1

Progress of Theoretical Physics, Vol. 47, No. 1, January 1972

Inelastic Scattering of Light by Paramagnetic Spin-Waves*)

Roberto LUZZI**)

Department of Physics and Electrical Engineering

University of Southern California, Los Angeles, Cal. 90007
(Received July 9, 1971)

, l.

Introduction

Inelastic scattering of light can occur in paramagnetic metals embedded in

a constant magnetic field as a result of local fluctuations of the magnetization.
Such fluctuations, spin waves in non-magnetic metals, were detected experimentally for the first time by Schultz and Dunifer using EPR techniques. 1) In this
note we discuss the feasibility of studying paramagnetic spin waves by means
of light scattering, and its advantages and limitations with respect to magnetic
resonance experiments.
As in the case of light scattering by spin waves in magnetically ordered
materials 2) the interaction between the radiation field and the magnetization can
result from: 1) a direct magnetic dipole coupling of the light with the spin
wave magnetization, or 2) an indirect electric-dipole coupling via the spin-orbit
interaction.
Using a similar method to that devised by Bass and Kaganov, 2) for the study
of light scattering in ferromagnetic dielectrics, and the results for spin susceptibility as given in the literature, 3),;L), 5) it is possible to evaluate the intensity of
the scattered light which results from the direct magnetic-dipole coupling. This
calculation is briefly described in the Appendix. For Na and K this intensity
is several orders of magnitude smaller than the intensitY: of the scattered light
from processes involving the indirect electric-dipole coupling, discussed in this
article. The latter mechanism was considered by Genkin and Genkin 6 ) to estimate the absolute Raman cross section due to spin wave scattering in K. They
suggest, on the basis of t~eir results for the integrated intensity of the scattered
'4i

*) Work supported in part by the National Science Foundation.

**) Present Address: Departamento de F!sica do Estado Solido e Ciencia dos Materiais-Instituto
de Flsica-CP.: 1170-Universidade Estadual de Campinas, Campinas-S.P. Brazil.

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Inelastic scattering of light by paramagnetic spin-waves in metals in a constant magnetic

field is analyzed. A method to calculate the scattering cross section using the generalized
self-consistent field method is introduced. The advantages and limitations of light scattering
experiment with respect to EPR techniques in the study of these excitations are pointed out.
Frequency shifts, polarization selection rules and line shapes of the Raman spectra for arbitrary
orientation of the magnetic field are discussed.

R. Luzzi

~~

2. The scattering cross section

We consider an N-conduction electron system embedded in a static and uniform magnetic field H 0, applied in z-direction. This electron system interacts
with a radiation field characterized by the vector potential
A (r, t) = ~ (2 Vscok,.)- 112 (ek,.ak,.ei<kr-rot) + h.c.),
(1)
k.f.l

where k is the wavevector, f.L the polarization index, e unit polarization vectors,
V the volume of the sample and s the background dielectric constant. Absorption and dispersion at the incident and scattered photon frequencies will be neglected.
The interaction hamiltonian is given by 9 )
(2)

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radiation, the possibility of studying experimentally the region of spinwave vectors qRo':?l, where Ro is the magnetic length R 02 =hc/eH0
In the present article we calculate the differential scattering cross section to
discuss intensities, frequency shifts, polarization selection rules and line shapes
of the Raman spectra for arbitrary orientation of the magnetic field. For that
purpose we introduce a new method of evaluating the scattering cross section
for Raman scattering by fermion systems. We include the effect of non-magnetic
impurities randomly distributed which result in spin-difusion, which is basically
responsible for the line-shape of the Raman spectra of paramagnetic spinwaves.
The effect of the impurity potentials, after averaging over the impurity positions,
can be incorporated into an orbital relaxation time r 2 Futhermore, we consider
here the case in which the wavelength of the incident radiation is in the transparency region of the alkaline metals, e.g., X<2100A for Na and X<3150A for
K. A reflexion-type experiment can also be performed. Then one can use laser
light in the visible part of the spectrum, but to obtain the experimental cross
section it is necessary to solve the boundary value problem at the metal surface.
Futhermore, the interaction of the magnetization with light is restricted to the
skin-depth region, thus limiting the experimental scattering volume. In reflexion
as well as transmission-type experiments, single-particle scattering, luminescence,
etc., will be superimposed on the spin wave scattering making observations very
difficult .
.In 2 a method is devised to derive the Raman scattering cross section.
The formalism due to van Hove 7) is used to express the cross section in terms
of appropriate matrix elements of the Landau quasi-particle density matrix. These
are calculated using the generalized self-consistent :field (GSCF) method. 8)
Section 3 is devoted to the numerical evaluation and discussion of the cross
section, while 4 concludes the paper with a summary and evaluation of the
results.

