Original manuscript, Proceedings of 20th International Workshop on

RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________

Recent Progress in Sm-Co Type Permanent Magnets

M. Marinescu, J. F. Liu and M. H. Walmer

Electron Energy Corporation, Landisville, PA, USA

Abstract. This paper presents research results reported in the past two years on high performance
Sm-Co permanent magnets. The work discussed is organized in two parts: (1) Sm-Co based bulk
permanent magnets referring to results on various magnetic and structural studies and new
achievements in the fabrication of (i) Sm(Co,Fe,Cu,Zr)z magnets with almost zero reversible
temperature coefficient of residual induction, (ii) Sm(Co,Fe,Cu,Zr)z magnets with increased
electrical resistivity, and (iii) Sm-Co bulk nanocomposites and (2) Sm-Co based ribbons,
nanoparticles and nanocomposite powders, for potential small scale applications or consolidation
into bulk specimens, referring to the latest results on their synthesis and characterization.

Keywords: permanent magnets, Sm2Co17, SmCo5, SmCo7, Sm(Co,Fe,Cu,Zr)z, thermal stability,

radiation stability, electrical resistivity, ribbons, nanoparticles, nanocomposites.

Contact author: M. Marinescu, Electron Energy Corporation, 924 Links Ave, Landisville, PA
17538, USA; tel: 717 898 2294; fax: 717 898 0660; mmarinescu@electronenergy.com

I. INTRODUCTION (micro)magnetic analyses. We did not

Though Sm-Co permanent magnets can
not compete with Nd-Fe-B magnets in the
maximum energy product at room
temperature and cost, they are far more
superior for high temperature applications
and for their corrosion resistance. This, in
conjunction with maximum energy products,
(BH)max, exceeding 30 MGOe in some
Sm(Co,Fe,Cu,Zr)z grades, makes Sm-Co
magnets vital for high performance in
applications with a service temperature
between 250- 550 oC.
This work is an attempt to summarize
the past two years of research results related
to both material development and
investigations of Sm-Co based alloy
systems. Our focus was on consolidated
permanent magnets and their possible
precursor forms (ribbons, nanoparticles and
nanocomposite powders), with a strong
emphasis on a practical point of view
without discussing the works on
include here the work on thin films.
II. Sm-Co bulk permanent magnets
Sintered RE(Co,Fe,Cu,Zr)z magnets with
zero reversible temperature coefficient of Br
Permanent magnets with very low α
(reversible temperature coefficient of
remanence, Br) over a temperature span
between -50 oC and 250 oC are needed in
applications such as traveling wave tubes for
satellite communications and microwave
directed energy systems, accelerometers,
torquers, and gyroscopes, especially for
military and aerospace operations. For many
years, EEC has produced magnets with near
zero α in the temperature range of -50 oC to
150 oC and (BH)max up to 16-18 MGOe.
New modified compositions with combined
substitution of Gd and Er for Sm and
optimized processing conditions resulted in
reversible temperature coefficient of
remanence, α = -0.009 ÷ 0.0001 ppm/oC (as
derived from close-circuit remanence

