The effect of the interface roughness on the magnetotransport properties in Ni 81 Fe 19 /Zr multi-layers
K. El Aidoudi a , A. Qachaou a,n , M. Lharch a , A. Fahmi a , H. Lassri b
a
LPMC Faculté de Sciences, Kenitra, Morocco
b
LPMatériaux Faculté de Sciences, Ain Chock, Casablanca, Morocco
a r t i c l e i n f o
Article history:
Received 15 January 2014 Received in revised form 7 July 2014
Accepted 9 July 2014 Available online 18 July 2014 Keywords:
A. Interfaces A. Magnetic materials A. Multilayers D. Magnetic properties D. Transport properties
a b s t r a c t
In this work, we study the effect of the chemical and/or structural disorder existing in the interface on the magnetotransport properties of the multilayered system NiFe/Zr. The assumption that the possible apparition of a disordered alloying phase NiFeZr is caused by diffusion of non-magnetic alloying Zr atoms at the interface is proposed. This assumed interfacial degradation is used to calculate the magnetoresistance rate MR
calðtÞ in the framework of Johnson–Camley semi-classical model. This allowed us to reproduce quite faithfully the experimental measured results MR
expð t Þ , con fi rming thus the important role of the interface roughness on the electronic transport properties. The behavior of calculated and measured magnetoresistance versus NiFe magnetic layer thickness (t ¼ t
NiFe) shows one maximum of 1.8% at t
NiFe¼ 80 A ̊ . When the thickness of the non-magnetic layer t
Zrvaries, the MR ð t
ZrÞ ratio shows an oscillatory behavior with an average period (7 A ̊ ). An overall weakness is showed by measured rate probably due to a degradation of the interface quality.
& 2014 Elsevier Ltd. All rights reserved.
1. Introduction
Even more than a decade after the discovery of the GMR effect in Fe/Cr thin fi lm multilayers [1 – 3], magnetic multilayers systems composed of alternating of magnetic and non-magnetic layers still attract considerable amount of scienti fi c interest because of their already proved utility in data storage and magnetic sensor technique.
One of the main aims of these studies is to improve the magnetic sensitivity (S ¼ Δ R = R Δ H). Thus a special attention was given to multilayers based on NiFe layers because of the soft magnetic character that they exhibit.Theoretical investigation showed that the GMR effect is closely related to the spin dependent scattering asymmetry effect of the conduction electrons both in bulk and interface which is a characteristic property of the transition metal (TM) elements like Fe and Ni. When an electron crosses one of the magnetic layers it is easily transmitted if its spin is parallel to the magnetization vector of the magnetic layer leading to weak MR ratio, whereas this electron is diffused in the contrary magnetic con fi g- uration supporting MR. Moreover the composition and the quality of the interface have an important role on the electronic transport proprieties [4]. In fact the values of the mean free path (MFP) and the spin dependent scattering asymmetry coef fi cient (SDSA) depend strongly on the interface roughness [5].
In this work, we present a study of the interface quality effect on the magnetotransport properties of Ni
81Fe
19/Zr magnetic multi- layer using the semi-classical model of Jhonson – Camely [6] based on the resolution of the Boltzmann transport equation and adapted to the interface degradation approach. A good agreement between experiment and calculation results is obtained.
2. Experimental methods
The multi-layer Ni
81Fe
19/Zr studied were prepared by the method of cathode sputtering with a magnetron by using NiFe and Zr targets of high purity. The pressure of the room before the deposit was about 6 10
8Torr, while the pressure of the gas (ultra-high purity Ar) was maintained constant at 2 10
3Torr.
The DC power was 80 W. The fi lms were deposited on a water- cooled Si(001) substrate maintained at a temperature of 293 K.
The multi-layers were prepared in two series of samples S
1and S
2follows as: (i) S
1: Magnetic layer thickness t
NiFevarying in 20 A ̊ r t
NiFer 120 A ̊ when the non-magnetic layer thickness was fi xed at t
Zr¼ 15 A ̊ ; (ii) S
2: non-magnetic layer thickness t
Zrvarying within 3 A ̊ r t
Zrr 20 A ̊ for a fi xed magnetic layer thickness at
t
NiFe¼ 30 A ̊. The choice of t
NiFe¼ 30 A ̊ is imposed by the fact of
being able to measure the impact of variation of the thickness of the non-magnetic Zr layer on the magnetotransport properties in NiFe/Zr. Indeed, according to high-angle X-ray (HXRD) diffraction measurements performed previously on this multilayered system [7], when the magnetic layers are thick (t
NiFeZ 60 A ̊ ) the effect of Contents lists available at ScienceDirect
journal homepage: www.elsevier.com/locate/jpcs
Journal of Physics and Chemistry of Solids
http://dx.doi.org/10.1016/j.jpcs.2014.07.011 0022-3697/& 2014 Elsevier Ltd. All rights reserved.
n
Corresponding author.
