)

Publication Date:: Fri Jan 25 00:00:00 EST 2019

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1494934

Alternate Identifier(s):: OSTI ID: 1492120

Report Number(s):: IS-J-9882
Journal ID: ISSN 2331-7019; PRAHB2

Grant/Contract Number:: AC02-07CH11358

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Applied

Additional Journal Information:: Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2331-7019

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    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., and Palasyuk, Andriy. Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo5 Systems.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevApplied.11.014052.

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                    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. Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo5 Systems.  United States.  https://doi.org/10.1103/PhysRevApplied.11.014052

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                    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., and Palasyuk, Andriy. Fri .  
"Single-Crystal Permanent Magnets: Extraordinary Magnetic Behavior in the Ta-,Cu-, and Fe-Substituted CeCo5 Systems".  United States.  https://doi.org/10.1103/PhysRevApplied.11.014052.  https://www.osti.gov/servlets/purl/1494934.

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@article{osti_1494934,

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

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

  abstractNote = {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 Ce15.1Ta1.0Co74.4Cu9.5, Ce16.3Ta0.6Co68.9Cu14.2, Ce15.7Ta0.6Co67.8Cu15.9, Ce16.3Ta0.3Co61.7Cu21.7, and Ce14.3Ta1.0Co62.0Fe12.3Cu10.4. 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.},

  doi          = {10.1103/PhysRevApplied.11.014052},

  journal      = {Physical Review Applied},

  number       = 1,

  volume       = 11,

  place        = {United States},

  year         = {Fri Jan 25 00:00:00 EST 2019},

  month        = {Fri Jan 25 00:00:00 EST 2019}

}

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Works referencing / citing this record:

Computational screening of Fe-Ta hard magnetic phases
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Arapan, S.; Nieves, P.; Herper, H. C.
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Rare-earth-lean Sm(Fe,Co,Ti)₁₂ alloys with the ThMn₁₂ crystal structure and less than one Ti atom per formula unit have the potential of exceptionally powerful permanent magnets, but all prior attempts to develop high coercivity in bulk alloys, especially coercivity combined with crystallographic texture, have fallen short of the expectations. This study was aimed at improvement of the currently best Sm(Fe,Co,Ti)₁₂ magnets prepared through melt-spinning which are inherently isotropic. Modifications of the alloys with B and Zr, already demonstrated in earlier studies to be effective separately, have been implemented simultaneously. Here, a systematic study of Sm_1.1-x(Fe,Co)_11.3-yTi_0.7B_y alloys melt-spun at a tangential speedmore »« less
https://doi.org/10.1016/j.jmmm.2021.167867

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Development of Mischmetal–Fe–Co–B Permanent Magnet Alloys via High-Throughput Methods

Journal Article Chaudhary, Rakesh P. ; Gandha, Kinjal H. ; Meng, Fanqiang ; ... - ACS Combinatorial Science

Additive manufacturing synthesis using laser engineered net shaping (LENS) is utilized in this work to rapidly print libraries of mischmetal (MM = La, Ce, Nd, and Pr) containing R₂TM₁₄B alloys (R = MM + separated Nd and TM = Fe and Co) enabling robust evaluation of physical properties over a wide composition range. High-throughput characterization of the magnetic and thermal properties are used to identify compositions for potential high-temperature, high-performance permanent magnets with reduced critical rare-earth elements. Improved Curie temperature (T_c ~ 450 °C) is obtained with substitution of Fe by Co in pseudoternary R₂TM₁₄B alloys. Furthermore, a 4-fold decreasemore »« less
Cited by 6
https://doi.org/10.1021/acscombsci.9b00190

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

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Citation Formats

Permanent magnets: Plugging the gap journal, September 2012

Generalized Gradient Approximation Made Simple journal, October 1996

Microstructure of a Cerium, Cobalt and Copper Alloy with a High Coercivity journal, January 1969

Effect of Processing on Permanent Magnet Materials Containing Rare‐Earth Metals journal, September 1969

An empirical correction for absorption anisotropy journal, January 1995

Projector augmented-wave method journal, December 1994

Local spin density functional approach to the theory of exchange interactions in ferromagnetic metals and alloys journal, May 1987

Magnetocrystalline anisotropy in cobalt based magnets: a choice of correlation parameters and the relativistic effects journal, April 2018

Structural and magnetic properties of Nd 2 Fe 1 4 B (invited) journal, April 1985

Influence of cerium content on the structure and magnetic behavior of Co-Fe-Cu-Ce permanent magnets journal, September 1973

X-ray and neutron determination of a so-called Th2Ni17-type structure in the lutetium-iron system journal, December 1972

The structure of Co-Cu-Fe-Ce permanent magnets journal, September 1973

Structural and magnetic properties of iron-rich compounds in the Yb–Fe–Ga system journal, May 2006

Spin-Fluctuation Mechanism of Anomalous Temperature Dependence of Magnetocrystalline Anisotropy in Itinerant Magnets journal, November 2015

