Faraday Effect in Ferromagnetics.

237

interaction, and the sum of the two effects can be represented as varying very
closely as the square of the atomic number.

It is a pleasure to express my appreciation for the interest th a t Lord R uther­

ford and Dr. Chadwick have taken in this work, and to thank Dr. L. H. Gray
for his helpful discussion and advice. The work was made possible by grants
from the Goldsmiths’ Company and from the Department of Scientific and
Industrial Research, whom I also desire to thank.
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The Faraday Effect in Ferromagnetics.

By H. R. H u lm e , Gonville and Caius College, Cambridge.

(Communicated by R. H. Fowler, F.R.S.—Received November 5, 1931.—Revised

December 23, 1931.)

§ 1. Introduction.—If plane polarised light be transm itted through a medium

under the influence of a magnetic field parallel to the direction of propagation,
the plane of polarisation is in general rotated. This circumstance is known as
the Faraday effect, after its discoverer. For light of a given wave-length, the
magnitude of the rotation per unit distance is found to be proportional to the
magnetisation. The direction of rotation varies with different substances,
being termed diamagnetic, or positive, if in the direction of the current pro­
ducing the field, and paramagnetic, or negative, if in the opposite sense. The
sign of the effect does not depend upon whether the substance is dia- or para­
magnetic ; negative diamagnetics are, however, infrequent. Thin films of
ferromagnetics exhibit an enormous negative rotation, proportional to the
magnetisation,* and in the following we shall attem pt to explain the origin
of this by using a very simple model for the substance.
We shall consider a single crystal of the metal, and, following Heisenberg,f
we shall choose the Heitler-London model, where each electron is considered
as being attached to an atom, as a first approximation. The interaction of the
electrons gives rise to the well-known exchange forces. In a ferromagnetic

* H. E. J. G. Du Bois, *Wied. Ann.,’ vol. 31, p. 941 (1887); H. Behrens, ‘ Z. Wiss

Photog.,’ vol. 7, p. 207 (1909).
t W. Heisenberg, ‘ Z. Physik,’ vol. 49, p. 619 (1928).
 238 H. R. Hulme.

these exchange forces are of vital importance, and it is therefore necessary to

consider states and transitions of the crystal as a whole. Further, it is well
known th at in a ferromagnetic the average orbital angular momentum is
zero. In view of this fact, and in the interest of simplicity, we shall consider
a model where each atom possesses one electron in an s-state, outside a closed
shell. This, of course, does not correspond to the facts, but any other model
would be very much more difficult to handle. Having chosen a model with
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bound electrons, we shall have no conduction (without including polar states),

and shall therefore not have the typical metallic absorption of light, such as is
associated with “ free ” electrons. W ith the extremely rough model used,
it is obvious th a t we can only expect to obtain the order of magnitude of the
rotation, and some idea of its variation with the intensity of magnetisation.
For simplicity we shall choose a simple cubic crystal with all the atoms
initially in the ground state, and the magnetic field we shall take parallel to
one axis. Since the exchange forces are essential to the problem, we cannot
calculate the dispersion by considering each atom independently, as in a gas.
Instead we shall take an element of the crystal with dimensions small compared
with the wave-length of the light, containing, however, a large number of
atoms. This is quite possible for ordinary light. For this system we shall
find the possible wave-functions and the corresponding energies, when all the
atoms are in the ground state and also for excited states. The wave-functions
in each case will be orthogonal, and every one will represent a particular
microscopic state of the system (the “ reiner Fall ” of Weyl). The actual, or
macroscopic, state is then found by means of the usual partition function
involving the. energies of all the microscopic states.
We choose one of the microscopic states of the system when all the atoms
are in the ground state, and consider one of the transitions where a quantum
of left or right circularly polarised light is absorbed. (We must remember
th at the transitions which occur in the dispersion formula are virtual ones
only.) The corresponding energy changes of the system are slightly different
in the two cases. This is because the energy of the final state contains a term
which is due to spin-orbit interaction, and this is different for the two polarisa­
tions of the absorbed quantum. These energy changes enter into the dis­
persion formula, with the result th at the indices of refraction for right and left
circularly polarised light are different. Suppose we have a beam of plane
polarised light travelling parallel to the magnetic field. If we consider the
beam as being composed of two oppositely circularly polarised components
of equal intensity, these will have different indices of refraction and the
 F a ra d a y Effect in . 239
resultant beam will suffer a rotation. For a given microscopic state of the
small element considered, it will be shown that the rotation is proportional to
the magnetisation, when this is in the region of saturation. The result then
follows for the macroscopic state of the same element, and finally for the whole
crystal, considered as being made up of such elements.
In § 2 we shall obtain the approximate wave-functions and energies, and in
§ 3 we shall apply the results to estimate the rotation.
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§ 2. Wave-functions and Energies for the Crystal.—We shall consider, for

simplicity, only those higher states with one atom excited, and for these and
the initial states we may obtain approximate wave-functions, valid at low
temperatures, by the method of Slater and Bloch.* To find the correct first
order wave-functions we include the spin co-ordinates from the start, and
build up determinants which are antisymmetrical in all the electrons. Suppose
we have N lattice points and N electrons, and let

