Packing fraction dependence of the coercivity and the energy product in nanowire based permanent magnets Ioannis Panagiotopoulos, Weiqing Fang, Frédéric Ott, François Boué, Kahina Aït-Atmane et al. Citation: J. Appl. Phys. 114, 143902 (2013); doi: 10.1063/1.4824381 View online: http://dx.doi.org/10.1063/1.4824381 View Table of Contents: http://jap.aip.org/resource/1/JAPIAU/v114/i14 Published by the AIP Publishing LLC. Additional information on J. Appl. Phys. Journal Homepage: http://jap.aip.org/ Journal Information: http://jap.aip.org/about/about_the_journal Top downloads: http://jap.aip.org/features/most_downloaded Information for Authors: http://jap.aip.org/authors Downloaded 13 Oct 2013 to 195.130.120.61. This article is copyrighted as indicated in the abstract. Reuse of AIP content is subject to the terms at: http://jap.aip.org/about/rights_and_permissions
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Packing fraction dependence of the coercivity and the energy product innanowire based permanent magnetsIoannis Panagiotopoulos, Weiqing Fang, Frédéric Ott, François Boué, Kahina Aït-Atmane et al. Citation: J. Appl. Phys. 114, 143902 (2013); doi: 10.1063/1.4824381 View online: http://dx.doi.org/10.1063/1.4824381 View Table of Contents: http://jap.aip.org/resource/1/JAPIAU/v114/i14 Published by the AIP Publishing LLC. Additional information on J. Appl. Phys.Journal Homepage: http://jap.aip.org/ Journal Information: http://jap.aip.org/about/about_the_journal Top downloads: http://jap.aip.org/features/most_downloaded Information for Authors: http://jap.aip.org/authors
Downloaded 13 Oct 2013 to 195.130.120.61. This article is copyrighted as indicated in the abstract. Reuse of AIP content is subject to the terms at: http://jap.aip.org/about/rights_and_permissions
Packing fraction dependence of the coercivity and the energy productin nanowire based permanent magnets
Ioannis Panagiotopoulos,1 Weiqing Fang,1 Fr�ed�eric Ott,1 Francois Bou�e,1
Kahina A€ıt-Atmane,2 Jean-Yves Piquemal,2 and Guillaume Viau3
1Laboratoire L�eon Brillouin CEA/CNRS UMR12, Centre d’Etudes de Saclay, 91191 Gif sur Yvette, France2ITODYS, Universit�e Paris 7-Denis Diderot, UMR CNRS 7086 2, Place Jussieu, 75251 Paris Cedex 05,France3Laboratoire de Physique et Chimie des Nano-Objets, INSA de Toulouse, UMR CNRS 5215,135 Av. De Rangueil, 31077 Toulouse Cedex 4, France
(Received 13 August 2013; accepted 20 September 2013; published online 7 October 2013)
The maximum magnetic performance which can be expected from elongated single domain particle
based permanent magnets is assessed. The results are derived using micromagnetic calculations to
model the behavior of large bundles of aligned nanowires. In particular, we discuss the cases of Co
and Fe nanowires and their packing fraction dependence of coercivity, which is the main limiting
factor. We show that it is, in principle, feasible to achieve BHmax values close to 300 kJ/m3 in Co
nanowires with a packing fraction p¼ 0.7 and close to 400 kJ/m3 at p¼ 0.85. The packing fraction
limitations are essentially non-existing due to the intrinsic magnetocrystalline anisotropy of Co. On
the other hand, if a low anisotropy material such as Fe could be produced in the form of fine, well
crystallized wires it could yield a BHmax close to 200 kJ/m3 at an optimum p¼ 0.7. As the
performance of iron nanowires is solely based on shape anisotropy it becomes coercivity limited
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Nevertheless Fe, being a high moment and low anisotropy
material, is an ideal system to test the effect of packing frac-
tion in a system in which the coercive field is mainly due to
shape anisotropy.
II. MICROMAGNETIC SIMULATION PROCESS
The micromagnetic calculations have been performed
with the Nmag package.7 The damping constant was set to
0.8 to achieve fast damping and reach convergence quickly.
