Professional Documents
Culture Documents
H. ZlJLSTRA
Philips Research Laboratories
Eindhoven
The Netherlands
37
CONTENTS
1. I n t r o d u c t i o n . . . . . . . . . . . . . . . . . . . . . . . . . 39
1.1. G e n e r a l p r o p e r t i e s a n d a p p l i c a t i o n s . . . . . . . . . . . . . . . . 39
1.2. T h e h y s t e r e s i s l o o p . . . . . . . . . . . . . . . . . . . . . 4O
2. Suitability criteria for a p p l i c a t i o n s . . . . . . . . . . . . . . . . . . 42
2.1. T h e e n e r g y p r o d u c t . . . . . . . . . . . . . . . . . . . . . 42
2.2. T h e m a g n e t i c free e n e r g y . . . . . . . . . . . . . . . . . . . 46
3. M a g n e t i c a n i s o t r o p y . . . . . . . . . . . . . . . . . . . . . . 49
3.1. A n i s o t r o p y field a n d coercivity a s s o c i a t e d w i t h m a g n e t i c a n i s o t r o p y . . . . . 49
3.2. S h a p e a n i s o t r o p y . . . . . . . . . . . . . . . . . . . . . . 52
3.3. M a g n e t o c r y s t a l l i n e a n i s o t r o p y . . . . . . . . . . . . . . . . . . 53
4. F i n e p a r t i c l e s . . . . . . . . . . . . . . . . . . . . . . . . . 55
4.1. Critical r a d i u s for s i n g l e - d o m a i n particles . . . . . . . . . . . . . . 55
4.2. B r o w n ' s p a r a d o x . . . . . . . . . . . . . . . . . . . . . . 6O
5. C o e r c i v i t y a s s o c i a t e d w i t h s h a p e a n i s o t r o p y . . . . . . . . . . . . . . 6O
5.1. P r o l a t e s p h e r o i d . . . . . . . . . . . . . . . . . . . . . . 60
5.2. C h a i n of s p h e r e s . . . . . . . . . . . . . . . . . . . . . . 64
6. C o e r c i v i t y a s s o c i a t e d with m a g n e t o c r y s t a l l i n e a n i s o t r o p y . . . . . . . . . . 66
6.1. M a g n e t i z a t i o n r e v e r s a l by d o m a i n wall p r o c e s s e s f o r / * 0 / / A > Js . . . . . . 66
6.2. T h e 180 ° d o m a i n wall . . . . . . . . . . . . . . . . . . . . 67
6.2.1. E n e r g y a n d w i d t h of a 180 ° d o m a i n wall . . . . . . . . . . . . 67
6.2.2. T h e e x c h a n g e e n e r g y coefficient A . . . . . . . . . . . . . . 69
6.3. I n t e r a c t i o n of d o m a i n walls w i t h cavities a n d n o n - f e r r o m a g n e t i c i n c l u s i o n s 74
6.3.1. D o m a i n - w a l l p i n n i n g at l a r g e i n c l u s i o n s . . . . . . . . . . . . 76
6.3.2. N u c l e a t i o n of r e v e r s e d o m a i n s at l a r g e i n c l u s i o n s . . . . . . . . . 78
6.3.3. D o m a i n - w a l l p i n n i n g at small i n c l u s i o n s . . . . . . . . . . . . 78
6.4. D o m a i n - w a l l n u c l e a t i o n at surface defects . . . . . . . . . . . . . 80
6.5. I n t e r a c t i o n of d o m a i n walls w i t h the crystal lattice . . . . . . . . . . 81
6.5.1. W a l l p i n n i n g at r e g i o n s w i t h d e v i a t i n g K and A . . . . . . . . . 81
6.5.2. P i n n i n g of a d o m a i n wall by an a n t i p h a s e b o u n d a r y . . . . . . . . 88
6.5.3. N u c l e a t i o n of a d o m a i n wall at an a n t i p h a s e b o u n d a r y . . . . . . . 93
6.5.4. T h i n - w a l l c o e r c i v i t y in a perfect crystal . . . . . . . . . . . . 94
6.5.5. P a r t i a l wall p i n n i n g at d i s c r e t e sites . . . . . . . . . . . . . 98
7. I n f l u e n c e of t e m p e r a t u r e . . . . . . . . . . . . . . . . . . . . . 100
References . . . . . . . . . . . . . . . . . . . . . . . . . . . 104
38
1. Introduction
39
40 H. ZIJLSTRA
TABLE 1
Examples of machines, devices and components using permanent magnets, classified by four functions
which the magnet can perform.
Function Application
Conversion of electrical in'~o mechanical energy Small electric motors, dynamos, loudspeakers,
and vice versa microphone% eddy-current brakes, speedo-
meters, magnetos
Exerting a force on a ferromagneticaUy soft body Relays, couplings, bearings, clutches, magnetic
chucks and clamps, separators (extraction of iron
impurities, concentration of ores)
B =/~o(H + M ) ,
or
B =/~oH + J ,
PERMANENT MAGNETS; THEORY 41
where M and J are are the local material contributions to the flux density,
respectively called magnetization and magnetic polarization, and H is the con:
tribution from all other sources and is called magnetic field strength. The
quantities H and M are measured in A m -1 (1 A m -1 = 4~r x 10 - 3 0 e ) . The quan-
tities B and J are measured in Vsm -2 or tesla (1 T = 10 4 Gauss). The vacuum
permeability ~0 is equal to 47r x 10 -7 V s A -1 m -t (or Hm-1). Both expressions for B
will be used in this chapter. Although magnetic polarization is the official n a m e
for J it will often be called magnetization.
If the magnetization M or J of a p e r m a n e n t magnet material is plotted as a
function of the applied field H a hysteresis loop is obtained in which the
magnetization is not a unique function of H, but depends on the direction and
magnitude of previously applied fields. A typical hysteresis loop is shown in fig. 1.
The initial magnetization curve starting at the origin is obtained when the
material is in a thermally demagnetized state. If the m a x i m u m applied field H m is
sufficient to saturate the material the loop is referred to as a saturation loop.
When the applied field is reduced the magnetization decreases to the r e m a n e n t
magnetization J,, which is generally less than the saturation magnetization Js. In
an efficient p e r m a n e n t magnet material Jr is usually 0.8-1.0Js. If the material is
subjected to a demagnetizing field (i.e. a negative applied field H ) the mag-
netization is gradually reduced and at a critical field - H = jHc the magnetization
is zero. This critical field jHc is known as the magnetization coercivity and is
defined as the reverse field required to reduce the net magnetization of the
material to zero in the presence of the field. The latter qualifying statement is
necessary because if the field is r e m o v e d the specimen may return to a small
positive r e m a n e n t magnetization J; < Jr. Instead of J we can plot the magnetic
/]I//]
/Z
jHc k .,11] /
Fig. 1. Saturation hysteresis loop for magnetic flux density B as a function of H (drawn) and for
magnetization J as a function of H with initial magnetization curve (dashed).
42 H. ZIJLSTRA
flux density B = / x 0 H + J as a function of H (drawn line in fig. 1). We then obtain the
flux hysteresis loop with remanence Br = Jr and with a smaller value of the coercivity
which is here called the flux coercivity ~Hc. Note that by these definitions the
coercivities are positive numbers quantifying negative field strengths.
It should be emphasized that the coercivities jHc and BHc are assumed to
correspond to demagnetization of the saturated material, though we shall see later
that permanent magnet materials are rarely if ever absolutely saturated even in
exceptionally high fields. Unless otherwise stated, it can usually be safely assumed
that the values of Hc quoted in the various scientific journals, books and papers
refer to the "saturation" values as defined above. In the following the prefix J will
be omitted when jH~ is discussed.
The extent to which a material will be suitable for applications in which electrical
energy plays a part (the first groups in table 1) depends on the amount of
magnetic flux linkage per metre squared and the maximum opposing field that can
be tolerated without loss of polarization.
The product of the flux density B and the associated opposing field H, referred
to as the energy product, is a useful measure of the performance of a particular
magnet, since it is proportional to the potential energy of the field in the air gap.
It is useful only, however, when the magnet is not disturbed by fields from
another source. To determine the energy product it is of course necessary to have
information about the hysteresis loop of the material (fig. 2). A permanent magnet
that is subject only to the influence of its own field will be in a state represented
by a working point in the second (or the fourth) quadrant of the hysteresis loop.
In these quadrants the field is opposed to the flux density, and is referred to as the
demagnetizing field.
It can be shown quite generally that the occurrence of a magnetic field outside
the permanent magnet does in fact relate to a field inside the magnet with B and
Fig. 2. Part of a magnetic hysteresis loop for magnetic flux density B; the shaded area is equal to the
maximum energy product (BH)....
PERMANENT MAGNETS; THEORY 43
curl H = O,
div B = 0.
fn(H. B ) d V = 0, (2.1)
where the integration is performed over the complete space R. If this integral is
written as the sum of the integral over the volume (Rrnagn) of the permanent
magnet and the integral over the rest of the complete space (Rrest), then
Assuming that the space Rrest is " e m p t y " , i.e., contains no magnetic substances,
then the flux density there is given by B =/x0H. The right-hand side of the last
equation is then negative, which is possible only if B and H inside the magnet are
of opposite sense or at least include an obtuse angle at least somewhere. This
result is not affected if Rrest contains soft magnetic material in which B and H
always have the same direction.