<f>, (xr) {f = 1, 2, ... N ; r = 1, 2, ... N)

be the wave-function of the rth electron at the h lattice point, xr being written
for the three co-ordinates xr, yr and zr. We shall neglect for the present, any
interaction between spin and orbit, so that the wave-function for the electron,
including the spin term, may be written

<f>t M (°r)>

j . = 1 or 2, and a1? a 2 may be taken to represent states with the spin directed
towards the right or left respectively. Let us now fix the spin on each atom,
supposing, for example, that the spins on the a t o m s / 2, . . . , / r, are directed
towards the right, and the others towards the left. The wave-function of the
whole crystal in zero approximation is then given by the determinant

'kifiJz, v / r )
<f>iW • (CTi) (*2) • % (^2) •••
<£2 K ) . a* (oi) (f>
2»2)
( • a*2(<*2) •••
1
• (1)
VN! (x i) • tiff

<f>N(*n) • % (aN)
* J. C. Slater, ‘ Phys. Rev.,’ vol. 34, p. 1293 (1929); P. Bloch, *Z. Physik,’ vol. 61,
p. 206 (1930).
 240 H. R. Hulme.

The r numbers j fl, j ft, ... j f ,are to be put equal to 1, and

j f , ... equal to 2. The resultant spin moment to the left has then
the magnitude
J- ms = \tr C— r+ (N — r)], m
Art Z tz

putting N = 2 n.
If there were no interaction energy between the various atoms, these would
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be the correct wave-functions. We have, however, an additional potential

energy, representing this interaction, given by

V= S V,(*,) + s f- + s v,„,
i < k r ik f<g

where rik is the distance between two electrons, and Vfg the mutual potential
energy of two nuclei together with their closed shells of electrons. It is there­
fore necessary to find the correct combinations of the various possible wave-
functions of the type given by (1). We shall first neglect the magnetic inter­
actions, so th at only states with the same ms can combine together. The
most general antisymmetric function representing a resultant spin moment
of msh 2I tc is then given by

+ <>•)= 2
h-t,

where we must sum over the f ^ ) different distributions of those spins directed
r/
towards the right. The a’s are then found by solving the
of the perturbation energy V. We shall assume throughout th at the states
<{>f, <f>f +v etc., may be treated as approximately orthogonal, and that only
those terms in V relating to two neighbouring atoms need be considered. We
then find* the following (/N \) equations for the a ’s

EO (/, ... /,) + J 2 [a (A' ... / / ) - a (A ... /,)] = 0,

fl •** f f
where
A</ , < -
and the summation is over all those distributions ( / / . . . / / ) which differ
from ( /x ... f r) by the interchange of two adjacent, oppositely directed spins.
In (4)
£ = 7) - E 0 + NJ, (4a)

* F. Bloch, loc. cit.

 Faraday Effect in Ferromagnetics.241

where rj is the total energy of the system, E 0 is the electrostatic interaction

energy given by

E 0 = | (<f>! M )2 ... (</>n M )2 . V . ... dx^, (4b )

and J is the exchange integral between two adjacent atoms given by

J = I Ih M </>/+] (**) <t>* W <(xi) ~ + v /

—*12
ita
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+ V iW + Vm W + 2V/ , m (4o)

In order to avoid end effects we assume th a t the a s are periodic. If it were

possible to solve these equations accurately, we should obtain ( ^ j orthogonal

wave-functions. As it is, we can only solve them accurately when 0 or 1,

and approximately when r^ N. This has been done by Bloch, who
in the case of a simple chain of atoms the approximate wave-functions are
given by equation (3) with
27ri 2iri
an.....„ (/, ..Jr) = e ~ <w‘ ••• Vf> + e ~ i’,’> + ... , (5)

where we must sum over all permutations of Jcv k2, ... kr ; and the corre­
sponding values of s are given by

