Volume 2 Number 0406 ISSN 1979-3898

Journal of
Theoretical and Computational
Studies

Green’s Function in Magnetic Dichroism

Muhammad Hikam, J. Theor. Comput. Stud. 2 (2008) 0406
Received: May 19th , 2004 ; Accepted for publication: May 28th , 2004

Published by
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c 2004 GFTI & MKI

° ISSN 1979-3898
J. Theor. Comput. Stud. Volume 2 (2004) 0406

Green’s Function in Magnetic Dichroism

Muhammad Hikam
Departemen Fisika, FMIPA Universitas Indonesia, Depok 16424

Abstract : The relation between magnetic circular dichroism (MCD) and the local magnetic properties of metal
can be derived in the frame of spin polarized multiple scattering theory. Green’s function is used to solve the Dyson’s
equation of multiple scattering. Here we have used a non relativistic approach by treating spin-orbit as a perturbation
of the multiple scattering development using a spherical potential. By this method, we can interpret the real process
within atomic level, hence we can correlate the difference in x-ray absorption due to spin to the properties of nano
magnetic material. We have tested the theory on iron, cobalt, and nickel. We found that we obtain a good order of
magnitude compared with XANES (x-ray absorption near edge spectroscopy) experiment.
Keywords : MCD, EXAFS, XANES, Dichroism
E-mail : hikam@ui.edu

Received: May 19th , 2004 ; Accepted for publication: May 28th , 2004

q
1 INTRODUCTION where k = 2mE/h̄2 and V (r) is a reduced potential,
Green’s function technique has been widely used in which is 2m/h̄2 times the original potential. If we use
Quantum Chemistry and Molecular Physics to calcu- a function G0 (r) so that:
late excitation and ionization energies, bound state,
(∇2 + k 2 )G0 (r) = δ(r) (2)
transition matrix element, absorption coefficient and
scattering cross section [1]. Green’s function method then all free particle functions ψ0 (r) follow:
was originally introduced in Quantum Field Theory Z
by Feynman in 1948 and Schwinger in 1951. In this ψ(r) = ψ0 (r) + d3 r0 G0 (r − r0 )V (r0 )ψ(r0 ) (3)
article, this function is used to describe multiple scat-
tering process and cross section calculation for mag-
In a vacuum space, the Green’s function can be
netic dichroism application.
written:
Normally, the magnetic dichroism phenomenon [2, 1 eik|r−r |
0

3, 4] is related to two physical evident i.e. Faraday G0 (r, r0 , k) = − (4)

4π |r − r0 |
Effect: rotation of polarization vector when the beam
enters a magnetic material and MOKE (magneto- The function G0 (r, r0 , k) can be expanded in angu-
optical Kerr Effect): rotation of polarization by re- lar momentum representation (in term of Bessel and
flection. The practical use of the last phenomenon is Hankel functions):
for the development of high density magneto-optical  ∞
storage.  −ik X J (r)H (r0 ) if r ≤ r0



 L L
This paper is a continuation of two previous papers 0 l
G0 (r, r , k) = X∞ (5)
on magnetic x-ray dichroism at L2,3 edge [3] and mul- 
 0 0

 −ik H (r)J (r ) if r ≥ r
tiple scattering [4]  L L
l

2 DEVELOPMENT OF GREEN’S FUNC- here JL (r) = jl (kr)Ylm (b

r) and HL (r) =
TION h+
l (kr)Y ∗
lm (b
r ).
In a crystal (or in the influence of a potential V (r)),
To begin the discussion on Green’s function, the the Green’s function becomes:
Schrodinger equation can be written in the form: · ¸
2m
(∇2 + k 2 )ψ(r) = V (r)ψ(r) (1) k − 2 H G(r, r0 ) = δ(r, r0 )
2
(6)
h̄

