Physica B 353 (2004) 46–52
Thermal variation of magnetization in Ni/Vmultilayers
K. Benkirane
a,, R. Elkabil
a, A. Hamdoun
a, M. Lassri
b, M. Abid
b, H. Lassri
b, R. Krishnan
caLaboratoire de traitement d’information, Faculte´ des Sciences Ben’Msik Sidi-Othmane, B.P.7955 - Sidi-Othmane, Casablanca, Morocco
bLaboratoire de Physique des Mate´riaux et de Micro-e´lectronique, Faculte´ des Sciences Ain Chock, Universite´ Hassan II, B.P. 5366 Maˆarif, Route d’El Jadida, km-8, Casablanca, Morocco
cLaboratoire de Magne´tisme et d’Optique, URA 1531, 45 Avenue des Etats Unis, 78035 Versailles Cedex, France Received 21 August 2004; accepted 31 August 2004
Abstract
The magnetic properties of Ni/Vmultilayers, prepared by the RF sputtering method, have been systematically studied by magnetic measurements. The magnetization decreases with a decrease in Ni layer thickness
tNiand the analysis of the results at 5 K indicates the presence of a dead Ni layer about 12 A˚ thick. The effective anisotropy
Keffof Ni/Vmultilayers is obtained using a torque magnetometer. The interface contribution to the magnetic anisotropy is practically negligible. A spin-wave theory has been used to explain the temperature dependence of the magnetization and the approximate values for the bulk exchange interaction
Jb;surface exchange interaction
JS;and the interlayer coupling strength
JIfor various Ni layer thicknesses have been obtained.
r
2004 Elsevier B.V. All rights reserved.
PACS:75.70.i; 75.60.Ej; 75.30.Gw; 75.30.Et
Keywords:Ni/Vmultilayers; Magnetization; Magnetic anisotropy; Exchange interactions
1. Introduction
Magnetic multilayers with suitable magnetic properties would offer improvements over con- ventional magnetic materials for applications in
high-density magnetic recording, both as recording media [1] and as heads [2]. One of the main requirements for perpendicular recording and magneto-optic recording is a high perpendicular magnetic anisotropy, which can be achieved in magnetic multilayers.
Compared with the corresponding bulk materi- als, ultrathin films exhibit drastic differences in their magnetic properties. Long-range ferromag- netic order in solids is a collective phenomenon
www.elsevier.com/locate/physb
0921-4526/$ - see front matterr2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.physb.2004.08.025
Corresponding author. Ecole Royale Navale, Physique, 59 rue Guercif, Appt 6, Casablanca, Morocco. Tel.: +212 22 484 160; fax: +212 22 506 188.
E-mail address:karbenkirane@yahoo.fr (K. Benkirane).
depending strongly on the coordination number, which is effectively diminished in films consisting of only one or a few monolayers. In addition, the lowered dimensionality of thin films in relation to the bulk leads to important changes in the shape of magnetization as a function of temperature and in critical exponents.
Research on interlayer exchange coupling of magnetic multilayers and double layers is becom- ing active, and many characteristics of interlayer coupling have been discovered, such as antiferro- magnetic, ferromagnetic, and oscillating exchange couplings [3,4]. The MðTÞ behavior and the Curie temperature T
Cwill of course not only be determined by an interlayer coupling but also by the interplay between anisotropy [5], size effects [6], and coupling effects. Furthermore, interdiffu- sion causing graded interfaces and disorder result- ing in a distribution of exchange interactions can play an important role. Especially, when the magnetic layer thickness is in the monolayer regime the latter two factors might dominate the temperature dependence.
The magnetic properties of multilayers are strongly dependent on their detailed structure and composition, which are determined by the growth conditions used during fabrication [7–9].
For example, the degree of mixing between adjacent layers determines the amount of Ni able to contribute to the magnetic properties of the film, and the degree of crystallographic texture within the layers, combined with any surface anisotropy present, determines the overall aniso- tropy of the multilayers.