=2J £ (l-c o s ^ ), ... k ) ... i , = 0 ,1 ... N — 1. (6)

j = 1 N /

To obtain these solutions it is first necessary to neglect those equations in (4)

where a(ft ... f r) contains two or more neighbouring spins directed towards
the right. If rN, the number of these equations is small compared with the
N
total number, f ^ ). The remaining equations are then satisfied by the values

of the a’s and the e’s given by (5) and (6). Further, it can be shown th at (5)
and (6) are approximate solutions of those equations which we have neglected.
The results can be extended without difficulty to the case of a crystal. The
wave-functions obtained in this way are unsatisfactory for our purposes since
' Nx
there are (N -J- r— 1) !/(N — 1)! r \ of them instead of I ^ ); and, further,
they are not all mutually orthogonal. The difficulty, however, is not very
serious, since we shall not require the explicit form of the wave-functions.
Let us now consider the possible states of the crystal when we have one atom
in a p-state and the others in s-states. Let the three possible wave-functions of

vol. cxxxv.—a . R
 242 H. R. Hulme.

the excited atom be (f)1, </>2 and </>3, corresponding to — 1 ,0 and -j- 1.
'N \ /N \
Instead of f _ ), we now have 3N . ( ) antisymmetrical wave-functions, of
which an example is

<Al (®l) * Sx K ) •••

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<$W % • M ••• <f>t • % • fo)

i>u ( f l - f r >
’ f) = V N !

<f>r (X i) • a#r (<*i)

% . a?- (aN)

t = 1, ... N ; u — 1, 2, 3, and/* refers to the excited atom.

Since we are neglecting for the present the magnetic interactions, the states
with different values of ms do not combine to this approximation, and hence the
states with ml— — 1, 0 and -f- 1 are also separate to this order
total angular momentum is conserved. The three states — 1,0, 1,
are assumed to have the same electrostatic energy, which, in general,
would not be true for a linear chain, but is true for a cubic crystal.
We may, therefore, say th a t the 3N . (^ ) states given by (7) split up into

three sets of N . ( states, there being no combinations between states be­

longing to different sets. Take one of these sets and consider first of all the
very simple case of a chain of atoms with all the spins pointing in the same
direction. This case is exactly analogous to th at where all the atoms are in
5-states and one spin only is directed towards the right. The equations for
the a’s become*

z ua u (j *) la u (f)a u ( f * — 1 )] + J« ( f 1) — a u U ' + 1 )]
} ( 8)
f = 1, ... N.
where
— + (N — 2) J + 2 Jm. (8a)

E w is the electrostatic interaction energy given by

E „ = [(& (* ,))* ... ( # ( * - ) ) ! - ( ■ M * n))2-V . dx8(b)

* F. Bloch and G. Gentile, 6Z. Physik,’ vol, 70, p. 395 (1931).

 Faraday Effect in Ferromagnetics.243

and J wis the exchange energy between an excited atom in the state u and one
in the ground state, given by

J„ = i f F
f%
( ) <f>f+ 1(*2) 4>T (*2) — + (aq)
J L*12
L f 12

+ V/ W + V/+ j (aq) + V/+1 (x2) + 2V/(

/, /+1
f+i idx dx2. (8c)

The equations are soluble, and we find

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2iri«/#
(9)
and
( 10)

W ith r spins directed towards the right we have the same difficulty as before.
If r N, we can write down a set of solutions which satisfies the large majority
of the equations, namely, those in which a ( f 1 ... f r ; satisfies the condition
th a t of the r -j- 1 positions f x...
since may be equal to one of the / / s. The approximate solutions (for a
chain) may then be w ritten

with

y , (ii)
the sum being taken over all the permutations of the s, and

where
k v ... k r ; k = 0, 1, ... N — 1.

These solutions suffer from the same disadvantages as those given by (5).
We can, however, obtain a better solution, which is sufficient for our purposes,
as follows. We assume th a t we have found the correct normalised, orthogonal
solutions of equations (4), writing them as

( 12)

with corresponding values of s

e*(r). (12a )
 244 H. E. Hulme.

The equations for the quantities a(/x /*

types :—
(a) Of the positions ... f r; /*, no two are adjacent o
((3) f* is not adjacent to or coincident with any and (a) not true ;
(y) those remaining, th at is, those where f l is adjacent to, or coincident
with, som e/r.
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If na be the number of type (a), we have

wa ny, provided N r > 1.