The convergence criterion for each field step was that the
magnetization should move slower than 10�/ns (globally or
on average for all spins). The nanowire dimensions (length
L¼ 100 nm and diameter D¼ 14.5 nm) were chosen to
match those observed in recent high coercivity, polyol-
synthesized, mono-disperse cobalt nanowires.3 The bulk
magnetic parameters have been used. Namely, MS¼ 1.4
MA/m, KU¼ 520 kJ/m3, A¼ 28pJ/m for cobalt and
MS¼ 1.7MA/m, K1(cubic)¼ 48 kJ/m3, A¼ 21pJ/m for iron.
According to these values, the exchange lengths are 3.4 nm
and 2.4 nm for Co and Fe, respectively. A mesh length 7 nm
was used in order to be able to include a large number of par-
ticles (>400) within the simulation cell. For such large sam-
ples, the memory usage was 30 Gb. When using a mesh
smaller than the exchange length (2.4 nm), the calculated
switching fields are only increased by 1.3% and 6% Co and
Fe, respectively (as calculated for an isolated wire). We con-
sidered that increasing the system size was more important
to produce realistic results than aiming for (pseudo)-accurate
switching field values which are experimentally anyway
very sensitive to any defect in the system.
The external field was applied at 5� with respect to the
nanowires’ axes. In order to be able to simulate aligned
nanowire aggregates with a systematic variation of packing
fractions (ranging from zero up to close to unity) in a con-
sistent manner, 209 nanowires have been placed in regular
arrays of 19 rows arranged in an hexagonal 2D-lattice, each
row consisting of 11 nanowires stacked along their lengths.
For some packing fractions, larger aggregates consisting of
407 nanowires in 37 rows of 11 wires have been also simu-
lated. The numbers 19 and 37 are simply neighbors up to dis-
tances 2a and 3a, respectively from a central point in a
hexagonal lattice with a lattice constant a¼D þ d, where D
is the nanowires diameter and d is the distance between the
nanowires. The maximum packing fraction for a 2D hexago-
nal lattice (limit of d¼ 0) is pmax ¼ p2ffiffi3p . Different volume
packing fractions can obtained by adjusting d and the dis-
tance along the wire length dx according to p ¼ pmaxD
Dþd
� �2
LLþdx
h i. In order to consistently and uniquely define d and dx
for a given p, one could choose either to keep the bundle as-
pect ratio constant or simply set dx equal to d. We have cho-
sen the later in order to avoid large distances between
consecutive wires in a row at low packing fractions. A ran-
dom displacement of each row along the bundle axis by dL,
with �25 nm � dL � þ25nm was used to produce more re-
alistic bundles of nanowires, as it has been shown that such
configuration leads to a strong effect of coercivity (HC) loss
due to local stray fields.8 In order to validate the coercivity
values obtained in elongated bundles, especially for the case
of low anisotropy Fe, we have also performed calculations in
samples with aspect ratios close to unity consisting of 374
nanowires in 187 rows (neighbors up to 7a) of two wires.
The simulation of a single nanowire with the same character-
istics is considered as the p¼ 0 point.