Recent advances in magnetic structure determination by neutron powder diffraction journal, October 1993

From ultrasoft pseudopotentials to the projector augmented-wave method journal, January 1999

A critical review on solvent extraction of rare earths from aqueous solutions journal, February 2014

Directional solidification of Co-Cu-R permanent-magnet alloys journal, March 1972

Intermetallic compounds in the cobalt-rich part of the R-cobalt systems (R = Ce, La, CeLa) journal, February 1974

Oxidation study of monocrystalline CeCo5−xCux by X-ray diffraction methods journal, June 1980

Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators journal, August 1995

Ce 3 − x Mg x Co 9 : Transformation of a Pauli Paramagnet into a Strong Permanent Magnet journal, February 2018

Growth of single crystals from metallic fluxes journal, June 1992

Prospects for Non-Rare Earth Permanent Magnets for Traction Motors and Generators journal, June 2012

New Permanent Magnet Materials journal, June 1968

Cerium, Cobalt and Copper Alloy as a Permanent Magnet Material journal, August 1968

Aspects of spin dynamics and magnetic interactions journal, October 1999

X-ray study of monocrystalline alloys near the composition CeCo3.5Cu1.5 journal, August 1979

Formation of TbCu7-type CeFe10Zr0.8 by rapid solidification journal, August 2013

Micromagnetic simulations with periodic boundary conditions: Hard-soft nanocomposites journal, April 2017

Rare earth-cobalt permanent magnets journal, November 1991

Phase equilibria in the CeCo5-CeCu5 system and structural characterization of the Ce(Co1−xCux)5 phases journal, August 1985

Magnetic anisotropy and high-field magnetization process of CeCo5 journal, March 1994

Structural and magnetic properties of iron-rich compounds in the Yb–Fe–Al system journal, May 2003

A study of the physical properties of single crystalline Fe5B2P journal, March 2016

Permanent-magnet properties of Sm-Ce-Co-Fe-Cu alloys with compositions between 1-5 and 2-17 journal, June 1974

Local atomic order in the vicinity of Cu2 dumbbells in TbCu7-type YCu6.576 studied by Bragg and total scattering techniques journal, October 2009

2Flux growth and characterization of Ce-substituted Nd 2 Fe 14 B single crystals journal, July 2017

Cast Permanent Magnets of Cobalt, Copper, and Cerium: Process and Performance Characteristics journal, March 1971

Preparation and properties of sintered CoCuFeCe permanent magnets journal, May 1972

Sintered Ce‐Co‐Cu‐Fe‐Ti magnets journal, June 1977

Special points for Brillouin-zone integrations journal, June 1976

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Sintered magnets of copper- and iron-modified cerium cobalt journal, September 1972

High performance Nd-Fe-B permanent magnets without critical elements journal, May 2016

Practical Aspects of Modern and Future Permanent Magnets journal, July 2014

The crystal structures of the rare-earth compounds of the form R2Ni17, R2Co17 and R2Fe17 journal, September 1966

Structural and Ferromagnetic Properties of an Orthorhombic Phase of MnBi Stabilized with Rh Additions journal, July 2015

Composition and crystal structure of hexagonal Cu-rich rare earth–copper compounds journal, June 1971

Cerium: An Unlikely Replacement of Dysprosium in High Performance Nd-Fe-B Permanent Magnets journal, March 2015

Permanent magnets based on (Ce,Sm)(Co,Fe,Cu) z journal, October 1978

Theory of ferromagnetism in CeCo 5 journal, May 1990

What determines the demagnetization in Nd-Fe-B magnets? journal, October 1991

New Permanent Magnet Materials Containing Rare‐Earth Metals journal, March 1969

Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets journal, May 2021

Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect journal, February 2020

Structural and Magnetic Properties of Iron-Rich Compounds in the Yb—Fe—Ga System. journal, July 2006

Structural and ferromagnetic properties of an orthorhombic phase of MnBi stabilized with Rh additions text, January 2015

Micromagnetic simulations with periodic boundary conditions: Hard-soft nanocomposites preprint, January 2015

Computational screening of Fe-Ta hard magnetic phases journal, January 2020

Computational screening of Fe-Ta hard magnetic phases text, January 2019

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

Permanent magnets: Plugging the gap
journal, September 2012

Generalized Gradient Approximation Made Simple
journal, October 1996

Microstructure of a Cerium, Cobalt and Copper Alloy with a High Coercivity
journal, January 1969

Effect of Processing on Permanent Magnet Materials Containing Rare‐Earth Metals
journal, September 1969

An empirical correction for absorption anisotropy
journal, January 1995

Projector augmented-wave method
journal, December 1994

Local spin density functional approach to the theory of exchange interactions in ferromagnetic metals and alloys
journal, May 1987

Magnetocrystalline anisotropy in cobalt based magnets: a choice of correlation parameters and the relativistic effects
journal, April 2018