The solutions (11) satisfy only equations (a). A set of solutions satisfying
(a) and ((3) is as follows :
| ‘Z nixft
W i n 1 ) -----7= S a'{fx ...} r)e *
VN/i.
where
I — l, ... (^ ); k = 0, 1 ... N — 1 ; and 1,2, 3,
\T / >• (13)
the corresponding values of e being

l; K(r .!) = t i (r) 2J m 1 — cos 27T/c\

/N \ .
These solutions are all orthogonal and normalised, and are 3N . ( ^ ) in number.
We shall assume that they are a better solution of the equations than those
given by (11).
In the problem under consideration we assume that, under the influence of
a light wave, the crystal is capable of making transitions from the ground
state to a state where one atom is excited. For the refraction of left and right
circularly polarised light, the transitions to states with ml = 1 and — 1 appear
in the dispersion formula. We are therefore concerned with the matrix
elements of the polarisation and energy changes involved in these transitions.
The difference of these energy changes arises from the magnetic interaction of
the spins with the orbit of the excited atom. Strictly speaking, we should
also consider the mutual interaction of the spins, both in the ground state
and in the excited states. This is more difficult to calculate, and as the
difference of its influence on states where = -f- 1 and ml = — 1 is very
small, we shall neglect it. We shall further assume th at the interaction
of the orbit with the spin of the same electron is large compared with the
interaction of the orbit with the spins of the other electrons, so that only
 Faraday Effect in Ferromagnetics.245

the former is of importance. If the perturbation energy due to spin-orbit

interaction is large compared with the exchange energies, the usual perturba­
tion theory does not apply. Indeed, in this case we cannot describe the
atom by the wave-function
4>f i x r) • * j f

which separates the two sets of co-ordinates. We should have to consider the
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spin and orbit in the excited atom as being coupled together, and then this
vector coupled with the remaining spin vector. We shall assume, however,
th at the spins are all strongly coupled together by the exchange forces, so th a t
the wave-functions may be w ritten as above, the spin-orbit interaction being
treated as a small perturbation. Expressed in term s of a model, we assume
th at all the spin vectors are coupled together, forming one vector S, which may
then be combined in the ordinary way with the vector L, representing the
orbital angular momentum.
Let us see how far we can justify these assumptions. As mentioned, we
shall consider only the interaction of the spin of an electron with the orbit of
the same electron. If the electron, j, is near the lattice
energy, is given by H tJ-, where
H _ e2Z [r„. v j
Si ’
2mc2 r A
and is zero otherwise.
As each electron is “ distributed ” over the whole crystal, we shall write
the total interaction energy as

The important point in the above is th a t there are no terms referring to more
than one nucleus or electron.
Let us now consider how the wave-functions and energies given by (13)
are affected by the perturbation H. Take first the simplest case, th a t of
complete saturation. The normalised wave-functions are

N~* S (f), k= 1, 2, ... N - 1 I

ft r• (14)
u = 1,2,3 J

These have energies which are very close together when N is large, so th at
they should really be treated as degenerate. There is also another set of
 246 H. R. Hulme.
states with the same total angular momentum, and energies not far removed.
They are given by the N2 states

•Z-nikfr -Znixf*
N-> S e ~ S e— +ti+, ( / , ; /<), (14a)
fr f*

where k —0, 1, ... N — 1 ; k —0, 1, ... N —1

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considered as degenerate with the set (14). States with different total
angular momentum need not be considered, since the perturbation H does not
affect this quantity. To find the effect of II on any of the states (14), we have
therefore to solve the secular determinant involving the N -f- N2 states (14)
and (14a). We shall show in the appendix, th a t these N 4- N2 states break
up into N non-combining sets. Each set comprises one state out of (14) and
N out of (14a). The secular determinant therefore splits up into N deter­
minants, which may be treated separately. These are quite easy to solve.
We find th a t the states (14) do not combine together, and that provided J is
large compared with the magnetic interaction energies, the effect of the
states (14a) may be neglected, so th a t the wave-functions (14) remain the
correct first order ones, their energies being increased by the corresponding
diagonal matrix element of H. This is given by

+ „ ( /') | H | S e — +„</ ") )

wdiich reduces to
($ l (*1) • a 2 (°i) I H n | (aq) . a 2 (eq)). (15)

On the model used, the orbit precesses round the resultant angular momentum,
the direction of which is practically th a t of ms. The interaction is therefore
given by
C . ms' . (15a )

where m /, m{,refer to a single atom, and the constant, C, is positiv

independent of the magnetic field. We shall put (15) equal to 0, according
as ml— m{ = i 1 or 0 respectively. We have thus shown that in the case
of complete saturation, when ms = n, the wave-functions (14) remain the
correct first order wave-functions, but th at there energy change given by dz <*>,
0 in the three cases.
Consider now the case of incomplete saturation, and let r spins be directed
 Faraday Effect in Ferromagnetics.247

towards the right. Instead of the three non-combining sets of N states given

by (14), we have three (non-combining) sets, each of N . states, given by

a1 ( f v —/r)e N (fv - / r ; f )

1 = 1,2, ...
y (is)
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«: = 0, 1, ... N .
w = 1, 2, 3.