The aspect ratio 19 � 11 bundle of nanowires as a whole
AR ¼ 11 � ðLþ dxÞ=ð5Dþ 4dÞ, ranged from AR¼ 6.8 to 15
for p¼ 0.05 to 0.87, respectively. Approximating their
demagnetizing factors by those of ellipsoids with the same
aspect ratio, these aspect ratios yield N¼ 0.04 to
N¼ 0.0015. Cylinders9 and prisms10 with the same aspect
ratios present equally low values. Based on these values, the
maximum demagnetizing field is found to be 0.009MS (for
p¼ 0.87), which is low compared to the HC derived from our
simulations for the isolated nanowires (HC¼ 0.54MS for Co
and HC¼ 0.21MS for Fe). Thus, the simulation samples can
be considered to reproduce well the conditions of closed
magnetic circuit measurements used for the characterization
of permanent magnet materials,2 in which the demagnetiza-
tion factor is practically zero. Nmag offers the possibility to
include the effects of the demagnetizing field by specifying
an appropriate arrangement of copies of the primary simula-
tion cell.11 However, we found that, in this specific case, it
should be used with caution as creating very long samples in
this way tends to create square loops with HC close to that of
a single nanowire. So we chose to simply work with high
AR prolate simulation cells without introducing further elon-
gation through extra copies. Examples of the magnetic con-
figurations close to the nucleation and coercivity of the 407
Fe nanowire bundle are shown in Fig. 1. The snapshots of
Fig. 1 represent static magnetic configurations after conver-
gence has been achieved for each field step. If the
in-between magnetic states are monitored during the relaxa-
tion process, it is revealed that the reversal starts by nuclea-
tion at both wire edges and propagation of two domain walls
towards the center. Of course, in bundles of wires nucleation
begins by one of the two edges, whichever is favored by the
interactions. For isolated wires, the loops qualitatively
resemble those of the SW model (for ellipsoids with similar
aspect ratio) and the nucleation field shows an angular de-
pendence similar to that of the SW model, though the values
differ. Thus, these particle assemblies show macroscopically
a magnetic response that can be mistaken for SW particles.
The reversal of the bundle as a whole proceeds by nucle-
ation and propagation along the length of the bundle in a
domino fashion. This can be understood to a first approxima-
tion, by the fact that dipolar interactions tend to align the
magnetic moments of nanowires stacked along their lengths
and, on the contrary, antiparallel when stacked along their
diameters. Thus, dipolar interactions seem to promote rever-
sal in elongated regions since after a region has flipped, it
will tend to destabilize the lengthwise neighboring ones and
stabilize the lateral ones. Considering that this bundle has an
aspect ratio of 10, we can estimate an average demagnetizing
field pNMS¼ 0.013MS¼ 22 kA/m. This low value cannot
explain the huge difference of the nucleation field
HN¼�140kA/m compared to the one of an isolated
143902-2 Panagiotopoulos et al. J. Appl. Phys. 114, 143902 (2013)
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nanowire HN¼�335 kA/m. Thus, for these elongated struc-
tures, nucleation is instigated by local fields and cannot be
directly ascribed to macroscopic demagnetizing factors. Due
to the presence of highly inhomogeneous magnetic configu-
rations and collective reversal, it becomes questionable if
local effective fields can be reconciled by a mean field
approach of the type Heff¼ -NM with a fixed Neff for all the
magnetic configurations. This further poses a question con-
cerning the applicability of the derivation of the response to
the demagnetizing fields under different magnetic circuits
with different demagnetization factors using the zero demag-
netizing field measurement as a starting point. In a way, it is
the opposite process of the demagnetization correction for
which, a typical counter-example is the over-skewed
(S-shaped) loops6 that are obtained if one applies the demag-
netization correction by N¼�1 to a magnetic film sample.
It is known that the use of average homogeneous demagnet-
izing factors is limited to macroscopic samples in which the
details of the local magnetization M(r) can be ignored, while
the inhomogeneous magnetic states which exist in nanostruc-
tured materials create strong deviations.2,6,12 Since this
method has been empirically found to work in macroscopic
objects, addressing this question becomes more compelling,
in the case, where the effect of dipolar fields from a finite
number of nanowires is used to simulate macroscopic
objects. If the limited simulation cell represents in a correct
way the response of a macroscopic magnetic material, the
approximation Heff¼ -NM should give meaningful results.
To address this point, we have compared loops obtained in
bundles with the same p but different aspect ratios. A good
example is shown in Fig. 2 trying to reconcile the magnetiza-
tion curves of two bundles with p¼ 0.67 and AR¼ 1 and
AR¼ 10, respectively by a linear demagnetization factor
correction.