c 2004 GFTI & MKI

° 0406-1
Muhammad Hikam J. Theor. Comput. Stud. 2 (2004) 0406

2
h̄
where H = 2m ∇2 + V (r), therefore we can relate it to and
the one in vacuum:
Z T (z) = V + V G(z)V (14)
G(r, r ) = G0 (r, r ) + dr00 G0 (r, r00 )V (r00 )G(r00 , r0 )
0 0
in the real space, this equation becomes:
(7)
We can use operator method as the following: T (r, r0 ; z) = V (r)δ(r − r0 ) + V (r)G(r, r0 ; z)V (r0 ) (15)
G(z) = G0 (z) + G(z)V G0 (z) (8) or in matrix form:
Now the Green’s function can be utilized to calculate τeij = Vi δi,j + Vi GVj (16)
the scattering cross section. We can start the calcu-
lation using electric dipole interaction for initial and The physical significant of the multiple scattering
final wave functions: operator is as the following: τeij transforms a wave
X 2 function in the vacuum |φ0 i arriving to j site in τeij |φ0 i
σ = 4π 2 αh̄ω ² · r|Ψcin i| δ(Ef − Ei − h̄ω) (9)
|hf |b
which corresponds to the wave function in the aggre-
f
gate on the i site. We see that τeij (r, r0 ; k) = 0 when
or we can write: r(or r’) beyond the atom influence or when the poten-
X tial is zero.
σ = 4π 2 αh̄ω hΨcin |b
² · r|f i
f
3 GREEN’S FUNCTION APPLICATION
² · r|Ψcin i
× δ(Ef − Ei − h̄ω)hf |b (10) ON MCD
By using:
To develop the multiple scattering equation, we have
2m to be able to write the initial and final states of elec-
δ(Ef − Ei − h̄ω) = 2 δ(kf2 − ki2 − kω2 ) tron. The initial state can be described as spin-orbit
h̄
|j, mj i where mj varies from -j to j (j = 12 for L2
and due to the fact that |f i is an eigen vector of H, edge, j = 32 for L3 edge). If we do not consider the
then δ(k 2 − H)|f i = δ(ki2 − kf2 )|f i and we can obtain spin-orbit effect in the final state (this is true for local
δ(k 2 − H) = (− π1 )Im[G+ (k)], therefore density approximation), the spin is a good quantum
X number and the final state |f ↑ i and |f ↓ i are eigen
2m 1
|f iδ(Ef − Ei − h̄ω)hf | = (− ) Im[G+ (k)] function of the Hamiltonian:
f
h̄2 π
h̄2 2
H↑ = − ∇ + V ↑ (r)
The scattering cross section can be written in term 2m (17)
of the Green’s function: h̄2 2
H↓ = − ∇ + V ↓ (r)
2m ­ ® 2m
σ = −4παh̄2 ω 2 Ψcin |b ²∗ · rIm[G+ (k)]b ² · r|Ψcin
h̄ where the potentials V ↑ (r) and V ↓ (r) are sum of non
(11) overlapping spherical potential. They act on the up
or in spatial space: and down spins respectively. This Hamiltanian can
Z be used to understand by some means of calculation
2m
σ = −4παh̄2 ω 2 d3 rd3 r0 Ψcin (r)b²∗ · r several properties of the transition metals.
h̄
In term of spherical harmonics and considering all
× Im[G+ (r, r0 ; k)]b
² · rΨcin (r0 ) (12)
those spin, the matrix elements of the multiple scat-
It is clear that by using the Green’s function, we tering operator are
do not need to directly calculate the final state of the Z Z
s
wave function. τiLjL0 = d3 ri d3 rj0 jl (k s ri )YL∗ (b s
ri )τij (ri , rj0 )
After developing the Green’s function, we can define
transition matrix T (z) (t-matrix) as the following: × jl0 (k s rj0 )YL (b
rj ) (18)

G(z) = G0 (z) + G0 (z)T (z)G0 (z) (13) where s stands for up (↑) and down (↓) spins.
The multiple scattering operator can be used to
by using the equation (8), in a potential V (r), one can write the Green’s function:
obtain the following relationship: 2X
Gs (ri , r0j ) = k s s
Ril (ri )YL (b s
ri )τiLjL s 0 ∗
0 Ril0 (rj )YL0 (b
rj )
T (z) = V G(z)(z − H0 ) L,L0

0406-2
Green’s Function in Magnetic Dichroism J. Theor. Comput. Stud. 2 (2004) 0406