The m atrix element of H between any two of these states is given by

2niKft 2
: S « J' ( / i . - / r)e N /0 1 H I 2 S a , ( / i . . . / r ) e ~ + * ( / i , . . . / r ; / t,))(17)
tfi* I -/,/* ' y

As before, we must have f l = f u, and —k . Further, since the wave-

functions (12) are orthogonal
S a* {fi ■■■fr) • (fi - / r ) = V
i-fr

Hence we must have i — j, and again we see th a t the states do not combine
together. We should also consider all the states of the same total angular
momentum as being degenerate with the states (16), and show th a t their
effect may be neglected, as in the case of complete saturation. This is very
difficult to justify rigorously, owing to the non-orthogonality of the explicit
wave-functions (11). We shall, however, assume on physical grounds th at the
result, proved for ms = n, still holds when = — provided For
the diagonal m atrix element of H for each of the states of (16) we then find the
value
± ~ [(N — r)o) + r(— co)] = ± ; or 0, (18)

according as ml = db 1 or 6- To obtain this result we note th a t the expression

/N \ .
(17) yields N . ( J integrals of the type

(4>\ (xx). a, (ax) | H n | (Xj) . a, (ax) ), (19)

where j = 1 in a fraction r/N of them, and 2 in the others. These yield
contributions of opposite signs and, taking account of the normalisation, we
obtain the expression (18). The integrals of type (19) with 1 arise when
,/1 = f r, ht at is, when the spin on the excited atom is pointing towards the right.
Unfortunately, however, it is here th a t our solution (13) is likely to contain the
 248 H. R. Hulme.

largest error, since all the equations containing wave-functions of this type
occur in the set (y), which we have not satisfied by our solution (13). This
means that the wave-functions are not strictly cyclical in f K The value of
eu which would satisfy these equations neglected, differs from th at used by a
term of the form
(1 — cos 27T&/N) . (difference of two exchange integrals).
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From the approximate value of the energy given by (6) we see th at the relative
error is small when N > r 1. Since N is very large, this condition is realised
in the majority of microscopic states occurring in the distribution function,
provided the saturation is sufficiently great, so th a t N !> Our final result
is therefore th at the wave-functions (13) remain the correct first order wave-
functions, but the energies are increased by an amount

± I 0; (20)
according as ml= i 1 or 0. These results may be extended with
difficulty from the case of a linear chain of atoms to th a t of a three-dimensional
lattice. We have, for the a’s of the ground state, ex
where fi fr>kx ... kr are replaced by vectors with three linear com­
ponents, fj_, ... fr ,‘ k 15 ... k r, and f 1k1 by the scalar product (fx k x). The
period N is replaced by G where G3 = N, and the expression for e becomes
r
2tc ,
£k,... kr 2J 2 cos-— <! + + COS
i = i

When we have one atom excited, the exchange integrals between this and the
neighbouring atoms are not all equal, since the wave-function is no longer
spherically symmetrical. We cannot find their actual values, and to the
degree of approximation to which we are working it would be pointless to
distinguish between them. The expressions (13) may therefore be extended
to the three-dimensional case in a similar way as (5), and we obtain the same
final result (20).
§ 3. Calculation of the Rotation.—We may now examine the rotation of the
plane of polarisation of light transm itted through the crystal. Consider the
plane polarised beam as being composed of two components with opposite
circular polarisations. In a magnetic field the indices of refraction for these
two components are different, and the resultant beam is rotated by an amount

R = — (wp — nK), (21)

 Faraday Effect in Ferromagnetics.249

where A is the wave-length of the light in vacuo, d the distance traversed, and
np, nA are the two refractive indices. In a metal the phenomenon is com­
plicated by large and unequal absorptions, and further, np and nK must be
taken as the real parts of the refractive indices. As the model used contains
only bound electrons, it will not yield the typically metallic absorption associated
with free electrons, and we shall therefore neglect completely the absorption,
since we are only finding the order of magnitude of the rotation.
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We must now calculate np and nx from the dispersion formula for the two
kinds of circularly polarised light. Suppose we have a quantum system under
the influence of a light wave. As stated, we shall consider a simple cubic
crystal, choosing as our system an element of the crystal containing G3 = N
atoms. As the lattice constant is of the order 10~8 cm. and the wave-lengths
of visible light are 10-4 to 10~5 cm., we may take N to be large and at the same
time satisfy the condition th a t linear dimensions of the system should be small
compared with the wave-length of the light. We may then neglect the magnetic
forces due to the light, and the variation of the electric forces from point to
point, expressing the perturbation by the electric vector

E = | (E e2H,,t + (22)
G
where E is in general complex, and * denotes the conjugate complex. Let the
system be initially in a state defined by a set of quantum numbers, n. Under
the influence of the light wave of frequency v, it acquires an additional
electric moment given by
o o o
___ ! rivty
pZ j (JjjnJe Pfcw j
2 * ' M v fcn+ v ) ^ {^nk+ v)