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1
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________
measurements) for the temperature variation
between -50 oC and 150 oC. Values of Br
exceeding 9 kG and Hk of over 20 kOe for
some compositions (Hk is the
demagnetization field at which Br is
decreased by 10%; Hk is a measure of loop
squareness) allowed for excellent maximum
energy products (BH)max of 18-20 MGOe at
room temperature1. Figure 1 depicts the
demagnetization curve at different
temperatures for a selected magnet
composition with the ratio of the rare earth
elements Gd/Er/Sm = 30/26/44 and TM/RE
ratio z = 6.90.
Figure 1 Demagnetization curves at different
temperatures for (Sm,Gd,Er)(Co,Fe,Cu,Zr)z magnets
processed by isostatic pressing, sintering at 1210 oC,
solution treatment at temperatures in the range of
1195- 1200 oC and aging at 815 oC for 36h.
Sintered Sm(Co,Fe,Cu,Zr)z magnets with
increased electrical resisitivity
The electrical resistivity of Sm-Co
magnets typically ranges from 37-77
µΩ⋅cm, while of Nd-Fe-B magnets is about
0.14 µΩ⋅cm. Magnets with increased
electrical resistivity are needed in permanent
magnet motors and high speed power
generators in order to reduce eddy current
losses. One of the solutions is to use bonded
_____________________________________________________________________________
2
magnets which have a high resistivity due to
the insulation effect of polymer binders, but
in general the operating temperature is
dramatically limited by the polymer
softening above 200 oC. Recently2, fully
dense composite magnets were produced by
sintering blends of Sm(Co,Fe,Cu,Zr)z
magnet powder precursors and small
amounts of CaF3 powders. The resistivity of
the magnets with 2.5 wt% CaF3 increased by
30% whereas the magnetic performance was
only slightly altered: Br = 10.8 kG, Hci > 25
kOe, (BH)max = 27.1 MGOe. It was found
that some amount of Sm diffuses into the
CaF3 inclusions upon processing the magnet
at high temperatures. However, this can be
compensated with excess Sm in the magnet
powder precursor. A much higher increase
in the electrical resistivity of ~ 1000 µΩ⋅cm
was achieved in “glass-bonded” anisotropic
Sm(Co,Fe,Cu,Zr)z / B2O3 magnets produced
by hot pressing at 475 oC, which is slightly
above the melting point of B2O3. In this
case, the Sm(Co,Fe,Cu,Zr)z powder had
already developed hard magnetic properties
and B2O3 acted as a binder. The relatively
low-temperature consolidation preserved the
high coercivity of the Sm(Co,Fe,Cu,Zr)z
magnet powder, but the residual induction
was decreased due to a lower density and led
to a (BH)max of 8 MGOe.
Effect of oxygen and residual carbon in
sintered Sm(Co,Fe,Cu,Zr)z magnets
For applications above 400 oC,
Sm(Co,Fe,Cu,Zr)z magnets need to be
coated usually by Ni plating. A recent study3
reported results of the in-air oxidation
process of uncoated Sm(Co,Fe,Cu,Zr)z
magnets at temperatures between 300 oC and
600 oC. The respective findings suggest that
the oxides layers formed on the surface,
which is depleted in Sm, are CuO, Co3O4
and CoFe2O4. These layers do not exceed 15
µm and their effect on magnetic properties is
negligible. A so-called internal oxidation
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________
zone was found to follow the above oxide many years6. Magnets with a lower
layers and to consist of a CoFe matrix with a operating temperature (larger Fe content)
Sm-rich oxide and Cu and Co precipitates. showed more pronounced losses after
This zone grows parabolically in time exposure at 300 oC in air, while the Ni and
inwards the bulk body of the magnets and Al coated high temperature magnets able to
can be more damaging to the magnetic operate up to 550 oC showed almost no
properties. losses after the initial thermal stabilization,
Residual carbon in Sm(Co,Fe,Cu,Zr)z as shown in Figure 2.
magnets may become an important issue
when the magnets are produced from
powder milled in alcohol or consolidated
with an organic binder aid (especially in the
case of small specimens which are otherwise
difficult to be formed). A study4 showed that
the magnetic properties of the magnets start
to deteriorate when the carbon content is
above 0.1 wt%, and even extinguish for 0.43
wt% carbon. It appears that carbon reacts
with Zr forming ZrC, possibly during
sintering. The typical cellular microstructure
of Sm(Co,Fe,Cu,Zr)z magnets appears to be
highly distorted in the specimens containing Figure 2 Thermal stability at 300oC in air for more
0.43 wt% carbon and have much larger non- than three years, of various Sm(Co,Fe,Cu,Zr)z
magnets with an operating temperature of 250 oC to
uniform cells while the amount of the 1:5 550 oC.
cell boundaries is reduced. The widely-
accepted mechanism of Cu diffusion to the
1:5 cell boundary and hence the 1.0
development of coercivity intermediated by Sm-Co Magnet Sample

some Zr-rich lamellar phase may hold the 0.8

Normalized Magnetic Flux

answer to the non-existent coercivity when 0.6

Zr is consumed into the ZrC phase.