The nucleation field is HN¼�100 kA/m for the
AR¼ 10 bundle and HN¼þ150 kA/m for the AR¼ 1. This
difference of DHN¼ 250 kA/m corresponds to an effective
demagnetizing factor Neff¼DHN/pMS¼ 0.22. Indeed by try-
ing different Neff¼ 0.1 to 0.3 Neff¼ 0.2 seems to be the cor-
rect value to make the curve of the AR¼ 10 bundle coincide
with that of AR¼ 1. The coincidence is restricted in the sec-
ond quadrant (M> 0, H< 0) of the loop, while in the third
quadrant (M< 0, H< 0) sever deviations occur. These would
result in the well-known over-skewing if we were trying to
do the opposite, i.e., to obtain the AR¼ 10 curve by a
demagnetization correction of the AR¼ 1 curve. To fit the
data of the third quadrant, lower N should be used but strong
deviations would still exist. There are two interesting points:
(i) though the HC values seem to differ, the estimation of
BHmax (comparing between AR¼ 1 and Heff corrected
AR¼ 10) is not seriously affected as it is based on the shape
of the loop on the second quadrant away from coercivity (see
discussion below). (ii) The differences of the HN of different
AR bundles seems to give results that can be reconciled with
a choice of an appropriate Neff, in contrast to the comparison
between an elongated bundle and the isolated wire, discussed
in Fig. 1.
An example of demagnetization curves and BHmax cal-
culation is shown in Fig. 3 for the same bundle of 407 Fe
wires with p¼ 0.67. In comparison, the hysteresis curve of
an isolated nanowire scaled to magnetization pMS
FIG. 2. Magnetization curves of two bundles with p¼ 0.67 and AR¼ 1 (2 �187 nanowires, solid circles) and AR¼ 10 (11 � 37 nanowires, diamonds).
The continuous curves are the (H, M) data of AR¼ 10 transformed to
(HþNM,M) for different N.
FIG. 1. Magnetic configurations of an
aggregate of 407 iron nanowires (37
rows of 11 nanowires) from nucleation
(top left) to coercivity (bottom right).
The numbers next to each configura-
tion denote the applied field H in kA/m
and the normalized total magnetization
m¼M/MS. The colors represent the
component of the magnetization vector
along the nanowire axis (red for
m¼þ1 to blue for m¼�1).
143902-3 Panagiotopoulos et al. J. Appl. Phys. 114, 143902 (2013)
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(representing the hypothesis that the wires could be packed
without any HC loss). A first observation is that a coercivity
HC>Mr/2¼ 569 kA/m (i.e., much higher than that of an iso-
lated nanowire HC¼ 335 kA/m) is required to take full
advantage of the BR¼ l0MR¼ 1.43T remanence. Thus, for
Fe wires at this packing fraction, the performance is anyway
HC limited. The BHmax of the Fe wire bundle is estimated to
196 kJ/m3 (circle). The energy product that corresponds to
HC¼ 335 kA/m is BHmax¼ 315 kJ/m3 (indicated by a star in
Fig. 3). Even with HC¼ 220 kA/m, if the loop of the Fe bun-
dle was square, we would get BHmax¼ 255 kJ/m3 (yellow tri-
angle in Fig. 3). In other words not only HC but the
nucleation field HN (the field value at which M departs from
MR) and the loop shape are important for the energy product.
The corresponding example of demagnetization curves
and BHmax calculation for a bundle of 209 Co nanowires
with p¼ 0.7 is shown in Fig. 4. The HC and HN safely exceed
the value of 488 kA/m required to take full advantage the
remanence BR¼ 1.22T.
III. PACKING FRACTION DEPENDENCE OF THECOERCIVITY AND THE ENERGY PRODUCT
As mentioned, in the case of magnets consisting of
packed particles the saturation magnetization is simply pro-
portional to pMS, where MS is the magnetization of the pure
magnetic phase. The main concern is the limitation imposed
through the HCðpÞ and HNðpÞ dependence. There is a scarcity
of experimental work on the HCðpÞ and especially in the case
of high packing fractions, as the published work is mainly
related to recording media.13,14 Thus, the main contributions
on the effect of packing fraction on elongated particles
remain that of Luborksy5 on Co-Fe and Morrish and Yu15 on
iron oxides. These contributions refer to materials that are
not nanostructured and thus deviations from the SW homo-
geneous rotation are not surprising.