+ | e - 2™'*2! P«*(P*n E*) (23)

k \ h (v*n — v) A (vwfc — v) / '
O
where P nfc is defined by
nk (fin 2 I <£*)>
electrons

(f>n and (f>k being the wave-functions in the presence of the magnetic field.
Formula (23) is true provided the mean value of Pnn in the neighbourhood of
the system, P wri, is small compared with E. Let us consider for a moment
the symmetry properties of the system. In writing down equation (1), we
might assume th a t <f>f(xn) is to be taken as the wave-function of the free
This, of course, is hardly the case, but we shall assume th a t in a magnetic
 250 H. E. Hulme.
field it has approximately the same symmetry properties as the wave-
function of the free atom. These are, firstly, symmetry with regard to a
rotation about the axis of the field ; and secondly, symmetry with respect to
reflection in a plane through the nucleus perpendicular to the axis. Under
the conditions enumerated we may apply the ordinary theory of the Faraday
effect, and we find* that, for a given microscopic state of the system,
"\
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— i = y « + K)
(24)
n ? -l = Y « ~ K )

where V is the volume of the system, and , , are given by

= 2 v V iX J X ^ J 2 1
" h r ^ ^ J - , 2
V. (25)
or = 2 y (m — m') V I X + J 2* [
h r', V
'mwTm2 — V2 J

Here is 4he ^-component of P ^ m, and we have separated the set of

quantum numbers, n,into the set r, and the quantum numbe
the total angular momentum about the field direction.
If P w= Prm, is not small compared with E, the formula (23) is no longer
valid. According to Lorentz, the effective value of the perturbing electric
vector is no longer E but E + | P m, and we find instead of (24) the expressions

V. (24a)
~ 1
%2 + 2

If n 2— 1 is small we may put n 2+ 2 = 3, an

same. For iron nk, np, 2-5, so that we must use (24a). Put

np— nK =
(26)
h (nP+ nA) =
We have in general
An

* Born and Jordan, ‘ Elementare Quantenmechanik,’ p. 267. This is only true when
(X= 1, but for frequencies corresponding to the visible spectrum we may put g = 1 even
for ferromagnetics.
 Faraday Effect in Ferromagnetics.251

so th a t
6 n . An £ approximately,
(n2— 1) ( n2-j- rm2) a
giving
x>r = nd (n2 — 1) (^2 + 2) 2 ft,
■W 0 r * (27)
A bn al

Consider now the values of arm and $rm for an initial microscopic sta,te of th e
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systei
system where ms = ^ — r * There are i ) of these states, a typical one
2 \*
being

fi ••• ff

Corresponding to the absorption of one light quantum , the possible final

states which yield non-vanishing m atrix elements of the polarisation are
given by
1 2
b = - % s s <*” ( / , . . . / r) e ~ < k , (A •■■/,; /')•
V N /,.../, ft

The m atrix element, X, between these two states is then

(4»i j S [ (28)

For non-vanishing elements we m ust have

k = 0, — (29)
and we obtain for (28)
X = V N ( ^ (aq) | | (aq)).

By the usual selection rules we now have

(<f>i (aq) | xx + iyx | ^ (aq)) 5* 0,

(</>! (aq) | aq + iyx | cf>* (aq)) = 0,
(<f>i (xi) I xi~ |iy <t>i K ) ) = 0,
(<£i (xi) I xi — %i I i3 (xi ) ) 9*
(<£i (aq) | aq ± %i | 4>i ) = 0,

since msremains the same and m'l —— 1, 0, + 1,

* This r refers to the number of atoms on which the spin is directed to the right.
All the other r ’s in this section refer to the set of quantum numbers defined above, so
that no confusion will arise. *
 252 H. R. Hulme.
For the type of atom we are assuming—one electron outside a closed shell—
the non-zero elements are equal. Suppose each be 2Q. We then have
I (A K ) I xi I ^ i 1 (xi ) ) I2 = I (A (xi) I xi I ( )) I2 = Q2,
I (A (xi) I xi I A2
(* i)) I2 = °-
The corresponding values of vrm*m are found as follows. In the initial state
we have from (4a ) and (12a)
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t] — E 0 — N J + zl

In the final state, from (8a ), (12a ), (13), and (18),

v)' = E „ - ( N - 2 ) J - 2 J „ + e‘ 2J„ ( l - cos ±

To these energies we must add the sum of the energies of the isolated atoms,
which differ by an amount required to raise one atom from the ground state
to the excited state considered. If this be E, we have

7)' - 7, = (E„ - E 0 + E) + 2 (J - J ,) + 2J„ ( l - c o s ^ j ± « .