As Ni is ferromagnetic, a study of the magnetic properties of this system also can bring additional information on the state of the interface. There- fore, we have undertaken such a study and describe our results here. We calculate the thermal variation of the magnetization as a function of Ni layer thickness and compare it, qualitatively and quantitatively, with experimental results.
2. Experimental
The multilayers were deposited onto water- cooled glass substrates by RF diode sputtering.
The chamber was first evacuated to a pressure of 1–2 10
7Torr using a turbomolecular pump.
Argon of 5N purity was used as the sputter gas and its pressure was kept constant at 6 10
3Torr: The RF power density was 2.1 W/cm
2. The thickness of each layer was monitored by individual quartz oscillators. The Ni layer thick- ness t
Nivaried from 18 to 96 A˚ and that of Vlayer t
Vwas fixed at 20 A˚. The number q of bilayers were in the range 5–15. All the samples were grown on vanadium buffer layers 100 A˚ thick. In all the cases the first and the last layers were V. In what follows, the growth parameters of the samples will be indicated as ðt
Ni=t
VÞ
q: The samples were studied using the X-ray diffraction. Magnetization M was measured using a vibrating sample magnetometer under magnetic fields up to 2 T and in the temperature range 5–300 K.
3. Results and discussion
The multilayer structure is found, by X-ray diffraction, to be polycrystalline and has FCC Ni(1 1 1) texture in the film growth direction (Fig. 1). FCC Ni (1 1 1) and BCC V(1 1 0) have close lattice plane spacing (2.034 and 2.14 A˚, respectively) in the film growth direction. So it is reasonable to consider that atomic intermixing may occur during sputtering. Ni and Vlayers are
Fig. 1. High-angle X-ray diffraction pattern of Ni(40 A˚)/
V(20 A˚) multilayer using CuKaradiation.
complicated alloys, which makes the Ni/Vmulti- layer a compositional modulated structure con- sisting of Ni- and V-rich layers.
The hysteresis loops of Ni/Vmultilayer mea- surements in parallel and perpendicular fields reveal that the easy magnetization of all our Ni/Vmultilayers lies in the film plane. The magnetization decreases strongly with a decrease in Ni layer thickness. Due to the decrease in the Curie temperature with t
Ni; the decrease in M at 300 K is stronger for thinner Ni layers. Therefore, let us consider the results only at 5 K which are shown in Fig. 2. The general t
Nidependence of M could be explained in terms of a dead layer of Ni at each interface, due to alloying effects. The thick- ness of such a Ni layer is estimated to be in the range 11–13 A˚. The calculated curves are also shown in Fig. 2.
Torque studies yield the effective anisotropy K
eff: The t
Nidependence of K
effcould be analyzed on the basis of the well known phenomenological model which predicts the following relation:
K
eff¼ K
Vþ 2K
S=t
Ni; where K
Vand K
Sare the bulk and surface anisotropies (the latter is the contribution of the surface atoms), respectively.
The bulk anisotropy K
V¼ 2pM
2þ K
cryst; where
the first term is the demagnetizing energy arising from geometry and the second term is the crystal- line anisotropy.
By plotting K
efft
Nias a function of Ni one obtains a straight line whose slope is K
V; and the intercept on the ordinate axis gives 2K
S: So graphically one obtains these values. Fig. 3 shows the results at 5 K in order to avoid the effects arising when lowering T
Cfor thinner Ni layer samples. The present results show that there is no contribution to K
Sfrom the Ni atoms. This is in agreement with our result on Ni/Ag [10] and on Ni/Pd by den Broeder et al. [11]. However, we have shown that in the Ni/Pt system a strong perpendicular anisotropy is present arising from the surface anisotropy [12]. It is well known that the surface anisotropy arises from the local crystal fields and hence should not only depend on the state of the interface but also on the electronic structure of the neighboring metal. It can be seen that all the samples studied show K
effo 0; in other words, the magnetization is in-plane.