It can also be shown directly from what we have said above why the product
BH is a good criterion of quality for the applications considered in this section. If
we assume that any field present in soft magnetic material is negligible, we may
write:
The right-hand side of this equation is twice the potential energy of the field
outside the magnet (i.e. in the air gap). This is proportional to H • B.
The exact location of the operating p o i n t - a n d hence the value of the energy
p r o d u c t - d e p e n d s on the relative dimensions of the magnet and the magnetic
circuit in which it is used.
In the limiting cases of an infinitely long needle of a closed circuit ( H = 0) or of
an infinitely extensive plate (B = 0) the energy product is equal to zero; then there
44 H. Z I J L S T R A
is no external field. Between these two extremes a situation exists in which the
energy product has its maximum magnitude. In the case of the needle-shaped
magnet the demagnetizing field is very weak and the working point is close to the
point Br in fig. 2. The value of the flux density at this point is the remanence. If
the magnet is made shorter and thicker, the working point then moves along the
loop in the direction of the point sHe, which it reaches if the magnet is given the
form of a thin plate magnetized perpendicular to its plane. The demagnetizing
field then has its maximum value and exactly compensates the magnetization. In a
properly dimensioned design the energy product will thus assume a maximum
value, ( B H ) .... which is determined solely by the material used. The suitability
criterion sought has thus been found.
The product can be represented by the area of the shaded rectangle in fig. 2; its
magnitude is equal to twice the total potential energy of the field produced
outside the magnet divided by the volume of the magnet. The higher the
remanence, the greater the coercive force and the more convex the hysteresis loop,
the greater is the value of the product. For an ideal magnet, i.e., a magnet that
maintains the saturation value Js of its polarization in spite of the presence of an
opposing field H, the hysteresis loop in the second quadrant is formed by a
straight line going from the point where H = 0, i.e., where B = Br = Js, to the
point where - H = BHc = Js/l~o. The maximum energy product is then given by:
1
(BH)max = 4/x~ j 2 . (2.3)
To reach this maximum it is sufficient if the magnet maintains its saturation until
the opposing field reaches the value -½JJl~o. A further improvement in the energy
product is then only possible with materials that have a higher saturation value J~.
The highest known saturation value at room temperature is shown by an FeCo
alloy (2.4 T); from this value the theoretical energy product could be as much as
1150 kJm -3 (144 MGOe). However, the coercive force of this alloy is very low, which
makes it unsuitable for permanent magnets.
Figure 3 shows the improvements achieved in maximum energy products over
the years, the record values being indicated on a logarithmic scale. It is interesting
to note how closely the curve approximates to an exponential development.
Once the material and thus the hysteresis loop and the (BH)max value are given,
the magnet system has to be designed to make optimum use of the material
parameters. Very schematically this is done as follows:
Consider a permanent magnet system as drawn in fig. 4. The magnet has a
length Im and cross-sectional area Sin. The air gap has a length Ig and cross-
sectional area Sg. The pole pieces are assumed to have infinite permeability
( H = 0 at finite B). The fields H and B are assumed to be uniform in the magnet
body and in the air gap. For simplicity the field spread outside the magnet and the
air gap is taken to be zero, although this is certainly not true in the given
arrangement. We then have from flux continuity
BmSm = - B g S g ,
PERMANENT MAGNETS; THEORY 45
I00C
k Jim 3 //
50C /
/
j11
(BH)mox
20C
, ~10
100
50 j zt ~
20
10
//
/
5 /
/
//
1
I
880 19'00 1920 19 0,960 1 80
Fig. 3. Historical trend of the maximum energy product (BH)mx achieved experimentally since the
year 1880; (1) carbon steel, (2) tungsten steel, (3) cobalt steel, (4) Fe-Ni-AI alloy, (5) 'Ticonal II', (6)
'Ticonal G', (7) 'Ticonal GG', (8) 'Ticonal XX' (laboratory value, Luteijn and de Vos 1956), (9)
SmCos, (10) (Sin, Pr)Co5 (laboratory value, Martin and Benz 1971), (11) Sm2(Co0.85Fe0.11Mn0.04)17
(laboratory value, Ojima et al. 1977). The energy in MGOe is found by dividing the value in kJm -3 by 7.96.
1
Ig
s/[
Fig. 4. Permanent magnet system with pole pieces. S m and Sg are the cross-sectional areas of the
magnet and the air gap respectively, and Im and lg their respective lengths.
46 H. ZIJLSTRA
Hmlm - G i g = O,
where the positive direction for H and B is taken to the right. From these
equations it is easily found that
H m = Hglg/Im,
and
B m = - tzoHgSg/ Sm
B m / H m = - tZoSglm / Smlg .
The latter expression shows that the reluctance of the system and hence the
working point of the magnet is entirely determined by the dimensional ratios of
the yoke. Allowance for finite permeability of the pole pieces and for flux leakage
can be made by factors o~ (resistance factor) and /3 (leakage factor) so that the
equations for magnetomotoric force and the flux in the air gap are written as
HgLg = otHmLm,
BgSg = - /3BmSm .
For good designs c~ may have values between 0.7 and 0.95 and/3 between 0.1 and
0.8. Detailed discussions of these factors have been published by Edwards (1962)
and by Schiller and Brinkmann (1970).
TdS + dA = dU.
The term T dS, the product of the absolute temperature T of the system and the
change of its entropy S, is equal to the amount of heat supplied to the system
from the environment. In addition the environment performs on the system an
amount of mechanical work dA, taken as positive. This sign convention for the
mechanical work performed is employed for systems in which magnetic effects
occur. Both amounts of energy are spent on the increment d U of the internal
energy of the system. The free energy F of the system is defined by
F=U-TS.
dF = dA- S dT.
dF = dA.
In a system that contains magnetic material the main problem is to find the
correct expression for the mechanical work.
The criterion used for the suitability of a magnetic material for applications of the
type we are now considering is the maximum possible reversible change of its
magnetic free energy. This value is usually calculated per unit volume of the magnet.
The mechanical work d A associated with an infinitesimal change of the
configuration is equal to
dA ½f_ (H. dS - S . d H ) d V,
magn
where the integration is performed over the part Rmagn of the space occupied by
the material. T o derive this expression for the mechanical work, let us imagine a
number of bodies of various magnetizations arranged in a particular configuration.
We assume that the bodies are situated in each other's magnetic field and that
their temperature remains constant. A slight change in the configuration causes a
change in the fields and hence in the polarizations. For each body the increase in
the magnetic free energy consists of a quantity dFp, connected with the build-up
of the polarization in the material, and a quantity of interaction energy dF~,
since in a field H a piece of material with the polarization vector J possesses the
potential energy, - ( J • H). For the body considered we can now write:
d F = dFp+ d E = H . d d - d ( J - H ) .
48 H. ZIJLSTRA
T o find the change in the free energy of the whole system we must perform a
summation over all the bodies. The contributions from the interaction energy
would then be counted twice, but putting a factor 1 in front of them corrects for
this. The total increase in the free energy is therefore
where both summations are made over all the bodies. Using the above expres-
sions for dFp and dF~ and applying the expression d F = d A for isothermal
changes, we obtain the required expression for the mechanical work, calculated
per unit volume of the material.
W e should note here that the energy change H - d J is positive, because the
structure of the material offers a certain resistance to the change of the polariza-
tion. The interaction energy, - ( J • H ) , has a minus sign because it is customary to
take this energy by definition equal to zero for two bodies that are an infinite
distance apart.
If the polarization vector in the expression for the mechanical work is replaced
by the equivalent quantity B -/~0H, then, after integration,
d A = ½fu ( H . dB - B . dH) d V.
magi
B/
P Br
S
Fig. 5. Part of a B hysteresis curve in the second quadrant. The area of the sector OPQ represents the
change in magnetic free energy when the working point moves from P to Q.
PERMANENT MAGNETS; THEORY 49
these applications is one in which the working point can move reversibly from
remanence over the greatest possible extent of the hysteresis loop. For an ideal
magnet, where the complete (linear) hysteresis branch in the second quadrant is
transversed reversibly, the maximum mechanical work made available per unit
volume during a change of configuration is given by:
½B~BH~ = (1/2/Xo)J 2 •
3. Magnetic anisotropy
Wk = K sin 2 q~,
where ~0 is the angle between the easy axis and the magnetization vector. In the
presence of a f i e l d / - / a l o n g the easy axis we assume that the magnetization vector
is rotated through an angle ~p as shown in fig. 6. In this state the total magnetic
energy is
1 2
W = g/x0Ms + K sin 2 q~ +/x0HMs(1 - cos q~).
Note that the first term, which is the magnetostatic energy of the magnetized
sphere, is independent of the angle q~ because the demagnetization factor of the
sphere is isotropic and equal to ½. For a minimum in the energy W corresponding
to a stable position of the magnetization vector we require
dW d2W > 0.
d~ - 0 and d~ 2
easy
axis
Ms
H > -2K/IxoMs.
Hc = 0.48HA
-1 0 1
I I I r I I I I I I I I [ I
0 0,10,90
1
M/M s
T
¢' 0
-1
0,10,90 0
I I I I I I I I I I I I
-1 0 ~ h 1
Fig. 7. Hysteresis loops for uniform rotation of the magnetization in a crystal with one easy axis for
the magnetization, with the orientation angle (in degrees) between easy axis and direction of applied
field as a parameter (Stoner and Wohlfarth 1948).