Inelastic Scattering of Light by Paramagnetic Spin- Waves

vvhere the current operator

(4)
vvhere r 02 =e2/mc 2 is the classical radius of the electron,(-) stands for statistical average at temperature T and V is the operator (in second quantization
notation)
~

(5)

I'

vvith

CV(r) = _!_ [eik 2 re2 P(r) [E- 3C- wl]- 1ACT L[E- 3{- wl]- 1e-ikpre1 P(r)]
m
(6)
and

P(r) = -iJ7+!!_A 0 (r).

c

(7)

A 0 (r) is the vector potential associated vvith the constant magnetic field and vve
have vvritten ACT L for the spin-orbit interaction hamiltonian. The unit vectors

el

e2

and
give the polarization directions of the electric fields of the incident
and scattered electromagnetic radiation. 3C and E are the hamiltonian and ground
state ~nergy of the N-electron system.
We revvrite Eq. ( 4) in the form
2

d rJ - r 2_!!!_
dQd(J)
0 0)1

dte-i(ro-ro 1 )t Sd 3r d 3r d 3r d 8r
1

vvhere vve have introduced the Wigner density matrix ~perator 10 )

(Sa)

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has been introduced. In Eq. (3) 7t is the canonical momentum operator including
spin-orbit interaction.
Raman scattering of a photon (kh w1) to state (k2, w) vvith creation or annihilation of a spin fluctuation (q = k 1 - k2, Wq = w1 - w) results in the third Born
approximation, involving the dipole coupling (A P) tvvice and the spin-orbit interaction once. (The latter is responsible for the spin-flip process.)
The Raman scattering cross section can be derived using the formalism due
to van Hove7) to obtain

R. Luzzi

Equation (8) can be expressed in a more convenient way using the fluctuation-dissipation theorem 11)

dte-i<"'-"' 1 )t(p"};a' (rh r2; 0) Pf3fl' (rB, r4;

t))

= [1- e-/3(ru-ru 1 ) ] - 1(1/n) Im X~~; (rh r2, rs, r4; t:U- t:01),

(9)

where X Is the time-Fourier transform of the generalized susceptibility defined by

X~~; (rh r2, rs, r4; t) = {) (t) ( [p"};a' (rh r2, 0), P.e/3' (rs, r4; t)])

(10)

d 8rld 8 r2e-i<efc)-"o<R 12 )r 12 D(rh r2)'t,nO'(r 2)k'n'O''(r 1),

(11)
where R12 = i- Cr1 + r2), r12 = r1- r2, Ao (r) = Ho (0, x, 0) and 's are Bloch functions
of states (k, n, (j) with k the wavenumber, n the band index and (j the spin m"
dex. In this representation the band hamiltonian

E(r,p)

(1/2m) [p+ (e/c)Ao(r)] 2 +

Vlattice

IS diagonal, i.e.,

{k, n, (jl Elk'n'(j'}

En(k)(]kk'(]nn'(]lfO''

(12)

where En (k) are Bloch band energies.

Using Eq. (11) we find for the scattering cross section of Eq. (8)

r 02__!!}____ [1 ~ e-.e<ru-.,
t:01

)]-

1 :E
vv'

:E (J)* (!1!1') (J) (vv') (1/n) Im x~t-' (w- t:01 +is),

!lfl'

(13)
where v, f1 stand for the set of indexes (k, n, (j),
rJJ (vv') =

d 8r1d 8r2 CV Cr2) ei<efc)Ao<R 12 )r 12 v (r1) v' (r2)

(14)

and x~,;;' (w- o>1) is the time-Fourier transform of the susceptibility of Eq. (10) in
Stinchcom be's representation.
Since we are interested in the coupling of the radiation to the fluctuations
of the conduction electron spin magnetization, one only needs to consider conduction band states v' = (k, <5) and v = (k + q, - <5), where q is the momentum
transfer in the scattering process. The relevant terms of the spin-orbit interaction are (A/2) (L+(j _ + L..._(j +) which result in the Stokes and anti-Stokes bands
of the Raman spectra, respectively. For brevity we will only consider the contribution L+(j - The calculation of the anti-Stokes band is completely identical.