Let us now examine the volume anisotropy energy K
V: To first order the magnetic cubic anisotropy energy of a single Ni crystal is K
cryst¼ 5:7 10
4erg=cm
3at 0 K [13]. The observed anisotropy energy equals K
V¼ 1:5 10
6erg=cm
3; which is almost 26 times larger than
Fig. 2.tNi dependence of the magnetization at 5 K; the solid lines represent the variation of the magnetization assuming
dead Ni layers of thickness 12 A˚. Fig. 3. Variation of the productKefftNiwithtNiat 5 K.
the anisotropy energy of Ni bulk. The demagnetiz- ing energy in the films results in the increase of K
V: Basically, the two main sources of the magnetic anisotropy are magnetic dipolar interaction and the spin–orbit interaction. Because of its long range character, the dipolar interaction generally results in a contribution to the anisotropy, which depends on the shape of the specimen. It is of particular importance in thin films, and is largely responsible for the in-plane magnetization usually observed. The shape effect of dipolar interaction can be described, via an anisotropic demagnetizing field.
In all real systems, there is, in addition to any short-range exchange interaction, a long-range dipole–dipole interaction always present between the magnetic moments. In many theoretical studies of magnetic systems this dipolar interaction is neglected, the rational for this being the small magnitude of the dipolar interaction relative to the magnitude of the exchange interaction.
The low-temperature magnetization was studied in detail for a few samples. Plots of the magnetiza- tion, for different thicknesses of Ni layers, versus temperature were drawn for the Ni/Vmultilayers (Fig. 4). According to spin-wave theory, the
temperature dependence should follow the relation Mð5KÞ MðTÞ
Mð5KÞ ¼ BT
3=2: (1)
In all cases this behavior is observed for temperatures as high as T
C=3: The spin-wave constant B decreases from 92 10
6K
3=2for t
Ni¼ 18 A to 26 ( 10
6K
3=2for t
Ni¼ 96 A: ( These values are much larger than the value of 7:5 10
6K
3=2found for bulk Ni.
The B versus 1=t
Niis plotted for the samples with 18 p t
Nip 96 A in ( Fig. 5. It is seen that the experimental points align well in a straight line.
The values extrapolated to 1=t
Ni¼ 0 are in good agreement with those found for the bulk Ni. It was observed that the parameters B in Eq. (1) depend on t
Niaccording to
Bðt
NiÞ ¼ B
1þ B
S=t
Ni; (2) where B
1is the bulk spin-wave parameter of Ni and B
Ssurface B value. The surface anisotropy strongly affects the thickness dependence of magnetization. The linear relation between the spin-wave parameter B and the reciprocal of the magnetic film thickness was reported for Co/V multilayers [14] and Fe (1 1 0) films on W(1 1 0)
Fig. 4. Calculated (continuous line) and measured (symbols) temperature dependence of the normalized magnetization of
Ni/Vmultilayers with varying Ni thickness. Fig. 5. Thet1Ni dependence of theB.
[15,16]. Recently, Pinettes et al. [17] examined the influence of the anisotropy on the thickness dependence of the spin-wave excitation spectra and calculated the thermal variation of magnetiza- tion as a function of film thickness.