1.0
f Y
Sf
0.5 M/Ms
-0.5
-1.0
:-1.5 -1.0
f ~ 0..=
J
0 0.5 1.0 1.5
Fig. 8. Hysteresis loop and initial curve for an array of non-interacting identical particles with one easy
axis, oriented at random (Stoner and Wohlfarth 1948).
52 H. ZIJLSTRA
interior. This may give rise to a magnetic anisotropy experienced only by these
superficial atoms, causing the spins to be oriented normal to the surface, or in
other cases, tangential to the surface. In a non-spherical crystal this leads to a net
anisotropy effect which, of course, becomes smaller with increasing size of
the crystal. The underlying theory has been treated by N6el (1954) and the effect
may contribute somewhat to the shape anisotropy of heterogeneous elongated
particle magnets like alnico. A similar kind of "surface anisotropy" has been
observed by Berkowitz et al. (1975) on fine ferrite particles covered with a
monomolecular layer of oleic acid.
Another interfacial type of anisotropy was discussed by Meiklejohn and Bean
(1957), namely, exchange anisotropy. It occurs when an antiferromagnetic crystal
with high anisotropy and a ferromagnetic crystal constitute one solid body such that
the spins on either side of the interface are coupled by exchange forces. The
(non-magnetic) antiferromagnetic crystal then imparts its anisotropy to the ferro-
magnetic crystal. The effect has been observed with small cobalt spheres covered by
an anisotropic antiferromagnetic oxide layer.
Shape anisotropy refers to the preference that the polarization in a long body has
for the direction of the major axis. The effect, which does not arise from an
intrinsic property of the material, can easily be described in the case of a prolate
ellipsoid. It is assumed that the ellipsoid is homogeneously magnetized in a
direction that makes an angle ~0 with the major axis (fig. 9). The demagnetizing
/
I
/
I
I
I
!
I
I
I
field Ha due to the magnetic poles at the surface is also homogeneous within the
ellipsoid. Along each of the three principal axes of the ellipsoid we can apply one
of the relations
I.l"ondi = -- NiJi ,
where i is the number of the principal axis; the coefficients N~ are the demag-
netization factors. In the case of a prolate spheroid we have the "parallel"
demagnetization factor NIl for the direction parallel to the axis of revolution and
two "perpendicular" demagnetization factors Na, which, for reasons of symmetry,
are identical. Using eq. (2.1)
f (H.B) dV=O,
it can easily be shown that the energy Em of the demagnetizing field, which is
given by
Em = II.~OIR n 2 d V ,
depends in the following way on the parameters that describe the situation:
In this expression Rmagnis the volume of the ellipsoid. The coefficient of the
directionally dependent part of the equation describes the shape anisotropy. For
small values of the angle ~0 we find from this an effective anisotropy field
HA = (N±- Nfl/~0 •
In the case of a long bar (needle) this field HA approximates to the value J/2l~o. If
the bar consists of iron (Js ~ 2 Wbm -2) it follows from the foregoing that HA
106Am -1 (~104Oe). This is the value of the coercive force when the mag-
netization is rotated uniformly.
Magnetic materials which derive their hardness from shape anisotropy consist of
a fine dispersion of magnetic needles in a matrix of non-magnetic or weakly
magnetic material, like alnico (fig. 10).
There are three situations that give rise to magnetic anisotropy as an intrinsic
crystal property. The first and most important one is that in which the atoms
possess an electron-orbital moment in addition to an electron-spin moment. In
54 H. ZIJLSTRA
Fig. 10. Microstructure of an alnico magnet. The alloy consists of a precipitate of elongated particles
(approx. composition FeCo, average thickness 30 nm) in a matrix of approx, composition NiA1. Left:
plane of observation parallel to the easy axis. Right: perpendicular to the easy axis. (Electron
micrograph of 'Ticonal XX' magnet steel (De Vos 1966).)
such a situation the spin direction may be coupled to the crystal axes. This arises
through the coupling between spin and orbital moments and the interaction
between the charge distribution over the orbit and the electrostatic field of the
surrounding atoms. There will then be one or more axes or surfaces along which
magnetization requires relatively little work. The crystal will then be pref-
erentially magnetized along such an easy axis or plane.
The second situation is encountered in non-cubic crystal lattices. In these
crystals the magnetostatic interaction between the atomic moments is also aniso-
tropic, which may give rise to easy directions or planes of magnetization.
The third possibility of crystal anisotropy is found in the directional ordering of
atoms as described by N6el (1954). This typically involves solid solutions of atoms of
two kinds, A and B, linked by the atomic bonds A - A , A - B and B-B. In the presence
of a strong external magnetic field the internal energy of these bonds may be to some
extent direction-dependent. Given a sufficient degree of atomic diffuson - as a result
of raising the temperature, for example - a certain ordering can be brought about in
the distribution of the bonds; in this way it is possible to " b a k e " the direction of this
field into the material as the easy axis of magnetization.
In addition to these sources of magnetocrystalline anisotropy mechanical stres-
ses may contribute through the magnetoelastic (magnetostrictive) properties of
PERMANENT MAGNETS; THEORY 55
4. Fine particles
TABLE 2
Comparison of anisotropy field HA and coercivityshe of various
permanent magnet materials.
HA jnc
We = A(V~p) 2 .
W r = K sin 2 ~ ,
/ I.l,o A \ 1/2
Rco = 5.099~-~s2 ) •
A ~ 2 x 10 -11Jm -1 ,
we find that
Rc0(iron) = 13 n m (130 ~ ) .
O b
Fig. 11. Demagnetization modes of a sphere. (a) Magnetization curling. (b) Two-domain state.
PERMANENT MAGNETS; THEORY 57
In order to calculate the critical radius above which the magnetization is non-
uniform we must distinguish between two cases:
(1) The material has a low magnetocrystalline anisotropy energy density. In this
case the energy associated with the uniform magnetization state is compared with
the non-uniform magnetization state known as "curling". The latter is considered
to have the l o w e s t energy because the curling mode (shown in fig. ll(a))
minimizes the sum of the magnetostatic, anisotropy and exchange energies.
(2) The material has a high magnetocrystalline anisotropy energy density. In
this case the energy associated with the uniform-magnetization state is compared
with the two-domain state having a single plane wall as shown in fig. ll(b).
Unfortunately the micromagnetic theory does not generate the magnetization
configuration that has the lowest energy, so that the non-uniform states as
mentioned have been chosen on the assumption that they have the lowest energy.
Simple calculations suggest that this is probably correct.
K<O.1781J~/~o
or
Wm = (1/6/x0)J 2 .
R > RCl ,
where
64053 ~---~ m 1 - 5 . 6 1 5 0 ~ 2 K ) -1
K > 0.1781J~/~0,
in which case the two-domain state shown in fig. 11(b) has a lower energy than the
uniformly magnetized state provided that the particle radius
58 H. ZIJLSTRA
R > Rc2,
where
Note that when R > Rc2 the two-domain state has a lower energy than the
uniformly magnetized state even when the material has a low magnetocrystalline
anisotropy density.
102
two doma ~s
10
curling
Fig. 12. Ratios of upper bounds beyond which magnetization curling occurs, Rcl (curve a) or the
two-domain state has the lowest energy, Rc2 (curve b), both with respect to the lower bound Rc0,
below which the uniform state is stable, as a function of the reduced magnetocrystalline anisotropy
x = t.LoK/J~. T h e critical radius separating uniform from non-uniform behaviour (Kittel's ap-
proximation) is also given as its ratio with Rc0 (curve c).
PERMANENTMAGNETS;THEORY 59
uniformly magnetized sphere. H e finds the latter to have lowest energy when
where the domain wall energy 3' = 4X/A-K. H e has assumed that the mag-
netostatic energy of the two-domain state is approximately half of that of the
uniformly magnetized state. The critical radius as determined by Kittel (1949) can
be compared with Rc0 as determined by Brown as follows:
R (Kittel) _ 3 6 / x 0 X / ~ / 5 . 0 9 9 ~ / / x 0 A
Re0 " / Z
/ p, o K \ 1/2
= 7.06~-2 ) .
The ratio R(Kittel)/Rco is also shown in fig. 12 and plotted as a function of the
parameter x = t~oK/J~. This line fits reasonably well between Brown's upper and
lower bounds but is certainly incorrect for values of x < 0.02. Note that in all the
above calculations of ratios of Rc~, Re2 and R (Kittel) with respect to Rc0 no assump-
tion has been made about the value of A.
From the above discussion it will readily be appreciated that single domain
particles, i.e., particles with radius R < Rc0, are necessarily uniformly magnetized
but that particles with R >Rc~ or R > R c 2 are not necessarily non-uniformly
magnetized. Although the latter particles can be uniformly magnetized, the
energy of that state is higher than that for the non-uniform state. Thus the
uniformly magnetized state may persist if there is an energy barrier between this
and the non-uniform state. This is true for a perfect single crystal in which the
nucleation of a domain wall requires a finite energy for nucleation (see section
4.2). It is also possible for particles with R < R c 0 to contain domain walls
provided they contain lattice defects where the domain wall energy is lower than
that in the surrounding matrix. The coercivity is determined by the height of the
nucleation energy barrier and hence by the presence of lattice defects and the
particular magnetic spin structure of the material (see section 6.5.3). The presence
of superficial features, such as scratches and sharp edges, may also influence the
coercivity owing to the associated local demagnetizing fields, which may assist
domain wall nucleation (see section 6.4). The coercivity can also be determined by
domain wall pinning at the lattice defect (see section 6.5.2). The behaviour of the
sphere for radii between Rc0 and Rcl or Rc2 is unknown, but it cannot be
excluded that the magnetization alternates from the uniform to the non-uniform
states. The region between Rc0 and Rcl or Rc2 is associated with the upper and
lower bounds to the magnetostatic energy of the non-uniform states (Brown
1962b). If this energy is zero as is indeed the case for a cylindrical bar which
demagnetizes by the curling mode, the calculation is exact, and Rc0 and Rc~
coincide and therefore correspond to a single critical rod radius (Frei et al. 1957)
(see also section 5.1).