0.4

Thermal stability and radiation resistance of 0.2 Nd-Fe-B Magnet Smaple

high-temperature Sm(Co,Fe,Cu,Zr)z sintered
0.0
magnets
1E12 1E13 1E14 1E15 1E16 1E17 1E18 1E19
Sm(Co,Fe,Cu,Zr)z sintered magnets are 2
Neutron Flux (n/cm )
used also in space applications such as high
power ion propulsion engines where they Figure 3 Normalized magnetic flux of
Sm(Co,Fe,Cu,Zr)z and Nd-Fe-B permanent magnets
operate at elevated temperatures under versus neutron flux.
vacuum and radiation. Ultra high
temperature (UHT) Sm-Co magnets that can Sm(Co,Fe,Cu,Zr)z magnets have also a
be used up to 550 oC have been developed5 superior radiation resistance compared to
at EEC in the late 90’s. The thermal stability, Nd-Fe-B magnets. It was shown6 that Sm-
in terms of magnetic irreversible losses, for Co magnets do not have any noticeable
different grades of Sm(Co,Fe,Cu,Zr)z changes in magnetic properties (Figure 3),
sintered magnets has been monitored for while Nd13Dy2Fe77B8 magnets appear to
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3
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________
loose almost 100% of their magnetic flux
with a neutron flux of 1016 n/cm2. The
radiation resistance and thermal stability are
somewhat related because the irradiation
damage is most likely caused by a radiation-
induced thermal effect and less by structural
modifications.
Sm-Co nanocomposites
Sm-Co 2:17 alloy compositions with
lean-Sm content that provide reasonably
high magnetization, continue to be a
challenge with regard to the ability to
develop useful intrinsic coercivity. The
attempts to produce nanostructured Sm-Co
magnets with reduced amounts of non-
magnetic atomic species and no cellular
microstructure have not yet resulted in a
significant breakthrough. However, the
research conducted in the last two years
unveiled some new interesting aspects.
Finer grains (20-50 nm) developed with
the addition of Zr in Sm(CobalFe0.3ZrxB0.04)10
melt spun ribbons7 lead to a 67% increase of
Hci to 6.5 kOe and 70% increase of (BH)max
to 9.5 MGOe. Grain refinement is also
responsible for the increase in coercivity in
Nb added Sm(Co0.67Fe0.2Zr0.05B0.04Nb0.04)8
ribbons that show an Hci of 21 kOe.
However after the consolidation of these
ribbons into bulk specimens by hot
deformation, the magnetic properties are still
modest with a low remanence, and poor
demagnetization curve squarness. The
squareness is improved in hot deformed
specimens with the addition of Cu. It had
not yet been investigated why the addition
of Cu in Sm(CobalFe0.2Zr0.05B0.04Cu0.04)8
increases the Hci (from 15.1 kOe to 17 kOe)
– is it because Cu stabilizes the formation of
the hexagonal 1:5 and 1:7 phases or does it
form secondary phases that act as domain
wall pinning centers. Interestingly, a
crystallographic texture was formed in the
multiphase 2:17R/1:5H(1:7H)/2:7R
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4
Sm(CobalFe0.2Zr0.05B0.04Cu0.04)8 hot
7
deformed magnets . This may be the first
report on inducing texture in 2:17R phase
and further studies are needed. Development
of texture is usually expected for 1:5H and
1:7H phases upon rapid quenching when
there is a quenching temperature gradient or
upon hot deformation; however, 2:17R
phase is known to develop twin defects. The
following magnetic properties were reported
for measurements along the easy
magnetization direction of hot deformed
Sm(CobalFe0.2Zr0.05B0.04Cu0.04)8 specimens:
Hci ~ 9kOe, 4πMr ~ 7.5 kG, (BH)max ~13.2
MGOe; the demagnetization curves along
the easy and hard magnetic axis are shown
in Figure 4.
Figure 4 Demagnetization curves of