To understand better how the interlayer ex- change coupling between neighboring Ni layers affects the magnetic behavior of these films, we extended the model for spin waves in ferromag- netic thin films proposed by Pinettes et al. [17] to the case of ferromagnetic/non-magnetic multi- layers. We suppose that the multilayer ðX
n=Y
mÞ
qis formed by an alternate deposition of a magnetic layer ðXÞ and a non-magnetic one ðYÞ: The multilayer is characterized by the number ðqÞ of bicouches ðX=YÞ; the number ðnÞ of atomic planes in the magnetic layer m; and the number ðmÞ of atomic planes in the non-magnetic layer. We chose the lattice unit vectors (~ e
x;~ e
y; ~ e
zÞ so that ~ e
zis perpendicularto the atomic planes. We note by S
iamthe spin operator of the atom iði ¼ 1; 2; . . . ; NÞ in the plane aða ¼ 1; 2; . . . ; nÞ of the magnetic layer mðm ¼ 1; 2; . . . ; qÞ:
The system Hamiltonian is given by
H ¼ H
eþ H
aþ H
z: (3) H
edescribes the exchange interactions in the same magnetic layer (bulk and surface) as well as the exchange interactions between adjacent magnetic layers
H
e¼ J
bX
b hiam;jamiS
iamS
jamþ X
hiam;ja0mi
S
iamS
ja0m" #
J
sX
s hiam;jamiS
iamS
jamJ
IX
I hiam;ja00m00iS
iamS
ja00m00; ð4Þ
where J
band J
Sare the bulk and surface exchange interactions. J
Iis the interlayer coupling strength which depends on the number m of atomic planes in the non-magnetic layer.
The contribution of the surface anisotropy is estimated by
H
a¼ D
?X
iam
s
S
Ziam2þ D
kX
iam
s
ðS
Xiam2S
Yiam2Þ; (5)
where D
?and D
kare the surface anisotropy parameters for the uniaxial out of plane and in- plane components.
The Hamiltonian H
zis considered in the case where a magnetic field H
appis applied to the system in the z direction:
H
Z¼ gm
BH
appX
iam
S
ziam: (6) Further we denote by P
Xthe summation, the summation on the sites of the bulk layer planes by X ¼ b; that on surface layer planes by X ¼ S and on the surfaces planes coupled via the non- magnetic layer by X ¼ I: The symbol h i denotes the pairs of nearest-neighbor atoms or adjacent magnetic planes.
In the Holstein–Primakoff formulation [18], the creation and annihilation operators (a
iamand a
þiam) for each atomic spin are related to the spin operators by
S
Xiamþ iS
Yiam¼ ð2SÞ
1=2f
iamð2SÞa
iamand
S
XiamiS
Yiam¼ ð2SÞ
1=2a
þiamf
iamð2SÞ: ð7Þ In the framework of non-interacting spin-wave theory, the linear approximation of the Holstein–- Primakoff method is sufficient to describe the main magnetic behavior and the correction terms are quite-small at low temperatures ðT o T
C=3Þ [19,20]. So, the value of f
iamð2SÞ is fixed to 1.
We pass from atomic variables ða
iam; a
þiamÞ to magnon variables ðb
kam; b
þkamÞ after a two-dimen- sional Fourier transformation and we show that H ¼ H
0þ A X
k;am
s
b
kamb
kamþ b
þkamb
þkamþ X
k;am
s
B
kb
þkamb
kamþ X
k;am
b
C
kb
þkamb
kamþ X
k;ham;a0mi
D
kb
þkamb
ka0mþ X
I k;ham;a00m00iE
kb
þkamb
ka00m00; ð8Þ
where A ¼ 2D
kS;
B
k¼ ðJ
sð2n
jjðl
þkþ l
kÞÞ þ 2J
bn
?þ 2D
?ÞS
þ 2J
In
lS þ gm
BH
app;
C
k¼ ð4n
?þ 2n
kðl
þkþ l
kÞÞJ
bS þ gm
BH
app; D
k¼ J
bSl
0k;
E
k¼ J
ISl
00k: ð9Þ
H
0is a constant term, coefficients l
þk; l
k; l
0kand l
00kdepend on the crystallographic structure of the magnetic layer. n
krepresents the number of nearest-neighbor sites in the same atomic plane, while n
?ðn
lÞ is the number of nearest neighbors in the adjacent plane in the same (adjacent) magnetic layer. For FCC (1 1 1) (n
k¼ 6 and n
?¼ 3) with the lattice constant a and in the case where the non-magnetic layer does not disturb the succession order of the magnetic atomic planes ðn
l¼ 3Þ:
l
þk¼ l
k¼ 4 cosðak
xp
6=4Þ cosðak
yp 2=4Þ þ 2 cosðak
yp 2=2Þ
l
0k¼ l
00k¼ 4 cosðak
xp 6=12Þ cosðak
yp 2=4Þ þ 2 cosðak
xp
6=6Þ: ð10Þ
The spin system is characterized by 2nq 2nq equations, and then the resulting secular equation is given by a ð2nq 2nqÞ matrix:
W
ð2nq2nqÞ¼ U
ðnqnqÞV
ðnqnqÞV
ðnqnqÞU
ðnqnqÞ!