60 H. ZIJLSTRA
For high anisotropy a supercritical (R > Rc2) sphere has the non-uniform multi-
domain mode as the lowest energy state. However, if the particle happens to be in
a uniform state it cannot spontaneously transform to the lower energy state. For
this a wall has to be nucleated, which means that one or several spins must start
rotating.
Consider one particular spin. It is subjected to an effective field H which is
composed of
where H A is the anisotropy field; Hw is the Weiss field, accounting for the
exchange interaction between the spin and its neighbours; Ha is the demagnetiz-
ing field; He is the externally applied field.
For instability of the spin it is required that
Now Hw is of the order of 10 9 A m -1 which far outweighs any practical value that
Ha or He could reach. The conclusion is that the uniform magnetization is
maintained under all circumstances and that when
- H e > HA
H~=Ha,
which is in obvious contradiction with experiment (see table 2). This inconsistency
which is referred to as "Brown's paradox" (Shtrikman and Treves 1960) is solved
by considering that lattice defects are able to reduce Hw considerably and even
reverse it locally. Also HA can be influenced by a defect as the symmetry of the
crystal is disturbed locally. Finally sharp edges and scratches can locally increase
Ha. These matters are discussed in more detail in sections 6.4 and 6.5.
From calculations using micromagnetic theory Frei et al. (1957) and Aharoni and
Shtrikman (1958) have shown that magnetization reversal of a prolate spheroid
may occur by three basic mechanisms. These are:
PERMANENT MAGNETS; THEORY 61
(a) Uniform rotation of the magnetization for which the coercivity is equal to
the anisotropy field
where N~ and N]I are the demagnetization factors perpendicular and parallel to
the major axis of the spheroid (see also sections 3.1 and 3.2).
(b) Magnetization curling (see figs. l l ( a ) and 13(a)) for which the coercivity is
Hc=k Js 1 (5.2)
2/Zo p2,
Js > 1 . 3 9 Js 1
3tZo 2/Xo p 2, (5.3)
where the left-hand member is the self-demagnetizing field of the sphere and the
£1 b c
Fig. 13. Demagnetization modes of the infinite cylinder: (a) curling; (b) twisting; (c) buckling.
62 H.' ZIJLSTRA
right-hand member follows from eq. (5.2) with k = 1.39. This is rewritten as
p2 > 2.09,
or
/ lzoA \ 1/2
R > 5.121--=~/
which is about the result obtained by Brown (1969) for the critical radius of a
sphere (see section 4.1).
It is interesting to note the similarity between the quantity R0 and the thickness of a
domain wall. As discussed in section 6.2.1, the wall thickness 6 is determined by the
exchange energy competing with the anisotropy energy, so that 3 c~ ~/--A/K. In the
present discussion we deal with a balance between exchange energy and mag-
netostatic self-demagnetization energy, the latter being proportional to J2/iXo. If we
substitute this for K in 6 we obtain
{ l~oA "ll/2
6 oc\ j2 ] o:Ro.
1
Hc = ~ Js(1 - p ) . (5.4)
/-/xo
For a derivation of this result see Compaan and Zijlstra (1962). Thus in any
assembly of particles the hysteretic behaviour will be determined by the mag-
netization reversal mechanism which has the lowest coercivity (see fig. 14). In all
the above cases the particles remain uniformly magnetized until the reverse field
PERMANENT MAGNETS; THEORY 63
Uniform r o t a t i o n
Buckling or
twisting
0.2 HC/HA
o, l Curling
0.05
0.02
~- R / R o
0.01 I i i t
0.2 0.5 1 2 5 10 20 50
Fig. 14. R e d u c e d coercivity He/HA due to various demagnetization m o d e s of the infinite cylinder as a
function of reduced radius R/Ro.
which is obtained by putting Hc of eq. (5.4) greater than Hc of eq. (5.2). The
critical radius for an isolated cylinder is
/ i,~oA \ l/2
Rc = 3.68~---f{-2) .
If we assume that for iron A = 2 x 10-'1 Jm -1 (Kittel 1949) and Js = 2 T, the critical
radius for an isolated infinite cylinder is 9 x 10-9m. For an assembly of iron
cylinders with a packing density p = 2 (as it occurs for example in alnico 5)
Rc ~ 16 x 10-9 m. The measured coercivity Hc for alnico 5 is about 5.5 X 104 A m -1.
64 H. ZIJLSTRA
a b c
Fig. 15. Demagnetization modes of the chain of spheres: (a) symmetric fanning; (b) parallel rotation.
For comparison the uniform rotation mode of the prolate spheroid of the same dimensional ratio is
also indicated (c).
PERMANENT MAGNETS; THEORY 65
The coercivities of these models are compared with those of prolate spheroids
of the same length-to-diameter ratio. The three models are shown in fig. 15. The
symmetric fanning appears not to provide the lowest energy barrier owing to end
effects that have been ignored. Taking these into account leads to a modified
fanning process, called asymmetric fanning. The results of the calculations for a
system of non-interacting elongated particles oriented at random are given for the
various mechanisms mentioned as a function of the length-to-diameter ratio (fig.
16). The experimental points refer to samples consisting of electrodeposited
elongated particles (Paine et al. 1955) with diameters lying between 14 and 18 nm.
Coercivities are in good agreement with the asymmetric fanning model. However,
this might be a fortuitous agreement, since the experimental spheres have
certainly more than a point-like contact, and possibily exchange interaction
between the spheres has to be reckoned with. The mechanism must then be
something between symmetrical fanning and magnetization buckling as described
in section 5.1.
b
0
I I I
~- Elongation
Fig. 16. Coercivity of fine-particle iron oriented at random as a function of particle elongation. Chain
of spheres model: (a) parallel rotation; (b) symmetric fanning; (c) asymmetric fanning. Prolate
spheroid model: (d) uniform rotation. The points refer to experiments (Jacobs and Bean 1955).
66 H. ZIJLSTRA
Hn ~H
IHnl>lHpl
b
J
Hp Hn ~H
J IHnl<lHpl
Fig. 17. Hysteresis loops in relation to nucleation field H. and pinning field Hp: (a) Coercivity
determined by H.; (b) Coercivitydetermined by Hp.
PERMANENT MAGNETS; THEORY 67
,~ oo-o.--=
B C ':"
P I
-115 -1.10 0.~ H 1'10 L (MA/rn)
1.5
Fig. 18. Hysteresis loop of a SmCo5 particle of 5 i~m size. After magnetizing in a strong positive field a
wall is nucleated at an applied field of about -0.6MAre -1 (point A) or at an internal field of
-0.8 MAm-1 (due to the self-demagnetizing field of -0.2 MAm-1). The internal curve measured after
applying a weaker positive field reveals wall nucleation at zero applied field and subsequent wall
detachment at about -0.35 MAre-1 applied field (point B) which means a pinning field of 0.55 MAm-~
for this particular pinning site. The curve C demonstrates the absence of strong pinning sites in a large
part of the crystal (Zijlstra 1974).
easy
axis
I
I
We=A/d ] 2 (6.2)
d2~
K sin 2q~ - 2A ~ = 0,
stating that the torque is zero everywhere. Multiplying by dq~/dx and integrating
from -oo to x we find
K s i n 2~0=
A{d~] 2
\~-x] ' (6.4)
stating that the energy density due to magnetic anisotropy equals that due to
exchange interaction everywhere. The relation between q~ and x follows by
integration to be
------7------ y~
Y
0
6 Ii-
Fig. 20. Distribution of spin orientation angle q~across a 180° domain wall (schematic). The width 6 of
the wall is defined after Lilley (1950).
The wall energy is calculated by substituting WK for We in eq. (6.3) and shifting
from x to ~0 as a variable using eq. (6.4):
y = 2V'A-K
L sin ~ dq~ = 4X/A--K. (6.6)
Equations (6.5) and (6.6) are derived under the assumption m a d e in eq. (6.2) that
the magnetization is continuous, i.e., the discreteness of the lattice of magnetic
atoms is ignored. This is generally allowed provided that x0 is large c o m p a r e d with
the lattice p a r a m e t e r or the distance between magnetic nearest neighbours.
However, this approximation gives rise to errors when x0 approaches the lattice
p a r a m e t e r a, i.e., when a2K becomes comparable with A. This case of very strong
anisotropy is treated in section 6.5.4.
When a wall is pinned an applied field causes a contribution to the wall energy
which is treated in section 6.5.2.