Sm(Co0.63Fe0.2Zr0.05B0.04Cu0.04Nb0.04)8 hot deformed
bulk magnet (from ref. 7).
In an attempt to develop anisotropic Sm-
Co based magnets with a morphology
consisting of 2:17 grains insulated by a non-
magnetic phase, small amounts of Ag, C,
Ga, In and Sn were added to Sm2Co17,
Sm2(Co,Fe)17 and Sm2(Co,Fe,Mn)17 system
in the ingot preparation8. All the additions,
except Ga, are not soluble into 2:17 phase
and form secondary phases. However,
different aspects of the morphology and
properties of these secondary phases such as
poor wetting of the matrix grains (Sm-Ag
phase), high melting temperature (Sm-Co-
Ag-Sn phase) or ferromagnetic behavior
(when SmCo5 forms at the grain boundaries)
discard most of the respective elements. The
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
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most interesting results are from the addition
of In that results in the precipitation of a
Sm-Co-In (assumed) non-magnetic phase
with a low melting temperature (1070oC)
and fairly good wetting behavior, able to
support low temperature liquid phase
sintering for achieving almost full density.
Figure 5 shows the morphology of this
specimen along the fractured section in the
micrograph taken by scanning electron
microscopy in back scattering mode and
distribution of elemental In. Although the
grains are considerably large, it appears that
the addition of In leads to an increased Hci
of up to 8 kOe in
Sm12.5(Co0.85Fe0.11Mn0.04)86In1.5 magnets
sintered at 1075oC and annealed at 1000oC
with a subsequent quenching. The
remanence of the best specimens did not
exceed 9 kG, which limits the practical use
of these magnets.
(a) (b)
Figure 5 (a) BSE SEM image of a fractured surface
of Sm12.5(Co0.85Fe0.075Mn0.075)86In1.5 magnet sintered
at 1075 oC and (b) indium elemental map for the
selected area.
It has been shown in early studies9 that
the combined Mn and Fe substitution for Co
in Sm2Co17 sintered magnets with the
rhombohedral Th2Zn17-type structure results
in an increase of both anisotropy constant K1
and saturation magnetization Ms. Moreover,
a higher anisotropy can be obtained in the
disordered TbCu7-type structure of Sm2Co17
phase, which is mostly favored when
applying non-equilibrium synthesis methods
such as rapid quenching or mechanical
alloying or upon devitrification annealing of
non-crystalline precursors synthesized with
_____________________________________________________________________________
5
these methods. Thus, a recent study10 was
focused on Smx(Co,Fe,Mn)100-x (x= 9-16.7
at%) high energy ball milled powder and
consolidated magnets prepared by hot
pressing. The powder and magnets were
isotropic and, for a slightly
overstoichiometric composition, the (BH)max
was 15.6 MGOe for the annealed
Sm11(Co0.85Fe0.075Mn0.075)89 powder and 15.7
MGOe for Sm13(Co0.7Fe0.25Mn0.05)87 hot
pressed magnets with a 88% density.
Although the level of (BH)max was in the
range of that obtained for the Fe substitution
alone, the addition of Mn brings a better
structural stability of the magnets which can
be hot pressed at temperatures as high as
750- 800 oC without the precipitation of
unwanted phases (i.e. 1:3, 1:2 phases). The
variation of the hysteresis parameters as a
function of the annealing temperature
between 550 oC and 800 oC for
Smx(Co0.85Fe0.075Mn0.075)100-x is given in
Figure 6. The efforts to develop
nanocomposite counterparts by shifting the
composition towards a lean-Sm content
were not successful in terms of the achieved
levels of (BH)max. What is interesting to note
is that a low devitrification annealing