;
where
U
ðnqnqÞ¼
UðnnÞ1 UðnnÞ2 UðnnÞ3 UðnnÞ1 UðnnÞ2
UðnnÞ3 UðnnÞ1 UðnnÞ2 UðnnÞ3 UðnnÞ1 0
BB BB BB BB BB BB BB B@
1 CC CC CC CC CC CC CC CA
;
V
ðnqnqÞ¼
V
ðnnÞV
ðnnÞ0
B B B B B B B B
@
1 C C C C C C C C A
;
U
ðnnÞ1¼
B
kD
kD
kC
kD
kD
kC
kD
kD
kB
k0
B B B B B B B B B B B B B B
@
1 C C C C C C C C C C C C C C A
;
U
ðnnÞ2¼
0 0
0
E
k0 0 0
B B B B B B B B B B B @
1 C C C C C C C C C C C A
;
U
ðnnÞ3¼
0 0 E
k0
0 0
0 B B B B B B B B B B B @
1 C C C C C C C C C C C A
;
V
ðnnÞ¼ 2A
0
0 2A 0
B B B B B B B B B B B B B B
@
1 C C C C C C C C C C C C C C A
: ð11Þ
Among the 2 ðn qÞ eigenvalues of the matrix
W
ð2nq2nqÞ; we consider the n q positive ones
which correspond to the n q magnon excitation branches o
rkðr ¼ 1; 2; . . . ; n qÞ: The reduced magnetization versus temperature is computed numerically from
mðT Þ ¼ 1 1 N
knqS
X
k;r
1
expðo
rk=k
BTÞ 1 : (12) The coefficient N
kindicates the number of k points taken in the first Brillouin zone.
Using Eq. (12), satisfactory fits were obtained for the MðT Þ data for all of the Ni/Vfilms. The interfacial alloy is considered within the model by using the real magnetic layer thickness (Ni layer thickness t
Ni-dead layer thickness).
The MðTÞ theory curves obtained from the fits for the t
Ni¼ 18; 24, and 48 A˚ films are shown in Fig. 4, well matching the experimental data points.
The values of J
b; J
S; and J
Iobtained from the fits are listed in Table 1 for all films (taken S ¼ 0:3 and D ¼ 0 K). The derived bulk exchange interaction constants all consistently fall in the range expected for the exchange interaction of bulk Ni [13], compared to the bulk exchange interaction. How- ever, the interlayer coupling is considerably weak.
4. Conclusions
In conclusion, we have prepared Ni/Vmulti- layers by RF sputtering. The surface and volume
contributions to the anisotropy have been deter- mined at 5 K. The spin-wave constant B is found to decrease inversely with t
Ni: A simple model has allowed us to obtain numerical estimates for the exchange interactions and the interlayer coupling strength for various Ni layer thicknesses.
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Table 1
The fitting results from Eq. (12) for NiðtNiÞ=VðtV¼20AÞ:( Jbis the bulk exchange interaction between neighbouring Ni atoms, JSis the surface exchange interaction, andJI is the interlayer coupling
tNiðAÞ( Jb=kB(K) JS=kB(K) JI=kB(K)
18 300 49 0.05
24 301 48 0.07
48 300 49 0.11