6.2.2.1. Determination of the exchange energy coefficient A fro m the Weiss internal
field model of ferromagnetism. The Weiss internal field model describes the
ferromagnetic interaction between localized spins in a regular lattice. A particular
spin i is aligned with its nearest neighbours by an effective field per nearest
neighbour j
H,,j = N M / Z ,
70 H. Z I J L S T R A
where N is the Weiss field constant, M the magnetization of the crystal and Z the
n u m b e r of nearest neighbours or coordination number. Consider the spin pair i, L
each spin having a magnetic m o m e n t / z . They differ in orientation by an angle Aq~.
The exchange energy change associated with this orientation difference can be
written as
N M , ,t ,,2
wi~ = ~ - / x t a q ~ ) .
NM *2 [d~o'~2
wij = - ~ - ~t c o s 2 ,~ \ ~ x x ] "
13
NM a 2 [dq~ ,~2
w,j = ---fg- ~ T Td;x ] "
Per unit cell of volume a 3 there are 8 such pair interactions and two atoms
contributing with 2~//z0 to the magnetization M. Substituting this and dividing by
the cell volume results in the exchange energy density We due to the angular
gradient d~/dx:
N M 2 az{d~ ~2
We= ~ o ~ \~xl "
PERMANENT MAGNETS; THEORY 71
Cl
(b) Face-centred cubic (fcc, fig. 22). For an fcc lattice the n u m b e r of nearest
neighbours is 12, of which 8 with cos2A = ½ and 4 with cos2A = 0. The nearest
neighbour distance is ~: = ½a~/2 in all cases.
Per unit cell there are 24 pair interactions and 4 atoms. Weighting the
interactions with their proper values of cos2A we find the exchange energy per
unit volume
NM 2 2/d~\ 2
We =/z0 ~ a I~x-x,] .
(c) Simple cubic (sc, fig. 23). For an sc lattice the n u m b e r of nearest neighbours
9i
i
i
i i
i i PF
O-- • - :g-'- - -O
~×
Q,,
6
NM 2 a2{d~o'~2
We = ~ o - i ~ \dx-x/ "
(d) Hexagonal close-packed (hcp, fig. 24). For an hcp lattice the coordination
n u m b e r is 12. The nearest neighbour distance sc = a in all cases. Per unit cell there
are 23 pairs, which are tabulated below together with the proper value of cos2A
and the part p for which they have to be attributed to the unit cell under
consideration (table 3). There are two atoms in this cell contributing 2/x/~0 to the
72 H. Z I J L S T R A
-~ - -..-- - i- ; . ~
O- . . . . . -O-/- - / f ' -
0 / ~\
¢_~J \
~X
magnetization. With these data we find for the exchange energy density
N M 2 a2[ d~o,~2
w° = ~°-J3-- \TX-x] "
NM2.2{d~ \2
we = .
This is not the case when we expand the structures along the vertical axis in order
to obtain tetragonal symmetries from the cubic structures or to deviate from the
close packing in the hexagonal case. In all these cases, however, the expressions
TABLE 3
Interactions in an hcp cell.
F r o m centre plane 4 ¼ 1 1
to upper and lower
planes 2 0 1 0
1
In centre plane 3 1 ~ 1
2 ¼ 1 g
2 ¼ _2 1
3 3
1
In upper and 2 1 g 1
1
lower planes g ¼ ½
Total contribution 4
PERMANENT MAGNETS; THEORY 73
Ew = ½1~oNM2
w~j = -2J$~ • ~ ,
where St and Sj are spin vectors of two neighbouring atoms and J is a coefficient
called the exchange integral. For J > 0 parallel spins have minimum energy,
resulting in ferromagnetic coupling. We suppose an angular gradient d~/dx to be
present along the x-axis. The coupling energy between spins i and j can then be
written as
(d~'~ 2
Wi] = J S 2 ~ 2 COS2 a \ ~ X ] '
where sc is the distance between the spins, A is the angle between their connecting
line and the x-axis, and the moduli of the spin vectors are assumed equal. In the
same way as in the previous section these energy contributions are added for the
various spin pairs in a crystallographic unit cell. We then find for the exchange
energy density,
2 J S 2 {d~o'~ 2
bcc: We = - - 7 - ',~X ] '
4JS z {d~o"~2
fcc: We = - - 7 - - \d--x-x) '
JS 2 {dq~'~2
SC: we = --a- \ ~ x x j ,
JS22~/ 2 [ d~o'~2
hcp: W e - a k~xx] "
the same factor a, as only the cell volume increases by this factor and the rest
remains the same.
The coefficients thus derived are usually written as A, e.g., by N6el and Kittel,
or as C = 2A by Brown. They are associated with the Curie t e m p e r a t u r e Tc and can
be determined by calorimetry, spin-wave resonance m e a s u r e m e n t s or t e m p e r a t u r e
dependence of magnetization. A difficulty is that the models discussed here are based
on nearest neighbour interaction, although there is much experimental evidence that
interactions at a longer range cannot be ignored. Therefore determination of A will
seldom be better than an indication of the order of magnitude. Using the
approximate relation
A~105~ZTc, (SI),
with A in J/m, ~ the nearest neighbour distance in meters and Tc the Curie
temperature in Kelvin, fulfills most requirements in the present context. In cgs
units we have A in erg/cm, ~ in cm and Tc in Kelvin, for which the relation
becomes
A ~ 106~2Tc, (cgs).
radius p
0
0 © ©
0 )
d
0 )
t
Domain Wall
Fig. 25. Cubic array of spherical cavities interacting with a rigid domain wall.
PERMANENT MAGNETS; THEORY 75
the total volume of the material. The n u m b e r n of spheres per unit volume is
3
n = 0, 4 . / r p 3 ,
The distance d between the centres of the spheres on any (100) plane is given by
/4,B-'~ 1/3
F = r~
.~2/3g
Jm •
d W = n2/3fm dx + 2J~H d x .
( 3 )2/3fm0,2/3
Hc = \~-~] ~. (6.7)
The above model has been used by Kersten (1943) as the basis of a simple
theory of coercivity. Kersten assumed radii of the spheres to be much larger than
the domain wall width, i.e., p ~> 6, so that the wall can be regarded as a plane of
zero thickness. When a sphere is intersected by a planar domain wall, which is
also assumed to be rigid, the pinning force is due to the change in the wall
energy which occurs because an area ~rp2 is r e m o v e d when the wall intersects a
sphere through a diameter. However, it should be appreciated that the pinning
force is a m a x i m u m at the edge of the sphere where the rate of change of the wall
energy with position d y / d x is a maximum. For a sphere of radius p the area of
intersection with a plane domain wall changes at a m a x i m u m rate of 2~p so that
the m a x i m u m pinning force fm per sphere is
f~ = 2~-py.
76 H. Z I J L S T R A
Hence the coercivity for a simple cubic lattice of these spheres is given by
3 )2/3 ~-y
He=
_
4~r
_ _ _
pJs 'x
^ 2/3
" (6.8)
Unfortunately the above result does not agree with the experimental values for
ferromagnetic materials which contain dispersions of non-ferromagnetic particles,
principally because the effect of the magnetostatic energy due to the surface poles
has been omitted. When the spheres, each of volume V, are not intersected by a
domain wall the magnetostatic energy is
1 2
m = g/toMs V,
but when they are intersected across their major diameters the above magnetostatic
energy is reduced by a factor of about 2 (N6el 1944b). This magnetostatic energy
variation may not be negligible in comparison with the change in the domain wall
energy. Furthermore the assumption that the domain walls are rigid is unrealistic and
makes the model strongly dependent on the shape of the inclusions.
W m = l g/x0Ms47rp/3.
2 3
When the sphere is intersected by a plane domain wall through its centre the
above magnetostatic energy is reduced by a factor of about 2, i.e.,
AW m 9171"[.ZoIVl
. # 2s P 3•
A rigid wall moving through the crystal will have minimum energy when it
intersects the spherical hole just through the centre. The force required to move it
away from the centre is
f = d(Wm+ W~)
dx
where W~ is the contribution of the wall energy to the total energy. N6el (1944b)
has numerically calculated the energy Wm as a function of wall position x and the
PERMANENT MAGNETS; T H E O R Y 77
which maximum is attained when the wall is just tangent to the sphere• With eqs.
(6.7) and (6.8) we then find for the rigid wall pinned by a cubic array of spheres
Note that the magnetostatic term is independent of sphere radius and that the
wall energy term is inversely proportional to p. There is a critical radius pc, below
which the surface energy term is dominant, and thus Kerstens theory becomes
applicable.
Above pe the magnetostatic term is dominant and N6eI's theory must be
applied. The critical radius is
pe ~ ~o~/Y~ •
This value is exactly the same as that derived by Kittel (1949) for the radius below
which a ferromagnetic sphere is uniformly magnetized in its lowest state (see
section 4.1).
In order to test the validity of eq. (6.9) we substitute the parameter values of a
typical rare-earth magnet and of iron (see table 4). We then obtain for the
rare-earth magnet, with a = 0 . 1 and p = 1 0 - 6 m , H e ~ 1 0 4 A m -1, which is by
several orders of magnitude too low as compared with experiment. The coercivity
of these magnets is obviously not determined by wall pinning at large inclusions•
More likely models are discussed in sections 6.3.3 and 6.5. For iron with the same
dispersion of inclusions we find He ~ 105 Am -1, which is far too high. A possible
explanation for the latter discrepancy is discussed in the next section.
TABLE 4
Intrinsic properties (order of magnitude) of a typical hard magnetic material (lanthanide-cobalt alloy)
and a soft magnetic material (iron).