E s and J s are both real and E x— E3,
Ji — Ja-
Further k= 0 in those excited states to which transitions can occur (equ
(29) ). Hence we have finally
K ' ±1 ,. = W ± ^ ? , (31)

(“ m”may be either ml or ml-f- w&8, since is unch

W = (Ex - E 0 + E) + 2 (J - J x). (32)
Remembering the remarks at the end of § 2, we may easily generalisethe above
for the case of a three-dimensional lattice. For a simple cubic lattice we find
in the expression (32) for W, we must replace 2(J — J x) by 6(J — Jj).
In the above we have neglected the change of energy due to the action of the
external magnetic field on the orbit of the excited atom. This is the Zeeman
separation, and is very small compared with the spin-orbit interaction energy.
It produces, in fact, the ordinary diamagnetic rotation.
From equations (26), (30) and (31) we ha ve

Q2( w + ^ W) Q2(W m^ “ )
—9
( w + m^Tw f AV (W mg0if A2v2
V N /
Q2 . Av Q2 . Av
(W ml f )- AV(W + - A2v2
\ IS1 /
 Faraday Effect in Ferromagnetics. 253

giving
2$rm 4 ms
on neglecting
arw W2 - /*2v2 ' N ’
and
_ 7i d(
n2 — 1) ( 2 -j- 2) 4 ahv {ms)rm
w~ 6A *W2 - W N ’
putting ms as K ) ; .
So far we have only considered microscopic states of the system. To find
the actual macroscopic state of magnetisation and the corresponding rotation,
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we must find the most probable values of ms and R. These are given by

_ S (mX e - ^ / a
ms — h___
JH
S e - w- / fcT
r, m
and a similar expression for R. From (33) we have
R,; = constant . (m ,)',

which constant is independent of the quantum numbers r and It

therefore follows th a t
R = constant . ms,

so th a t the actual rotation is proportional to the actual magnetisation. This is

proved for elements of the crystal whose dimensions are small compared with
the wave-length of the light used. I t is further true of the whole crystal
regarded as made up of elementary crystals of the type considered.
To find the order of magnitude of the rotation to be expected we shall take
for simplicity the case of complete saturation. W is the excitation energy
of an atom in a crystal, which is certainly smaller than th a t for a free atom,
which is about 10,000 cm._1i Its value is very uncertain, but from (33) we
see th a t it has very little effect on the result. Putting, for iron,
W = 10~12 ergs (5,000 cm.-1
hv —4 X 10~12 ergs,
w = 6 X 10~14 ergs (300 cm.-1 h),
n —2*3 (experimental value),
d —A air,
we find a rotation of about 25°. The observed rotation in iron and cobalt is
about 10°,* so th a t the theory gives the correct order of magnitude.
* H. Behrens, loc. cit.
 '254 H. R. Huime.

Strictly speaking, the results only hold when the intensity of magnetisation
is very great—approaching saturation. We must, therefore, consider the
crystal as being in a strong field. In small fields, also, the model used is no
longer valid, since we have complicated demagnetising effects due to spin-
orbit and spin-spin interaction between all the atoms.
The model used gives the order of magnitude of the rotation and repro­
duces the observed variation with magnetisation for strongly magnetised
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films. I t also gives qualitatively the variation with wave-length—for ferro­

magnetics the rotation increases with wave-length. In the expression (33)
for the rotation, the part containing X and v decreases as X increases, but only
slowly since hv W. If we take into account the experimental fact that n
increases fairly strongly with X, we find th a t the rotation increases with the
wave-length. (For cobalt, ni
ncreases from 1 •4 to 2 -0

Appendix .

We have to justify the neglect of the non-diagonal elements between any

state of the set (14) and all those states which have very nearly the same
energy.
Consider the N states (14). The matrix element of H between any two of
them is given by

| ( S exp (2 m * //N ) ( f )| H | S exp (2™

Remembering the property of H mentioned we see th a t we must have

f* = f * and kv = k q,

so th at the N states do not combine together. Now take the combinations

with the states (14a). A typical matrix element is

N -* (S exp V m K . f l S ) + „ ( / ' ) | H | S exp (2mk,fr/N)

f* fr
S exp (2t» * , / 4,/N) <h+1 {fr ;
.ft'
n) (A2)

Again, for any non-zero contribution

f = /'' = /,.
so that we must have
— kp d- fcq + Kq — 0, N, 2N, etc.
 Faraday Effect *Ferromagnetics
in