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with {) (t) being the step-function.

Next we proceed to evaluate numerically the scattering cross section. For
that purpose, we find it convenient to use Stinchcombe's representation for an
operator D (rh r 2) 12 )
{kn(jiD(rh r2) lk'n'(j'} =

_,

Inelastic Scattering of Light by Paramagnetic Spin- Waves

Equation (14) can be evaluated using Eqs. (11) and (12) to obtain
(b

;.

<k

+ q~le2 piZ><ZIL+rJ -IZ'><Z' lel plkt>

(k q) = - ~ ---=-:---=------:--::-------:=--(Ez-Ekt-COl)(Ez,-Ekt-COl)
2m w
'
H
+same term with (e1~e2, -co1-'>co).

(15)

The states lkrJ) are Bloch conduction band states, ll), ll') Bloch states and
E the corresponding band energies.
In order to determine the generalized susceptibility X of Eq. (13) we resort
to the following approach. First we define
(16)

(17)

Here Eo is the unperturbed self-consistent hamiltonian of a single quasi-particle,

w the potential of the impurities, (b the external perturbation potential and OE
the induced variation of the self-consistent potential.
Taking matrix elements in Stinchcombe's sense, {k+q~llkt}, on both sides
of Eq. (17), and using the fact that P1 depends on time as exp [i (co- co1) t], one
gets
(CO - C01- Ekt + Ek +q t + i : (P k Ek

Ho) Pk) {k + q ~I P1l kj}

+ ~[ (k+ qlwlk' + q) {k' + q~IP1Ikt}- {k+ q~IP1Ik't} (k'lwlk)]

k'

+ (nkt-nk+qt)

{k+q~lvlkt} =0,

(18)

where n1M = {krJI Pol krJ} and v = (b + E.

The contribution from the terms involving OE is, in the context of the SCF
(r 1 - r 2) between the pair of electrons
theory 8> and assuming contact interaction
at positions r 1 and r2, given by

Uo

{k+ q~loEiki} = (U/N) I:; {k' + q~IP1ik't}.

k'

(19)

Using the same iteration process and averaging over the impurity positions
as in Ref. 4) we finally obtain

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and next we use the fact that X in Eq. (16) can be related to the fluctuation
of the mean value of the operator p in Stinchcombe's representation under the
action of a fictitious external perturbation @. 13>
Since p is the single quasiparticle density matrix of Eq. (Sa), we need to
solve the Liouville equation for p. Let us consider that the electron system is
in the presence of a small concentration of randomly distributed non-magnetic
impurities. The single quasiparticle density matrix p is expanded in the form
Po+ Ph where Po is the unperturbed density matrix. According to the self-consistent field method, B) one has to solve the linearized Liouville equation (h = 1)

R. Luzzi

- (nkt- nk+qJ.) (U/N) ~ p (k', q; co)-~

Tc'

CU (k,

k') [p (k, q; co) - p (k', q; co)]

k'

= (])* (k, q) (nkt- nk+qJ.),

(20)

where p(k, q; co)= {k+qt!Pllkf}, co' replaces co-oh and

CU (k, k') =Nil u (k- k') 2 [(co'- Ekt +

1

Ek'+qJ.)-

(co'- Ek't + Ek+q;.):.... 1]

Ekt= Ek- Un~t-

(wo/2),

Ek+ql = Ek+q- Un~+qJ. + (wo/2),

where
COo= /lHo (1- Ugo)-\

Here g0 is the density of states at the Fermi level, nL- is the Fermi-Dirac distribution function in the absence of the field H 0 , n~ 0 = N- 1 ~kn~~. and (1- Ug0) - 1
is the so-called Stoner enhancement factor. Equation (20) reduces to the Boltzmann-like equation
[co' -coo- q f7 kEk + (ie/ c) (17 kEk X Ho) f7 k] p (k, q; co)
- (nkt-nk+qJ.) (U/N) ~ p(k', q; co)
k'

- .,[;/U (k, k

[
p ( k'' q ; CD)
) 1- p (k, q; co) p (k, q, (J))

+ (/)H* (k, q) (nkt -

nk+qJ.).