temperature (600 oC) may lead to a fine 1:7 /
bcc exchange coupled microstructure that
exhibits a high 4πMr = 11.4 kG but the
respective temperature is apparently not
enough to develop a reasonable Hci. For
higher annealing temperature (800 oC),
which results in an Hci ~ 7 kOe, the
exchange coupling is altered as a
consequence of microstructure coarsening
and a pronounced kink appears in the
demagnetization curve.
Bulk nanocrystalline SmCo7-xHfx have
been produced with 98% full density by
spark plasma sintering of the precursor high
energy ball milled powder11. However, the
dramatic increase of Hci with the Hf addition
up to 20.8 kOe for SmCo6.08Hf0.2 is hindered
by values of 4πMr below 6 kG. Hysteresis
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________
loops for bulk nanocrystalline specimens
with different Hf content is given in Figure
7.
Figure 6 Effect of annealing temperature on intrinsic
coercivity, remanent magnetization and maximum
energy product of high-energy milled and annealed
Smx(Co0.85Fe0.075Mn0.075)100-x alloys.
Figure 7 Hysteresis loops of the bulk nanocrystalline
SmCo7−xHfx magnets produced by spark plasma
sintering (from ref. 11).
III. Sm-Co ribbons, nanoparticles and
nanocomposite powders
Sm-Co melt spun ribbons
The topic of the evolution of
microstructure and magnetic properties in
_____________________________________________________________________________
6
melt-spun binary SmxCo100-x alloys with x
ranging from 4 to 16 was also recently
revisited12. For the ribbons spun at 40 m/s
wheel speed, 1:7 and fcc/hcp Co phases
were observed up to x = 12. As expected, Co
dendrites precipitate at low Sm content
while the microstructure was eutectic when
x = 8. For compositions with x = 6 to 10, the
Co precipitates are scaled to less than 50 nm
with an elongated (rods) morphology and
the matrix consists of almost submicron 1:7
grains. For Sm-rich compositions the
structure becomes coarser. The formation of
1:5 phase leads to the increase of Hci up to
9.3 kOe, but the maximum energy product is
expected to be low due to modest
magnetization values.
Similar with the case of Fe-Pt and Sm-
Fe-N systems for which the magnetic
properties are dependent on the structural
ordering, the intrinsic coercivity and
magnetization / demagnetization processes
in Sm-Co melt-spun ribbons can be
correlated with the order-disorder phase
transformations. In a recent work13, the
small addition of C and Nb to the base Sm-
Co composition with a stoichiometry in the
neighborhood of 2:17 phase is not
necessarily accounted for the relative high
Hci (7.85 kOe) as developed through
microstructure refinement. The
microstructure of (Sm12Co88)94Nb3C3
ribbons spun at 40 m/s is reported to consist
of ~100 nm 1:7 grains and ~ 10 nm Co
precipitates (however, it may be hard to
distinguish fcc Co from fcc NbC). NbC
precipitates at the grain boundaries upon
annealing, part of the 1:7 phase transforms
into the long-range ordered 2:17R phase and
Hci is increased to a little over 9 kOe. The
authors suggest that the increased role of
domain wall pinning observed is a result of
the presence of antiphase defects, APD, with
a size of ~ 8 nm. The interface between the
defects and the matrix acts as domain wall
pinning sites in a way similar to the
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________
Sm(Co,Fe,Cu,Zr)z systems with a 2:17 /1:5
cellular microstructure.
The dramatic effect of microstructure
refinement14 with the precipitation of RCoC2
carbides that may act as grain growth
inhibitors was achieved in Sm-(Co,Fe)-C
and Sm-(Co,Fe,Mn)-C melt spun ribbons
and is shown in Figure 8. The combined