Taking account of the normalisation of the <j/s, we then find for (A2) the
expression
(<f>i (x±) .a 2 (of)| H n | </>?+1 (aq) . oq (<?!)).
For each kp there are N possible values of kQ and :
Jc = 0 , 1 , ... k ; k+ 1, ... N —
(A4)
Kg Kp, Kp1, 0 , IS 1, ... Kp | 1 j _J

so th a t we have N m atrix elements of type (A3). There are therefore only N

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wave-functions of (14a) which combine with the given wave-function of

(14). Further, these combine w ith each other, but not with any other
members of the set, since the m atrix element of H between two such states
is zero unless
K KQ= + Kr . .
We therefore have N non-combining sets, each comprising one state from (14)
given by k p , say, and N states of the set (14a ), given by Jca kq = k p . The
original secular determinant of N2 + N rows and columns now breaks down
into N smaller ones, each with N -f- 1 rows and columns.
We find th at, under the influence of a light wave, transitions cannot
occur to all states of (14), but only to those given by 0 (equation (29)).
Consider, therefore, the particular determinant in which this state occurs. We
have to find the correct combinations of the (N -f- 1) wave-functions associated
with this determinant. Let Xvbe th a t state of the set (14)
u = 1, and rip the corresponding energy obtained by neglecting spin-orbit
interaction. Further, let y Q1,yr/2, . . , yeN, be the N associate
(14a), with energies y)51, .., t]3N. Then in y p we have — 1 and in
y Qr we have mt = 0. I t therefore follows th a t the diagonal m atrix element
of the spin-orbit interaction is zero in the latter states (equation (15a ) ). We
have
(X» I H | Xp) = — to,
(Xar I H I xQS) = 0, for all r and
(X, I H | y^f) = 0N_ i,
where, from (A3),
0= ■a 2(<ii) | H n | • “lK ) )•
The quantities 0 and co are both spm-orbit interaction energies, and we shall
take them to be of the same order of magnitude. We have
rip = E x — (N — 2) J — 2JX

rlti = E„ + 2 J2 (1 - cos + (E , - E J - 2(J2 - J,).

 256 H. K. Hulme.

We shall put the last two brackets equal to zero, which is true for a cubic
crystal, though not, in general, for a chain of atoms.
Let a possible combination of the (N + 1) states be

aXv + 26/ XQ3

with an energy given by (E^ — X). We have the following equations to

determine a and the b’s :
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(X — to) a-j- 0N i Tibj = 0

0N“ *o + XA = 0,

where X, = X + 2J2 ^1 — cos ^ ), and X,. = XN_>

The secular determinant for X is easily reduced to the following—

N—1 r N-l
n x. (X - (o)x - e2**-1 - e x N -is e /x ^ = o.

We assume that the exchange energies are large compared with the spin-
orbit interaction energies, that is, J ^ <o. We then find that N roots are
given approximately by X^ = 0, j(== 0, 1 . . N 1
accurate, since X, = X ^ . ) The other root is equal to co (1 + 8), where 8
is small. When X ~ to, we find

which is small by virtue of the last factor. Thus the energies of the new states
lie near to those of the old ones. In particular, the state given by X= <o (I + &)
has an energy approximately equal to that of Xv Further,

so that the state is effectively Xv We therefore see that, to a first approxi­

mation, it is not necessary to take the correct combinations, and the additional
term in the energy of Xv niay be put equal to the diagonal matrix element of
the spin-orbit interaction. A similar argument holds when = 0 in the
state (14) and ml —+ 1 in the states (14a ).
 Faraday Effect in . 257

Summary.

The rotation of polarised light transm itted through very thin films of ferro­
magnetics is discussed, using the ordinary simple model for a ferromagnetic.
Owing to the importance of the exchange forces, we cannot treat each atom
separately ; but must take as unit a fraction of the crystal containing a large
number of atoms. For such a system we find approximate values for the
possible wave-functions in the ground state, and in excited states when one
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quantum of light has been absorbed. This enables us to find the energy
changes and the m atrix elements of the polarisation for those (virtual) transi­
tions occurring in the dispersion formula. Owing to spin-orbit interaction
in the excited states, these dispersion formulae are slightly different for left and
right circularly polarised light. The indices of refraction are therefore different
and a beam of plane polarised light suffers a rotation.
With the very rough model used we can only hope to obtain the order of
magnitude of the rotation. This is reproduced by the calculation, and for
magnetisations in the region of saturation it is found th a t the rotation is
proportional to the magnetisation, and increases with the wave-length of the
light. Both these results are experimentally true.

In conclusion, I wish to thank Professor W. Heisenberg for suggesting the

problem and for much valuable discussion and advice, and Dr. Bloch and
Dr. Gentile for the opportunity of seeing the manuscript of their paper before
publication.

vol. cxxxv.—A. s