(21)
To solve Eq. (21) we make use of the standard technique 14> introducing a
trial function
(22)

where 0 and </J are even functions of k. Futhermore, we assume spherical energy
surfaces, i.e., f7 kEk = k/m*, and since (]) (k, q) is an even function of k, one only
needs to know the function 0 in order to compute the scattering cross section
of Eq. (13).
We omit the lengthy but straightforward calculation that leads to the result
(to second order in q)
0 (k,~q;

())) =(J)i!_(k, q)F(k, q; (J))/[1- (U/N)G(q; ()))],

(23)

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with Ni the number of impurities and u (k- k') the matrix element between
plane waves of the potential of an individual impurity.
To solve the integral equation (20) we will only retain the linear term
qfi'kEk in the expansion of Ek+q-Ek. As shown in Ref. 4) the terms q 2fi'k 2 Ek
give negligible contribution in the case of strong paramagnetic substances we
are considering here. We also make use of the following relations :4>

Inelastic Scattering of Light by Paramagnetic Spin-Waves

where

G (q; ())) =

F(k, q; ()))

(24)

and
(25)
with

(J)c

fi= .fJ- Ci/r2) =

eHo/m*c,

())-

(J)l- Wo- (i/T2) - Ci/r2).

Here spin-lattice relaxation has been introduced phenomenologically by means of

the term i/T2 and r2 is the relaxation time discussed in Ref. 4).
The differential Raman scattering cross section for the anti-Stokes band is
then given by

which has peaks at the frequencies ()) 1 = (J)q, with (J)q the spin-wave frequency root
of the equation (spin relaxation and difusion neglected) 5)
1- (U/N)G(q; (J)) =0.

For not too-high field H 0, nkJ,- nkt is proportional to a delta function centered
on the Fermi surface. In this condition we can write
(27)
where X+ (q; ()) 1 ) is the spin susceptibility as derived by Platzman and W olff/1)
<(J) 2)F stands for the average value over angles of I([) (kF, O) j 2 and Vq = [e.SCco-co 1) -1]-I_
For the sake of completeness we write the expression for X+ which is

where

D* (())- (J)l) = ( VF 2/3) ( ())- (J)l- Wo2

X [

:J
2

cos a
+
sin a
(())- (J)l- Wo- Ci/r2) ) 2 ((J)- (J)l- Wo- i/r2) 2 - (J)c 2

(29)

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(J)c 2 (q P' kEk) (P' kEk Ho) (q Ho)

Ho2
fJ(fJ2-(J)c2)

R. Luzzi

and
m(q; w-w1) = [gowo- (D*q 2/U)]ti,
VF

Is the Fermi velocity and

a is the angle between q and Ho.

3.

Discussion

(/)

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In this section we proceed to discuss the main characteristics of the Raman