Fig. 26. Spherical cavity in a ferromagnetic crystal with reverse-domain spikes. The arrows indicate
the domain magnetization. Concentrations of surface charges are indicated by their respective signs.
Hc = 1.23y/tzopMs. (6.10)
For the same two examples of the previous section (table 4) we calculate the
nucleation coercivity at an inclusion of radius p = 10-6m and find Hc(La-Co)
5 × 104Am -1 and H c ( F e ) ~ 103 A m -1. The nucleation at an inclusion in a hard
magnetic material is thus relatively easyl Inclusions of cavities should therefore be
avoided or indefinite expansion of a nucleated domain should be prevented by
some pinning mechanism. The spike formation at a cavity is analogous to the
formation of reverse domain spikes at the flat end face of a long magnetized
crystal, where as mentioned in section 6.4 the local demagnetizing field is
Hd = -½Ms (see also fig. 29).
(c) Wa = _~/x0Ms2[1-25P
2_ 2//dq~ 2] g
\ dx ] J '
where the second term is due to the inhomogeneous magnetization with angular
gradient dq~/dx. Outside the wall the magnetization is uniform and oriented along
the easy axis. Hence the energies WK and We are zero and
1 2
Wd = gtx0Ms V.
The difference in energy between the two situations: sphere outside wall and
sphere inside wall then is
[
A W = - / K sin 2 ~0 + A -~
dq~ 2
The pinning force (using eq. (6.3) for the relation between ~0 and x) is
f- d(zX
dxW ) _ 4 K V 3 / K~ sin 2 p cos p .
sV5 K V
Im-- ~ - - 'TT~--
Substituting this result into eq. (6.7) we find the coercivity due to a cubic array of
spheres with radius p ~ 8 as
2 K a2/3 V 1
Hc = 0.47-----0-~s p 28
(6.11)
= 1.95/-/1 ~ ol 2/s ,
The numerical factor of 1.95 depends on the geometry of the inclusions and
their distribution, but is expected to be of the same order of magnitude for a
variety of probable inclusion shapes and distributions.
Using the parameters of the two examples mentioned in section 6.3.1 (table 4),
we find for a dispersion of inclusions with a radius of 10 -9 m, occupying 0.1 of the
material Volume H c ( L a - C o ) ~ 106Am -1 and H c ( F e ) ~ 5 0 0 A m -1. Both orders of
magnitude agree well with experiment, which suggests that pinning at small
inclusions might be an explanation for the observed coercivities. For this pinning
mechanism it is assumed that the wall is rigid and moves through a cubic array of
spheres (see fig. 25). A non-rigid wall in a random distribution of spheres is able
to arrange itself so that it contains a maximum number of inclusions. The latter, a
more likely picture of a pinned wall is expected to obey eq. (6.11) as well.
,,//I////////////l
z
At an infinitely sharp point, i.e., when r2 = 0, the demagnetizing field at the point
P is infinite. However, as pointed out by Aharoni (1962), this is physically
unrealistic since a point cannot be sharper than the atomic radius --~10-1° m. For a
conical pit with a base radius of 1 p~m and sin 2 ~p cos ~b = 0.4 (i.e. ~b ~ 60 °)
Ha ~ 1.8Ms.
Similar demagnetizing field concentrations arise at sharp corners and edges and at
the bottom of cracks and scratches. Although they are appreciably stronger than
the overall demagnetizing field of a magnetized body and perfectly capable of
explaining the persistence of reverse domains in soft magnetic materials (De Blois
and Bean 1959) they are not sufficient to account for nucleation of reverse
domains in hard magnetic crystals. However, there is experimental evidence that
sharp edges do play a role in nucleating reverse domains, as demonstrated by the
following experiments on SmCo5 and related compounds. Becker (1969) has
measured a coercivity of 8.3kAm -1 (105 Oe) on a YCo5 powder made by
mechanical grinding. Subsequent treatment in a chemical polishing solution
increased the coercivity to 266 kAm -1 (3340 Oe). Becker attributed the increase to
the rounding off of the initially sharp edges of the powder particles, which he
observed by microscope. Ermolenko et al. (1973) prepared a single-crystal sphere
of 8mCo5.3 of about 2 mm diameter. After chemical polishing the sphere had a
coercivity of 460 kAm -1 (5800 Oe). Scratching the sphere reduced the coercivity to
practically zero (Shur 1973) and subsequent polishing restored it again. The
influence on the nature of the hysteresis loop was shown by Zijlstra (1974) who
compared the hysteresis loops of two single particles taken from a ground SmCo5
powder before and after annealing (fig. 28). The coercivity of the particle as
ground appeared to be determined by easy nucleation and subsequent pinning of
domain walls. For the annealed particle the nucleation proved much less easy.
The annealing process may have removed internal defects which also have their
influence on the hysteresis. However, McCurrie and Willmore (1979) have ~hown
that a similar behaviour is obtained when the particles are smoothed by chemical
polishing rather than by heat treatment.
A special case is the long body with a flat end face. The local demagnetization
factor equals ½ at this end face, although the average demagnetization factor
approaches zero for longitudinal magnetization. The associated superficial demag-
netizing field may give rise to homogeneous nucleation of reverse domains as shown
in fig. 29.
r~ e..
"" O
E
,- ©
o~
~E
r.~
=2
o
r~
O
PERMANENT MAGNETS; THEORY 83
/
a
Fig. 29. End surface of a magnetized body. (a) The body in cross section. Reverse-domain spikes
penetrate from the surface into the body (schematic). The arrows indicate the domain magnetization.
(b) Micrograph of a Sm2Co17single-crystal surface with the spikes seen from above.
a f r o m - ~ to Xl ,
b f r o m xl to x2,
c from x2 to + ~ .
Ja=Jc¢Jb,
A a = A~ ¢ A b ,
g . = K ~ gu.
84 H. ZIJLSTRA
I x
I ,/
c ,¸
, b , \
/ I I X2
a I
I Xl
Fig. 30. Domain wall distributed in three zones a, b and c of the ferromagnetic crystal.
The easy axis of the uniaxial crystal is along the z-axis; the planar defect is in the yz
plane. A field H is applied along the z-axis. A 180 ° domain wall parallel to the planar
defect has an energy per unit area of
f~[Ai\{d~2
Y = -~ L d x ] + Ki sin 2 ~ - H J / c o s ~ ] dx, (6.12)
where ~ is the angle between the magnetization vector and the z direction, and the
subscript i applies to the appropriate region where the wall is located. Minimizing Y
by variational calculus and integrating Euler's equations in the three regions yields
the following three equations:
i
i
[ i
I I
i 1
I I
I I
Fig. 31. Orientation angle ~0as a function of distance x near the interface between zone a and zone b.
Minimizing this with respect to q~l with fixed values of ~0a,~b and Ax and subsequently
letting Ax approach to zero, yields
The difference ~ b - ~Oahas a fixed value for fixed Ax, since it determines the local
exchange energy density. This must be equal to the anisotropy energy density, which
is fixed by ~1 lying between ~0, and q~b,which interval can be taken arbitrarily small.
Continuity of q~ and A d~p/dx at the interfaces xl and x2 produces four equations
from which dq~/dx and Cb are eliminated to give a relation between q~ and ~02 with
coefficients expressed in the parameters A, K, J and H :
2HAaJa - O. (6.14)
AaKa - AbKb
This equation describes a hyperbola shown in fig. 32. Only the upper right hand
branch applies to our model. For H = 0 this curve degenerates to its asymptote
cos ~j = cos ¢2. The width of the defect determines which point of the curve
represents the actual situation. Narrower defects shift the point to the right. In the
small-deviations approximation, A a ~ . A b , K a ~ K b and Ja-~Jb, eq. (6.14) can be
written as
7)/t-x-+-k-)j -
[cos K,12I
= -4h
/(A_k- ,,÷)
+ , (6.15)
86 H. ZIJLSTRA
cos %
J
cos "P2
-p
\
\\
with
d_~_~= 4 K b
dx ~ sin ~ ,
PERMANENT MAGNETS; THEORY 87
"it-- -- -- -- [ --
0 . . . . . I
XI X2 ~ X
Fig. 33. Orientation angle ~0 as a function of x of a pinned d o m a i n wall in zero field (drawn line) and
in a small positive applied field (dotted line).
w h e r e we take for ~0 the average value 1(~1 + ~pz). Integrating this gives
7r D / A A AK\
h- ~- 6b t--A---+--K--) sin(qh + ¢2)sinl(qh+ ~2). (6.18)
L o o k i n g at fig. 33 we see that u n d e r increasing field h the wall will shift to the
right thus steadily decreasing the average angle of orientation ~p inside the defect.
Starting from ~p = ~-/2, the position at H = 0, we see that the angular function of
eq. (6.18) starts at zero and increases to a m a x i m u m of the o r d e r o n e at a certain
critical value of h. F u r t h e r increase of h will give no solutions for ~1 and ~2 so that
no stable wall will exist. W e identify this critical field with the unpinning field or
coercive force
(6.19)
88 H. ZIJLSTRA
The minus sign in eq. (6.18) implies that pinning occurs only if the form between
brackets in eq. (6.19) is negative, i.e., the wall energy inside the defect is lower
than if the defect were not present. If the form in brackets is positive a wall will be
repelled, and the defect will form a barrier rather than a trap. It should be noted
that eq. (6.19) is valid only in the small-field, small-deviations, small-defect-width ap-
proximation. If deviations become larger the symmetry in AA and AK will be lost. In
particular a substantial lowering of A will contract most of the wall inside the defect
so that the condition 6 >> D is no longer satisfied. This particular situation is discussed
in secion 6.5.2. In the small-deviations approximation ~b may be replaed by 6a, the
wall thickness in the undisturbed crystal. Note that hc falls within the small-field
approximation as a direct consequence of the small-defect-width, small-deviations
approximation. In this approximation a deviation of J has no influence on he. In the
case where D >> ~b the wall will be almost entirely within the defect region at H = 0.