addition of Mn and C did contribute to an
intrinsic coercivity of Hci= 11.7 kOe but the
largest (BH)max = 14.7 MGOe was reached
with a Mn-free Sm13(Co0.75Fe0.25)82.5C4.5
stoichiometry. Stoichiometry and quenching
rate dictate the phase composition and, up to
a certain extent, C suppresses the formation
of the stable 2:17R in favor of the disordered
metastable 1:7H14. Another atomic specie
know to stabilize the 1:7 structure and
increase the anisotropy field is Ti whose
addition to SmCo7 lead to a Hci of 9.7 kOe
in SmCo7.1Ti0.4 ribbons spun at high wheel
speed15. However, the exposure at 750 oC
starts to transform 1:7 into 2:17.
(1) (2) (a)
Figure 8 Bright-field TEM images for (1)
Sm12(Co0.75Fe0.25)88 and (2a) Sm13(Co0.75Fe0.25)81C6
ribbons spun at 20m/s. EDX spectra for grain-interior
and grain boundary region are given in (2b) and (2c)
respectively (from ref. 15).
Sm-Co nanoparticles and nanocomposite
powders
Sm2Co17 nanoparticles synthesized by
surfactant assisted ball milling were
reported16 to have Hci of 3.1 kOe for a
particle size of 23 nm. Isotropic
nanocrystalline SmCo5 and Sm2Co17
powders were synthesized by reductive
_____________________________________________________________________________
7
annealing of core/shell structured Co/Sm2O3
nanoparticles17. The intrinsic coercivities at
room temperature were 8 kOe and 1.4 kOe,
respectively.
Isotropic SmCo5/Fe nanocomposite
powders were synthesized18 by high
temperature reductive annealing of Fe3O4
nanoparticles embedded in a SmCo-
hydroxide matrix. The general trend of the
magnetic properties of this isotropic
composite powder is typical: with increasing
amounts of Fe nanoparticles incorporated
into SmCo5 nanostructured matrix,
magnetization increases and intrinsic
coercivity declines. Figure 9 shows the
structure of the nanocomposite powder
together with the hysteresis of the Fe-free
SmCo5 and SmCo5Fe1.5 nanocomposites.
(a) (b)
Figure 9 (a) HRTEM image of a single aggregate of
the SmCo5/Fe1 nanocomposite powder with the
dashed lines circling the nanocrystalline grains of
either SmCo5 or Fe. (b) Hysteresis loops of the
SmCo5 and SmCo5/Fe1.5 nanocomposite powder
(from ref. 19).
Anisotropic composite
Sm(Co0.699Fe0.213Cu0.064Zr0.024)7.4 / nano-Fe
powders were synthesized19 by depositing
on anisotropic hard magnetic
Sm(Co0.699Fe0.213Cu0.064Zr0.024)7.4 core
powder, soft magnetic Fe nanoparticles
produced by the chemical reduction of FeCl2
with NaBH4. The core powders with the
particle size in the range of 10 to 400 μm
were coated with Fe nanoparticles with
particle size below 50 nm. Optimized
 Original manuscript, Proceedings of 20th International Workshop on
RARE EARTH PERMANENT MAGNETS AND THEIR APPLICATIONS, Sept. 8-10, 2008, Crete, Greece
_____________________________________________________________________________________________
deposition conditions lead to enhanced
remanent magnetization from 10.5 kG to 11
kG with Fe-nanoparticle coating while the
squareness of the loop and Hci>25 kOe are
also preserved. Upon hot pressing, the Fe
nanoparticles transform into a nanolayer
distributed around the original core powder.
However, some local agglomeration of Fe
still occurs. The magnetic properties of the
consolidated composite powders are yet to
be optimized. Figure 10 shows SEM
micrographs of composite
Sm(Co0.699Fe0.213Cu0.064Zr0.024)7.4 / nano-Fe
free powder and hot pressed magnets.
(b)
(a)
(c)
Figure 10 SEM micrograph of a composite
Sm(Co0.699Fe0.213Cu0.064Zr0.024)7.4 / nano-Fe free
powder (a) and (b) and hot pressed magnet (c).
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