spectra, namely Raman frequency shifts, line shapes, polarization selection rules
and intensity, as derived from Eq. (27).
a
1) The Raman frequency shift~ Llw It
is defined as the difference between the
:!::
frequency at which Im X+ is peaked and
c
:::J
the laser frequency (J) 1 Figure 1 shows
>.
....
....0
Im X+ for q = 100, 200 and 300 cm- 1 and q
:....
.0
perpendicular to the magnetic field Ho .
0
The strongest peak occurs at the spin wave
3
frequency Wq, which lies between Wo and
+
W0 Weaker peaks, not shown in Fig. 1,
X
b
appear centered at the Stoner spin-flip
single particle excitations, Wo and Wo We.
Stoner excitations at frequencies Wo + nwc,
Wo
n>2, do not appear in the Raman spectra
Fig. 1. The Raman line shape function Im
'X+ (q; w) for (a) q= 100 cm- 1, (b) q=200
described by Eq. (27) because of the apcm-1 and (c) q=300 cm- 1 It has been
proximations made in order to solve Eq.
used VF = 1.73 X 103 em/ sec, ..-2 = 2 X 10-10
(21). However, these peaks will show in
sec, Ugo=0.2, Wc=Wo and Wo't"z=10. q is
the Raman spectra with intensities proporperpendicular to the external constant
magnetic field.
tional to IRoql 2n, where Ro is the magnetic
2
length R 0 = he/ eHo. For the values of q of interest they have negligible contribution. 5)
Since q is the momentum transfer in the scattering process, this kind of
experiment would allow a determination of the spin-wave dispersion relation, (J)
vs. q, over a range going from qrvO (forward scattering) to qrv2kphotonr-v10 4 -10 5
cm- 1 (backward scattering). In Fig. 2 the Raman frequency shifts vs. q for
qj_H0 , and the line widths are shown. In the upper left corner is shown the
experimental geometry. For q larger than 400 cm- 1 the solution of Eq. (21) to
quadratic order in q begins to be invalid.
For q not perpendicular to H 0 the cutoff value of q, i.e., the value of q for
which the spin wave spectrum merges into the continuum of spin-flip excitations/)
can be estimated. For q approaching this value the spin-wave spectra begin to
smeared out and disappears in the Stoner continuum.
2) The line shape It is given by the line shape function X+, and is nearly
lorentzian. The line width is governed by the parameters T 2 and Im D* (w) q 2.

Inelastic Scattering of Light by Paramagnetic Spin-Waves

.......

------

(.)

20

..s:::
en

>.

..s:::

(.)

0.5 ~

Q)

::J

0"

Q)

Q)

.....
......

frequency shift

0.1
1.0 L . . . . - - - - - - - - - - ' - - - - - - - ' - - - - - - - L - - - - 1
100
300
200
400
500

q, cm- 1
Fig. 2. The Raman frequency shifts and linewidths as a function of wavevector q. Same parameters as indicated on caption to Fig. 1. A possible experimental arrangement is shown in the
upper left corner: dot and double arrow indicate polarization of the electric :field of the radiation.

In the experiments of Ref. 1) T 2 - 1 were of the order of 10 6 sec- 1 and then the
spin diffusion term will determine the Raman line width for similar samples. It
must be emphasized that D depends on frequency and orientation of the magnetic field ( cf. Eq. (29)). In the case q j_ H 0 and with the para,meters adjusted
as indicated in Fig. 1, we find that the line width of the spinwave peak in the
Raman spectra remains smaller than 1 em - 1 for values of q in the range 10 to
300 cm- 1 However, we can observe that for increasing values of q the Raman
line, because of spin-diffusion effects, spreads out in frequency with a rapidly
decreasing peak, thus making the experimental detection difficult.
3) Polarization selection rules They result from the symmetry properties of
the Bloch functions in Eq. (15). We consider only the conduction band and the
next upper band. We assume that the conduction band states for k values on
the Fermi surface are s-like (neglecting d-mixing which seems to be present in
Na and K) and that the states of the upper band are p-like. 16 ) In these conditions the only non-vanishing matrix elements are those containing the combinations Ce2x + ie2y) e1z and e2z (e1x- ie1y).
4) Intensity of the scattered radiation We will express it in terms of the extinction coefficienti 6l

To estimate

<([) 2)F

we make the approximations

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linewidth

R. Luzzi

10

and

__!__I<Zieplk)l
2m

2
'"'-'

[1-~](l)exc
m*

where (l)exc is the optical frequency for interband transitions and m* the optical
effective mass. Using the values appropriate to the case of K, (l)exc"'-' 1016 sec-1,
"'--'10 14 sec-1, vFrv10 8 em/sec, m*rvl.1m, n 6 rv10 23 em-S, Ug 0 rv0.2 and for laser radiation (1) 1 rv8 X 1015 sec- 1 and Ho"' 10 kG we find

hrv (vq+ 1) 10-s to 10-7 cm- 1Sr-I,

4.