With field increasing from zero we deal with a wall penetrating from region b into
region c, i.e., a wall pinned by a phase boundary. Using eq. (6.13) with i = b, we
impose boundary conditions ~ = 0 and d~/dx = 0 for the far left-hand end of the
wall, which yields Cb = -HJb. Similarly we find with q~(+~) = 7r and d p / d x ( + ~ ) = 0
in eq. (6.13) with i = c the integration constant Cc = HJa, recalling that region c has
the s a m e properties as region a. Eliminating d~o/dx from these equations we find
Looking at fig. 33 we expect that the highest rate of energy change will be found at
about ¢2 = ~-/2, so that the coercivity becomes
_ He 1/AA AK\
(6.20)
hc HA(b)~ ~-A--+--K--)'
which is the pinning force exerted upon a wall that penetrates from a phase with
low A and K into a phase with high A and K. In a material as SmCo5 with
HA = 2.5 x 1 0 7 A m -1 (300 kOe) this pinning mechanism could account for a coer-
civity of the order of 1 0 6 A m i (~104 Oe) with a 10% variation in A and K.
This section treats a theoretical model of the interaction of a plane domain wall
with a certain type of plane lattice defect, namely the antiphase boundary (APB).
The A P B occurs in ordered crystals where the atomic order on either side of the
PERMANENT MAGNETS; THEORY 89
X X X I0 0 0
I~ I~ I~III'IX'XI'X ~ X
I
x x × f×?×?×?×
~x~x~×~?x?x?×? x
I
APB
Fig. 34. Ferromagnetic ordered crystal with magnetically active antiphase boundary (APB).
At
w~ = g
~ - [1 - c o s ( ~ , 2 - ~ , ) ] , (6.21)
where pl is the orientation of the left-hand layer and ~2 that of the right-hand
layer. The coefficient A ' is different from A and can be negative, in which case
antiparallel coupling across the A P B is favoured. The structure of the wall in an
arbitrary position with respect to the A P B is shown in fig. 35 by the orientation
90 H. Z I J L S T R A
0 -×
Fig. 35. Orientation angle p as a function of distance x normal to a domain wall pinned at APB.
angle q~ as a function of x. T h e wall energy per unit area can then be written as
T h e first two terms follow by integrating eq. (6.6) from 0 to ~1 and f r o m q~2 to ~,
respectively. T h e third term is the exchange coupling energy in the slab of
thickness ~ at the A P B and the last term accounts for the anisotropy energy in the
same slab. N o w approximating to continuous magnetization with the A P B as a
mathematical plane of zero thickness (~: ~ 0) where the j u m p in p is concentrated,
we can ignore the anisotropy energy term and write (omitting constant terms)
3' =
x/)-g 2(cos q~2- cos ~1) - r/cos(r/2 -- ~1) (6.23)
where the coefficient r / = A'/~X/--A-K can take values f r o m -oo to 0 for antiparallel
coupling, and f r o m 0 to +o0 for parallel coupling across the A P B . F o r r / ~ oo the
difference between q~l and q~2 vanishes and we have the undisturbed wall with
3' = 4X/A--K following from eq. (6.22). Using standard differential calculus with
respect to the two variables ~pl and q~2 we find for r / > 1 stability at cos qh = l/r/
and cos ~0z = - l / r / , i.e., the wall is pinned with its centre coinciding with the A P B .
F o r r / < 1 the wall collapses into the A P B with q~l = 0 and ~2 = ~r. Such a
d e g e n e r a t e d wall will still be called a wall here. T h e energy of the pinned wall
follows f r o m eq. (6.22) with the a p p r o p r i a t e values of cos ~01 and cos q~2 substituted
as
and
-5
I
1'0
"-5
--10
Fig. 36. Energy ~/of domain wall pinned at A P B in zero field as a function of the coupling p a r a m e t e r
~7 across the APB.
Y(~o, H ) =
F[ K sin e ~ + HJ(1 - cos ~ ) + A [ d~'~2]
\ d x ] J dx, (6.24)
d2~p
2 K sin ~ cos ~ + H J sin ~p - 2 A ~ = 0,
{dq~ ,~2
K sin 2 q~0+ HJ(1 - cos q~0)= A \d-x-x] "
Detachment of a pinned wall. Consider the wall in zero field symmetrically pinned
at x = 0 with q~2= ~" - qh. A field applied along the z axis will rotate ~Pl and q~2
towards 0, i.e., the centre of the wall will be shifted from x = 0 to the right in fig.
35. If the field is varied f r o m zero to increasing positive values, the force exerted
on the wall will increase, at first being in equilibrium with the rate of change of
wall energy. But as the latter quantity reaches a m a x i m u m a further increase of
the field detaches the wall from its pinning site and makes it travel to infinity. T h e
total energy of the wall when pinned is
where 7(qh, h) follows from eq. (6.25) with qh substituted for q~0, and 7(qh, h)
follows by substituting 7r - q~2 for ~0 and - h for h. T h e m i n i m u m of 3' with respect
0.5
\
0.2
0.1
\ \
0.05
\ \
\
\
0.02
0.01
0.1 0.2 0.5 1 2 5 10 20 50 100
_ ~ r]
to the independent variables ~01 and ~02 is sought and the critical value h~ of h
where this extreme ceases to be a minimum is determined. This critical value h~ is
identified with the unpinning field or the coercivity and its relation with r/ is
shown in fig. 37. The curve applies only to positive values of ~7. At negative 7/ the
zero field values of q~l and ~2 are 0 and ~-, respectively, and it would take a
stronger field than h = 1 to detach the wall. However, at h = 1 uniform rotation
occurs and the whole concept of wall detachment becomes irrelevant.
where ~/ is a negative n u m b e r and Y(q~l, h) and 7(q~2, h) are given by eq. (6.25)
with @1 and q~2 respectively substituted for ~P0. For equilibrium the partial
derivatives of y with respect to the independent variables ~/91and q~2 must be zero.
Since in equilibrium q)l --@2 for symmetry reasons, these two conditions reduce
~
to one:
2(1 - cos 2 q~l- 2h cos ~pl+ 2h) 1/2+ ~ sin 2q~1 = 0. (6.26)
q~
q01 -~ x r
a
Fig. 38. (a) Magnetization orientation near A P B after saturation in a strong positive field. (b) Wall
emitted from A P B by a negative field moves to the right, leaving the A P B in antiparallel configura-
tion.
94 H. Z I J L S T R A
By investigating second derivatives we find that the equilibrium of eq. (6.26) loses
its stability when cos q~l + h ~<0. This gives a simple relation between the critical
field hc and the critical angle qh:
he = cos q~l •
Elimination of ~1 from this formula and eq. (6.26) then gives the relation between
hc and 7 as shown in fig. 39. The nucleation described here occurs only for
negative values of 7 and at a negative field which approaches zero for large
negative values of 7/. The Lorentz microscope observations by Lapworth and
Jakubovics (1974) and by Van Landuyt et al. (1978) of the APBs in thin slices of
MnA1 crystals being always decorated by a domain wall are explained by
assuming that a strong negative coupling at the APB is present.
0.5
02 \
ho
l 0.1
"..
0.05
0.02
0.01
0.1 0.2 0.5 1 2 5 10 20 50
\ 100
9_ b
Fig. 40. Spin orientation in domain wall of fig. 19 viewed along a row of atoms normal to the wall
plane. (a) High-energy transitional position. (b) Low-energy stable position.
plane and a wall with its centre just b e t w e e n two lattice planes. T h e two situations
are shown in fig. 40(a) and (b), where the (b) configuration has the lowest energy.
T h e energy difference gives rise to pinning of the wall (Zijlstra 1970a).
T o calculate the wall e n e r g y we divide the wall along its thickness into three
zones: two continuous zones away from the centre, where the angle b e t w e e n
adjacent spins is small, and a central zone of N + 2 discrete magnetic m o m e n t s .
T h e continuous zones end in the first (or, as the case m a y be, the last) discrete
m o m e n t (fig. 41). T h e energy of this wall in a field h along the z-axis is
7 = y(q~0, h ) + ')/(~DN+I,h)
hK(2- cos q~0- cos q~N+I)
+ laK(sin2 q~0+ sin 2 q~N+l)+
2A
-1-
a {1 -- COS(@N+ 1 -- qON)} , (6.27)
I I I I I
i i 1 x\
I t
Fig. 41. Domain-wall model consisting of centre part with discrete spins sandwiched between
continuous zones.