X
+ δi,j k s s
Ril (ri< )YL (b
ri )Jils (ri> )YL∗ (b
ri ) (19) where li = (lix , liy , liz ) is the local angular momentum,
L and σi = (σ x , σ y , σ z ) are the Pauli matrices. For a
where s
Ril and Jils (ri ) are two real solutions of the
(ri ) spherical potential:
radial Schrodinger equation:
(a0 α)2 1 dVj
· 2 ¸ ζj (rj ) = (26)
d 2 d s2 l(l + 1) s 4 rj drj
+ + k − − V i (r i ) ψl (ri ) = 0
dri2 ri dri ri2
(20) where α = 1/137 (the fine structure constant).
The value of µB is 9.27 × 10−24 Joule/Tesla or
s
Here Ril (ri ) is regular function and it has a value of 5.79 × 10−5 eV/Tesla, thus for a magnetic field of sev-
jl (k ri ) cot δils − nl (k s ri ) at muffin-tin radius, whereas
s
eral Tesla, the order of magnitude of the Zeeman in-
the function Jils (ri ) is irregular at the origin and it has teraction energy, µB , is about 10−4 eV, which is too
a value of jl (k s ri ) at muffin-tin radius. δils is the phase small compared with the molecular field or the split-
shift for angular momentum l and for the potential ting between up and down spins in band energy. On
Vis (ri ), and ri> (ri< ) is the bigger (or the smaller) of the other hand, in the magnetic materials the spin-
ri , ri0 . orbit coupling coming from the magnetic anisotrophy
By using the initial states (for example in the case is much smaller than the splitting of magnetic band
of L2,3 edges): [7]. In this case, we can treat that the final states as
X 1 a perturbation of the normal spin states.
|jmj i = (lm s|jmj )φl j(r)Ylm (b r)|lsi (21) Using this scheme, we have calculated the compar-
m,s
2
ison between the MCD effect of L2 and L3 edges, we
where (lm 21 s|jmj ) are Clebsch-Gordan coefficients et found:
φl j(r) is the radial part of core hole state, we can then · + ¸ · + ¸
σ − σ− σ − σ−
write the cross section in the Green’s function: = −2 (27)
σ + + σ − L2 σ + + σ − L3
2m
σ(b ², ω) = −4παh̄ω 2 ×
X h̄ The result indicated in the equation (27) is observed
Im{hjmj |(b ² · r)∗ G↑ (k)(b
² · r)|jmj i correctly in the experiment for the gadolinium, cerium
mj and 5d transition metals. But it has slight different
² · r)∗ G↓ (k)(b
+hjmj |(b ² · r)|jmj i} (22) value for other rare earth materials, undoubtedly be-
cause of multiplet effect of 4f layer.
We have also calculated the K -edge of MCD effect
4 RESULT AND DISCUSSION
for BCC Iron using muffin tin potential approach [6].
The MCD effect can be obtained by evaluating the The lattice parameter is a = 2.86645 Å. To calculate
equation (22) for both the right and left polarizations the multiple scattering effect we employed 15 atoms
which correspond to the photon helicity h̄(−h̄). The consist of a central atom, eight nearest neighbours and
dipole interaction is [5]: six next nearest neighbours. Previously, we have cal-
culated the MCD using nine atoms.
· ¸1/2
1 4π The result of the calculation and its comparison
²b± · r = √ (x ± iy) = ∓ rYl±1 (b
r) (23) with the experiment are shown in the figure 1. The
2 3
calculation is in energy range from -30 until 130 eV,
²+ ) and left (b
respectively for right (b ²− ) polarizations. the maximum angular momentum used is l =5. We
By using the Green’s function in the equation (19) found that we obtain a good order of magnitude com-
and the initial states in (21), we can obtain the ab- pared with XANES (x-ray absorption near edge spec-
sorption cross section for the right and left polariza- troscopy) experiment, especially when the more scat-
tion. The difference between these absorptions is the tering atoms are involved. Furthermore, we can in-
magnetic circular dichroism (MCD) effect. terpret the contribution that interplays in the MCD
The equation (23) can used for MCD in L2,3 − edges, effect: at near edge this effect comes from the polar-
however for K−edge we use Hamiltonian: ization of spin of p and d neighbours, whereas at high
h̄2 2 energy, it is from the polarization of spin of p orbital
H=− ∇ + V (r) + µB σ · B + ζ(r) l · σ (24) of the absorber site.
2m
We further extend our calculation for the similar
The spin-orbit coupling can be written as effect on nickel and cobalt by employing 19 atoms.
X
ζi (ri )li · σi (25) We found a similarity of the result with the iron, both
i
for the calculation and the experiment.

0406-3
Muhammad Hikam J. Theor. Comput. Stud. 2 (2004) 0406

[6] V.L. Morruzi, J.F. Janak and A.R. Williams,

Calculated Electronic Properties of Metals,
Pergampn Press Inc., New York (1978).
[7] P. Bruno, Physical Review B39 (1989) 865.

Presented at the Workshop on Theoretical

Physics 2004 (WTP2K4), University of In-
donesia, Depok, Indonesia, 19th May 2004.

As a part of migration to the J. Theor. Comput.

Stud., this article has been republished from the
Physics Journal of IPS vol. C.
Figure 1: The MCD effect for BCC Iron

5 CONCLUSION

We can conclude that the Green’s function is very

useful to facilitate the calculation and to understand
the process of magnetic circular dichroism. By this
scheme, for L2 and L3 edges we obtained that the
calculated result is in good comparison with the ex-
perimental result for gadolinium, cerium and 5d tran-
sition metals. Whereas, for the K -edge, we found that
the calculation has a good order of magnitude com-
pared with XANES (x-ray absorption near edge spec-
troscopy) experiment.

ACKNOWLEDGMENT

The author would like to thank Christian Brouder for

showing the way to solve multiple scattering problem
and to Terry Mart for the help in preparing the format
of this paper.
JTCS

REFERENCES

[1] G.Y. Csnak, H.S. Taylor and R. Yaris, Advanced

Atomic Molecule Physics 7 (1971).
[2] C. Brouder and M. Hikam, Physical Review B43
(1991) 3809.
[3] M. Hikam, Proc. XVII National Physics Sympo-
sium and AAPS Seminar on Physics of Materi-
als, Yogyakarta (1998)
[4] M. Hikam, Proc. Seminar Nasional Bahan Mag-
net, Serpong (2000).
[5] J. Goulon, A. Rogalev, F. Wilhelm, Ch. Goulon-
Ginet, P. Carra, I. Marri and Ch. Brouder, Jour-
nal of Experimental and Theoretical Physics 97
(2003) 402.

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