Empirically, it has been found that the data can be
described by a relationship of the form
HCðpÞ ¼ Að1� pÞ þ B: (1)
Intuitively, the first term that has been proposed by N�eel,16
can be attributed to the shape anisotropy contribution and the
second to the magneto-crystalline anisotropy. Of course this
kind of assignment can only be approximate. One could
argue that for diameters large enough to favor curling modes
of reversal (for which, in principle, there is no magnetostatic
energy contribution), the HC should be independent of p as
opposed to coherent rotation. The values of A that can be
estimated from the data in literature5,15 are more than 3 times
lower than what is expected from the SW model (A¼MS/2)
indicating that a large part of the shape anisotropy is already
lost due to the large diameter of the particles and does not
contribute to the p dependence. The reported HC dependence
of elongated FeCo particles in Ref. 5 extrapolates to zero
before p¼ 0.8. On the other hand, nickel nanowires grown in
nanoporous alumina templates show very weak coercivity
dependence on packing fraction,17 despite the fact that this
variation is achieved by simultaneous increase of their radii,
which should cause further loss of HC. Interestingly, devia-
tions from the linear relationship have been observed close
to p¼ 0, which seem to follow an exponential decay law,13
but these are not relevant to energy product optimization
considered here. A complication of the experimental studies
in low p comes from the tendency of magnetic particles to
form clusters, which locally increases packing fraction.
The simple relation of Eq. (1) suggests that there are no
BHmax coercivity limitations up to a packing fraction of pc <AþB
AþMS=2and thus, no coercivity limitation at all, for materials
with high enough magnetocrystalline anisotropy to ensure
B > MS=2. Assuming A ¼ MS=2, B ¼ HK ¼ 2K=l0MS; we
get for Co pc ¼ 0:92, while for iron pc ¼ 0:52.
Above pc the optimum packing fraction would be
popt ¼ ðAþBÞAðAþMS=2ÞðAþMSÞ . For needle-like particles of negligible
FIG. 3. Magnetization curves M(H) (open blue circles), B(H) (open red dia-
monds) in the quadrant H< 0, M> 0, and BHmax (solid black circles) for a
bundle of 407 Fe nanowires with p¼ 0.67. The solid lines represent the
same curves for an isolated wire. The dashed line shows the energy product
for the non Hc limited case. The maximum energy product for the Fe wires
bundle is 196 kJ/m3 (red circle). The energy product that would correspond
to the same bundle, if there was not any HC loss due to packing is denoted
by a star. The energy product for a square loop with the same HC (i.e., in the
absence of nucleation effects at HN before HC) is denoted by a triangle.
FIG. 4. Magnetization curves M(H) (open blue circles), B(H) (open red
squares) in the quadrant H< 0, M> 0, and BHmax (solid black circles) for a
bundle of 209 Co nanowires with p¼ 0.70. The solid lines represent the
same curves for an isolated nanowire. The maximum energy product
obtained for H ¼ �MR=2 is denoted by a star.
143902-4 Panagiotopoulos et al. J. Appl. Phys. 114, 143902 (2013)
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magneto-crystalline anisotropy, B¼ 0 and A ¼ MS=2 give
popt ¼ 2=3. For non-zero B, popt ¼ 23
1þ BMS=2
� �which shows
that for any material with B > MS=4, popt> 1 so that the ma-
terial should, in principle, be made as densely packed as pos-
sible. For instance, with the Co bulk parameters, popt > 1,
while in contrast for Fe popt ¼ 0:702.
The results of Nmag simulations for cobalt and iron bun-
dles are summarized in Fig. 5. The coercive field HC and the
nucleation field HN are plotted as a function of p. Their val-
ues are in agreement with those reported in literature: for
D< 15 nm iron nanowires HC¼ 280–320 kA/m at 5 K and
HC¼ 190–220 kA/m at 300 K,12 while for cobalt with
D¼ 6 nm HC � 1000 kA/m at 5 K and �600 kA/m at 300 K
have been have been reported.18 HC and HN show a linear
dependence on p. However (as summarized in Table I),
when fitted to Eq. (1) the values of the parameters A and B
differ considerably from the A ¼ MS=2, B ¼ HK , even if cor-
rected by a factor of aw ¼ 0:766 for the 5� misalignment
according to the well-known expression of the angular de-
pendence of the switching field for SW particles (page 187
of Ref. 2 for instance). Of course such a difference is not sur-
prising as the reversal mechanism differs from the simple ho-
mogeneous rotation SW mechanism. Qualitatively the
results show that, as intuitively expected, low anisotropy
leads to a low B. The nucleation field of Fe nanowires is the
only one that has a dependence close to that predicted by
N�eel’s simple prediction (B¼ 0).