In

Raman

Conclusions

In summary we can say that Raman scattering of light could provide a way
to study in detail paramagnetic spinwaves in metals. It results in information
on the coupling of photons to spin magnetization, determination of the spinwave
dispersion relation over a broad range of wavenumber q with estimation of the
cutoff wavenumber, and the determination of the exchange stiffness parameter
A((l)) (related to Re D* 4 )) and the spin diffusion constant D ((I)) =Im D*. These
two quantities contain information on the interaction parameters in Landau's
theory of the charged normal Fermi liquids. 18) However, as was mentioned in
the Introduction, the experimental observation of the scattering process discussed
in this paper, can be impaired by the superposition on the spinwave Raman spectra of unwanted background of radiation and by strong absorption. Besides that,
according to the discussion of the previous section, very pure samples would be
required to minimize spin diffusion effects. For a discussion of a reflexion type
experiment, the present results must be used in connection with the solution of
the boundary problem to relate the theory to the experimental scattering cross
section. Futhermore, stretching out the present calculation to values of Ug 0
near 1, Eq. (28) seems to indicate the possibility of having giant scattering cross
sections for scattering of light by paramagnetic spin waves in quasi-ferromagnetic
metals.
Finally, we observe that, as shown in 2, calculation of cross section for
Raman scattering by interacting fermion systems can be related to the GSCF
method. The advantage of this method is its simplicity and clearness and that
permits to calculate rather easily many properties of an interacting fermion
system.

Acknowledgements
The author wants to express his acknowledgements to Dr. A. M. de Graaf
(Wayne State University) for invaluable discussions and useful suggestions on a

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which is of the same order of magnitude than the values observed

scattering by antiferromagnons 17 ) under optical excitations.

11

Inelastic Scattering of Light by Paramagnetic Spin- Waves

number of subjects related to this paper, to Dr. S. P. S. Porto for many discussions on light scattering in solids and to the Departments of Physics and Materials Sciences of the University of Southern California for the kind hospitality
received there.

Appendix
Case of direct magnetic-dipole coupling

aM
at

- = -r(MXHeff),

(A1)

where r is the gyromagnetic ratio and Heff is defined m Ref. 4), one obtains for
the Fourier amplitude of the vector potential A at the frequency of the scattered
radiation (})
2

f2A+ w e(w) A= 4nJ.

c2

(A2)

Here we have defined the magnetic current

J = cP' X M(w)

= ~c P' X [M(wq) X H(wL)],

(A3)

l(j)

where (J)L is the laser frequency and Wq the spin-wave frequency. In deriving
Eq. (A 2) we have neglected in Eq. (A 1) the term that couples the magnetization induced by the external radiation :field with the magnetic :field of the scattered radiation and the term that couples the magnetization (at frequency w) with
the static magnetic :field. Both terms are much smaller than the term that couples the spin magnetization (at frequency Wq) with the magnetic :field (at frequency WL).
Introducing this magnetic current into the interaction hamiltonian of Eq. (2)
and using Eq. (4), where now V stands for Hint we obtain after some mathematical manipulations
2
ww
-d-o- - 2,u 2 ~[1-e-fl(ro-roL)J-l
Im XLL(q, w)'
d!Jdw
c

(A4)

where XLL Is the generalized susceptibility

(A5)

with
(A6)

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To study the case of inelastic scattering of light by paramagnetic spin waves

resulting from the direct coupling of magnetization fluctuations and the magnetic field of the radiation, one can use a similar method to that devised by Bass
and Kaganov. 2) Solving Maxwell equations together with the equation of motion
for the magnetization

R. Luzzi

12

In the latter expression e, K, eL and J(L are unit vectors In the directions of
polarization and propagation of the scattered and incident electric fields of the
radiation.
In the particular case of q= /K/ ( -1, 0, 1), for instance, X reduces to X+ of
Refs. 3) and 4). Then for H 0 r-v50 kG and using the other values appropriate
to K, as given in the main text, one obtains

hrv (Vq+ 1) 10- 14 cm- 1Sr- 1

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17) P. A. Fleury, S. P. S. Porto and R. Loudon, Phys. Rev. Letters 18 (1967), 658.
18) W. F. Brinkman, P. M. Platzman and T. M. Rice, Phys. Rev. 174 (1968), 495.
1)
2)

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This value is several orders of magnitude smaller than the value for h which
results of considering the indirect electric-dipole coupling. For that reason we
do not go into the details of discussing the line shapes and polarization rules
that can be derived from Eq. (A 3).