Structural and magnetic properties of Nd ₂ Fe ₁ ₄ B (invited)
journal, April 1985

Influence of cerium content on the structure and magnetic behavior of Co-Fe-Cu-Ce permanent magnets
journal, September 1973

X-ray and neutron determination of a so-called Th2Ni17-type structure in the lutetium-iron system
journal, December 1972

The structure of Co-Cu-Fe-Ce permanent magnets
journal, September 1973

Structural and magnetic properties of iron-rich compounds in the Yb–Fe–Ga system
journal, May 2006

Spin-Fluctuation Mechanism of Anomalous Temperature Dependence of Magnetocrystalline Anisotropy in Itinerant Magnets
journal, November 2015

Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

A critical review on solvent extraction of rare earths from aqueous solutions
journal, February 2014

Directional solidification of Co-Cu-R permanent-magnet alloys
journal, March 1972

Intermetallic compounds in the cobalt-rich part of the R-cobalt systems (R = Ce, La, CeLa)
journal, February 1974

Oxidation study of monocrystalline CeCo5−xCux by X-ray diffraction methods
journal, June 1980

Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators
journal, August 1995

${Ce}_{3 - x} {Mg}_{x} {Co}_{9}$ : Transformation of a Pauli Paramagnet into a Strong Permanent Magnet
journal, February 2018

Growth of single crystals from metallic fluxes
journal, June 1992

Prospects for Non-Rare Earth Permanent Magnets for Traction Motors and Generators
journal, June 2012

New Permanent Magnet Materials
journal, June 1968

Cerium, Cobalt and Copper Alloy as a Permanent Magnet Material
journal, August 1968

Aspects of spin dynamics and magnetic interactions
journal, October 1999

X-ray study of monocrystalline alloys near the composition CeCo3.5Cu1.5
journal, August 1979

Formation of TbCu7-type CeFe10Zr0.8 by rapid solidification
journal, August 2013

Micromagnetic simulations with periodic boundary conditions: Hard-soft nanocomposites
journal, April 2017

Rare earth-cobalt permanent magnets
journal, November 1991

Phase equilibria in the CeCo5-CeCu5 system and structural characterization of the Ce(Co1−xCux)5 phases
journal, August 1985

Magnetic anisotropy and high-field magnetization process of CeCo5
journal, March 1994

Structural and magnetic properties of iron-rich compounds in the Yb–Fe–Al system
journal, May 2003

A study of the physical properties of single crystalline Fe5B2P
journal, March 2016

Permanent-magnet properties of Sm-Ce-Co-Fe-Cu alloys with compositions between 1-5 and 2-17
journal, June 1974

Local atomic order in the vicinity of Cu2 dumbbells in TbCu7-type YCu6.576 studied by Bragg and total scattering techniques
journal, October 2009

2Flux growth and characterization of Ce-substituted ${Nd}_{2} {Fe}_{14} B$ single crystals
journal, July 2017

Cast Permanent Magnets of Cobalt, Copper, and Cerium: Process and Performance Characteristics
journal, March 1971

Preparation and properties of sintered CoCuFeCe permanent magnets
journal, May 1972

Sintered Ce‐Co‐Cu‐Fe‐Ti magnets
journal, June 1977

Special points for Brillouin-zone integrations
journal, June 1976

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Sintered magnets of copper- and iron-modified cerium cobalt
journal, September 1972

High performance Nd-Fe-B permanent magnets without critical elements
journal, May 2016

Practical Aspects of Modern and Future Permanent Magnets
journal, July 2014

The crystal structures of the rare-earth compounds of the form R2Ni17, R2Co17 and R2Fe17
journal, September 1966

Structural and Ferromagnetic Properties of an Orthorhombic Phase of MnBi Stabilized with Rh Additions
journal, July 2015

Composition and crystal structure of hexagonal Cu-rich rare earth–copper compounds
journal, June 1971

Cerium: An Unlikely Replacement of Dysprosium in High Performance Nd-Fe-B Permanent Magnets
journal, March 2015

Permanent magnets based on (Ce,Sm)(Co,Fe,Cu) _z
journal, October 1978

Theory of ferromagnetism in ${CeCo}_{5}$
journal, May 1990

What determines the demagnetization in Nd-Fe-B magnets?
journal, October 1991

New Permanent Magnet Materials Containing Rare‐Earth Metals
journal, March 1969

Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021

Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020

Structural and Magnetic Properties of Iron-Rich Compounds in the Yb—Fe—Ga System.
journal, July 2006

Structural and ferromagnetic properties of an orthorhombic phase of MnBi stabilized with Rh additions
text, January 2015

Micromagnetic simulations with periodic boundary conditions: Hard-soft nanocomposites
preprint, January 2015

Computational screening of Fe-Ta hard magnetic phases
journal, January 2020

Computational screening of Fe-Ta hard magnetic phases
text, January 2019