96 H. Z I J L S T R A
where y(q~0, h) is given by eq. (6.25) and 7(~Pl, h) follows from eq. (6.25) by
substituting (Tr - ~N+I) for ¢P0 and - h for h. The third term accounts for half of the
anisotropy energy of the spins 0 and N + 1, the other half being included in the
continuous zones. Similarly the fourth term accounts for the magnetostatic energy
of the same spins in the field h = HJ/2K (where J is the saturation magnetization
per unit volume). The fifth term is the sum of the anisotropy energy and the
magnetostatic energy of the spins 1 to N and the exchange-coupling energy
between spins 0 to N. The last term adds the exchange-coupling energy between
spins (N + 1) and N. The energy difference between the two spin configurations of
fig. 40 in zero field has been calculated by Van den Broek and Zijlstra (1971) by
minimizing eq. (6.27) with h = 0 for variations of ~i. The result is given in fig. 42
where the energy barrier is plotted as a function of ~7 = a2K/A. The angle
between the two central spins of the wall in its lowest state is shown in fig. 43 as a
function of ~7. For values of ~7 greater than 4 the wall collapses to a configuration
with one part of the spins oriented in the + z direction and the rest in the - z
direction.
The critical field hc required to let the wall pass the energy barrier is calculated
by minimizing eq. (6.26) and finding the value of h for which the equilibrium
becomes unstable. The result is given in fig. 44 where log hc is plotted as a
function of r/. With increasing ~7 we see that a sharp rise occurs at r / ~ 1. This
phenomenon is indeed found to occur in a family of lanthanide-transition metal
compounds investigated by Buschow and Brouha (1975) and Brouha and Buschow
10-1
aK
10-2
10.3
10-~
10-5 t
o 1 2 3 /.
_-~rt
Fig. 42. Energy difference between configurations of fig. 40(a) and (b) as a function of ~t = a2K/A.
PERMANENT MAGNETS; THEORY 97
TC
3
&,.p
0 I I I I I I I ~ ~ I
1 2
~-rt
F i g . 43. A n g l e b e t w e e n t h e t w o c e n t r a l s p i n s in t h e c o n f i g u r a t i o n o f fig. 4 0 ( b ) as a f u n c t i o n o f r/ a t z e r o
field.
f
0.5
hc
0.2
O.OE
0.02
O.Ol
o.1 0.2 0.5
j 1
Dq.
5 10 20 50 100
(1975). Their results are summarized in fig. 45, in which the coercivities of various
compounds measured at 4 K are plotted as a function of HA/Ixs, where /zs is the
magnetic m o m e n t per formula unit. This variable can be rewritten as HAI.~J~, in
which expression the n u m e r a t o r is proportional to K and the denominator is
proportional to A. There is only qualitative agreement since the proportionality
factor between K/A in the model and HA/I~ in the experiment is not known.
98 H. ZIJLSTRA
/
30 - [kOe) /A
o y (Co,Ni)s /
x Th {Co,Ni)s /
,, Lo (Co,Ni)5 /
2c I
I,,
ac "1
I
~o I
I
4
I x
I
i °° ':'~ " ~ 2
°o 10 20 30 0 50
(kOe/jaB )
HA/-IJs / F.U./
Fig. 45, Coercivity of various lanthanide-transition metal compounds at liquid helium temperature, as
a function of HA/t~s, which variable is proportional to ~7 (Buschow and Brouha 1975, Brouha and
Buschow 1975).
Q7
Fig. 46. Wall pinned at discrete sites and bulging under the pressure of an applied field.
A S = o l ( x / a )2 (per unit S ) ,
where /3 is another geometrical factor of the order one. The energy of the
magnetic system varies by
AE = yAS - 2HJ A V
where J is the saturation magnetization and y is the wall energy. If the wall is not
parallel to the magnetization direction a magnetostatic term is contributed to the
wall energy. This situation occurs with the " p a d d e d surface" and also with
cylindrical surfaces whose axes deviate from the magnetization direction.
However, when the anisotropy field is large compared with the demagnetizing
field, i.e.,
K > 210 J2 ,
100 H. ZIJLSTRA
as is the case in the hard magnetic materials discussed here, the magnetostatic
contribution is small compared with the wall energy and may be ignored (Zijlstra
1970b, Hilzinger and Kronmfiller 1976).
The equilibrium position of the wall follows by minimizing h E with respect to x
for fixed H :
x = HYa2/y, (6.29)
where a and/3 are taken equal to one. When H is increased until it reaches the
pinning field strength Hp the wall is about to leave its pinning sites. The force exerted
on these sites by the wall is determined by the wall energy y and by the boundary
angle ~0 (see fig. 46). This angle is geometrically connected with the ratio x/a, and
the pinning field strength Hp can thus be related to a critical value (x/a)~rit which is
a property of the pinning sites. The coercivity H~ then follows from eq. (6.29)
(x) (6.30)
Hc = ~aa crit"
This formula is not to be taken too seriously in view of the many assumptions
made. However, the inverse proportionality of Hc with the distance a between the
defects implies
n c o( /,/1/3
where n is the density of point defects distributed in a regular array. If the defects
are distributed at random one might expect different results. Hilzinger and
Kronmiiller (1976) have made computer simulations of a moving wall pinned by
randomly distributed centres and found empirical proportionalities of Hc with n x,
with x ranging from 0.5 for weak pinning to 1.5 for strong pinning. Any
distribution of the inter-defect distance will give rise to a lowest unpinning field, at
which the wall will be detached somewhere. In the new wall position there will
again be a lowest unpinning field, which is not necessarily stronger than the
previous one. By this the observed coercivity will be lower than which follows
from the average a. Moreover, thermal fluctuations will cause wall creep at fields
weaker than the coercivity. Small applied-field fluctuations may have the same
effect. For this reason permanent magnets with their coercivity based upon wall
pinning at point or line defects must be considered as less stable than other
magnets. Substantial wall creep has been observed in copper-containing rare-earth
permanent magnet alloys which, indeed, have their coercivity determined by
wall-pinning at precipitates (Mildrum et al. 1970).
7. Influence of temperature
In the foregoing sections relations between coercivity and intrinsic properties like
anisotropy, magnetization and exchange coupling energy have been discussed.
PERMANENT MAGNETS; THEORY 101
p = v e -aE/kr, (7.1)
where v is a frequency factor, indicating how m a n y times per second the event
could occur and AE is the energy barrier which the system under consideration
has to overcome for the event to occur. The barrier AE is c o m p a r e d with the
average energy of thermal motion kT, where k is Boltzmann's constant and T the
absolute temperature. At r o o m t e m p e r a t u r e k T ~ 4 x 1 0 -21 J.
First we consider the case of an isolated particle with shape or mag-
netocrystalline anisotropy as discussed in sections 3.2 and 3.3. The thermal motion
of the magnetization orientation is expected to have peak amplitude at the
precessional resonance of the magnetic vector in the anisotropy field. This field
will be of the order of 105-107 A m -1, thus giving rise to ferromagnetic resonance at
101°-1012 s -1. W e take these frequencies as the frequency v in eq. (7.1). W e now
compare two situations: a highly unstable one with p = 10 s-1 and a practically
stable one with p = 1 0 . 7 s -1. For these situations we calculate the required barrier
height AE using the values for u and k T mentioned (table 5). There are two
points worth noting: (a) The value of AE is not sensitive to the choice of v and (b)
p has a very strong dependence on AE, establishing a critical value AE-~ 10 19j
below which the system is thermally unstable at r o o m t e m p e r a t u r e and beyond
which it is stable. The barrier A E against rotation of the magnetization vector is
associated with the anisotropy constant K and the particle volume v
AE = Kv.
TABLE 5
I n s t a b i l i t y of m a g n e t i c particle d u e to
t h e r m a l a g i t a t i o n at r o o m t e m p e r a t u r e .
{dZY/m)l/2
w = \dx2 / , (7.2)
where 3' is the wall energy as a function of the distance x from its pinning site and
m is the wall mass associated with the precessional m o t i o n of spins inside a
moving wall. For 3' we write arbitrarily
which means that 3' is lowered by a fraction a at the pinning site and is equal to
its undisturbed value 3'o when it is displaced by half the thickness 6 of the undis-
turbed wall. T h e effective mass of a wall has been discussed by D 6 r i n g (1948).
F r o m his work we have the relation
47r/z0 ( 1 )
m - 2c~26 = 2 a 2 6 , cgs , (7.4)
where a is the g y r o m a g n e t i c ratio of the spins in the wall. Substituting eqs. (7.3)
and (7.4) into eq. (7.2) and using eqs. (6.5) and (6.6) we have
o) ~- ( a o l 2 K X 106) 1/2 ,
~ 10 lo s-1 ,
P E R M A N E N T MAGNETS; T H E O R Y 103
to be used in eq. (7.1). Now consider a part of the wall of area S displaced by a
distance ½6 from its pinning site (fig. 47). This excitation requires an energy of
A E = 7 ( a S + 28X/S), (7.5)
in which the second term accounts for the peripheral wall that has to be made. W e
may safely assume that an excitation with S < 62 will not give rise to an increasing
unpinning of the wall. We thus take the energy of an excitation with S = 62 as the
minimum 2~E for wall detachment and see whether this may occur at r o o m
temperature. The activation energy for this excitation is
A E = 23/6 2 ~ 20A6,
p= 10 -207S 1,
\,
UFeU
S
pinning site
Fig. 47. Part of wall area S displaced by half its thickness ~ from its pinning site.
104 H. ZIJLSTRA
[2X\ 2
3'(x) = a3"o~--~.-) + (1 - a)3'0 , (7.6)
w ~ 3 x 10 22s -1
or
1-'~'1012S 1.
A E = a3"oS,
S = 10-27 m 2 ,
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