The HC¼MR/2 limit can be estimated by the intersec-
tion of the each set of data with the corresponding pMS/2
line. According to the previous discussion, the intersection
with the HN is also meaningful as nucleation also lowers the
energy product. Above p¼ 0.35 for iron, BHmax becomes
coercivity limited and the magnet has to be supported by an
elongated shape. For instance, at the maximum p¼ 0.7, the
working point must be defined by a low demagnetizing fac-
tor N¼ 0.16 (load line B¼�5.25l0M), compared to N¼ 0.5
(B¼�l0M) in the non-Hc limited case. For Co, this limit is
above p¼ 0.8. As the shape anisotropy related coercivity
seems to persist even at high packing fractions, the realiza-
tion of permanent magnet materials with high anisotropy
materials seems, in principle, feasible.
In Fig. 6, the calculated BHmax values for Co and Fe
nanowires as a function of the packing density are summar-
ized and compared with the ones obtained by the simple pre-
diction that the loops are square and have a remanence
MR ¼ pMScos w and coercivity
HCðpÞ ¼ awMS
2ð1� pÞ þ HK
� �: (2)
For Co, the values are really close to those predicted for this
simple model as coercivity limitations appear at very high
packing fractions. In other words, the loops remain square with-
out any significant nucleation up to fields greater than pMS/2.
For Fe, the deviations are greater but the maximum is still close
to p¼ 2/3 as the magneto-crystalline anisotropy is low.
IV. CONCLUSIONS
Micromagnetic simulations show that it is, in principle,
feasible to achieve BHmax values close to 300 kJ/m3 in Co
nanowires with a packing fraction p¼ 0.7 and close to
400 kJ/m3 at p¼ 0.85. The packing fraction limitations are
essentially non-existing due to the intrinsic magnetocrystal-
line anisotropy of Co. On the other hand, if a low anisotropy
material such as Fe could be produced in the form of fine,
well crystallized wires it could yield a BHmax close to
FIG. 5. Coercivity (HC, solid symbols) and nucleation field (HN, semi-filled
symbols) for cobalt (red diamonds) and iron (black circles) nanowires bun-
dles determined by micromagnetic simulations. The intersections with the
pMS/2 straight lines show the critical packing fractions above which the
BHmax is HC limited.
TABLE I. Comparison of the constants A and B derived by fitting the Nmag
simulation data to Eq. (1) to the shape and magneto-crystalline anisotropy
fields. All values are in kA/m.
Material Field A (calc.) aw � ðMS=2Þ B (calc.) awHK
Co HC 169 453 582 536
HN 263 471
Fe HC 142 651 196 34
HN 262 69
FIG. 6. Energy product as a function of packing fraction for cobalt (red dia-
monds) and iron (black circles) nanowires. The continuous lines show the
calculations under the assumption of square loops with a coercivity given by
Eq. (2).
143902-5 Panagiotopoulos et al. J. Appl. Phys. 114, 143902 (2013)
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200 kJ/m3 at an optimum p¼ 0.7. This value is coercivity
limited and corresponds to a low demagnetization factor
(N¼ 0.15) working point (on the load line B¼�5.25l0M).
As the performance of iron nanowires is solely based on
shape anisotropy it becomes coercivity limited above
p¼ 0.35. If we want to extend the results to other low anisot-
ropy high magnetic moment materials, we can state that this
value amounts to �l0M2S=18 when compared to the upper
theoretical limit l0M2S=12 derived in Ref. 6.
ACKNOWLEDGMENTS
This work was supported from the European
Commission FP7 for the REFREEPERMAG (No. EU
NMP3-SL-2012-280670) project.
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