E-mail address: ahqachaou@yahoo.fr (A. Qachaou).
the non-magnetic Zr layer is practically masked, while for very low magnetic thicknesses (t
NiFer 20 A ̊ ) the effect of these magnetic layers is not probed (disappearance of the Bragg peak (111) NiFe at t
NiFe¼ 20 A ̊).
3. Results
3.1. Measured magnetoresistance rate MR
expThe dependence of the measured MR
expð t Þ ratio on magnetic and non-magnetic layer thickness in Ni
81Fe
19/Zr multilayer at room temperature is shown in Figs. 1 and 2 (Symbols). Fig. 1 depicts the evolution of MR
expð t ¼ t
NiFeÞ for the series S
1. The main features of this evolution show that for t
NiFe4 40 Å the MR increases with increasing t
NiFeand exhibits a maximum of about 1.8% at t
maxNiFe¼ 80 Å. The MR ratio then gradually decreases with increasing t
NiFeuntil it reaches a minimum of about 0.5% at t
NiFe¼ 120 Å. For t
NiFeo 40 A ̊ , a very weak MR ratio is obtained, showing that the magnetotransport process is strongly blocked at the interface, and generally the maximum ratio MR
maxobtained in the present structure is much smaller compared to other ratios obtained in similar systems such as NiFe/Cu [8,9].
Fig. 2 shows the curve MR
expð t
ZrÞ for the series S
2. MR
expð t
ZrÞ presents an oscillatory behavior re fl ecting the oscillations of the exchange coupling between ferromagnetic (F) and antiferromag- netic (AF) con fi gurations of the magnetization vectors of the adjacent magnetic layers NiFe. It shows clearly the existence of two oscillations. The fi rst one at t
Zr¼ 7 A ̊ with ratio of 0.4% and the second one at t
Zr¼ 14 A ̊ with ratio of 0.3%. These values of MR peaks are relatively weak because they are obtained for fi ne magnetic layers (t
NiFer 40 A ̊ ) where a disorder caused by the diffusion of non-magnetic alloying metal Zr in the interface provokes an important degradation of crystallinity of this interface where the existence of an amorphous phase was shown experi- mentally [7]. The average distance between MR peaks gives a period of oscillations of 7 Å which is inferior to these observed in other multilayer based on similar transition metal alloys deposited on copper such as NiFe/Cu (8.5 Å) and NiFeCo/Cu (8.5 Å) [9].
3.2. Calculated magnetoresistence ratio MR
calThe calculation of magnetoresistence ratio MR
calis carried out within the framework of the semi-classical Johnson – Camley (J – C) model based on the Boltzmann transport equation. The J – C model
takes account primarily of the interaction mixing the s – d states contribution to the exchange coupling between two successive magnetic layers NiFe and based on the assumption of spin- dependent scattering asymmetry of the conduction electrons.
The other contribution to the exchange described by RKKY approximation is known to be coarse enough in the case of 3d-TM and alloys like NiFe studied here [10]. In the multi-layer containing TM or their alloys such as NiFe/Zr the GMR effect is attributed to the mechanisms of scattering depending on spin. The electronic conduction is supposed to be carried out in two channels of electrons with independent opposite spins ( σ ¼ ↑; ↓ ).
Indeed, the existence of a fairly strong local magnetic fi eld in these TM is a sign of a strong separation of spin exchange. The Fermi surfaces with majority and minority spins can have very different topological forms leading to notable differences in densities of states corresponding to the Fermi level [11]. Consequently the electronic probabilities of s – d transitions are different for the two directions of spin leading to two distinct currents. Then we assumed that the electron transport through the multilayer is governed by the Boltzmann equation for the electron distribution function f ð ! r ; !Þ v given in the relaxation time τ approximation by
! v : ! ∇
! r f ð ! r ; !Þðe v = m Þ ! E
! ∇
! v f ð ! r ; !Þ ¼ ððf v ð ! r ; !Þ v f
0ð !ÞÞ=τÞ v . Here ð ! r ; !Þ v is the canonical pair of position and velocity of an electron and f
ois the Fermi – Dirac distribution. Then we can write, for each spin σ : f
σð ! r ; !Þ ¼ v f
σ0ð !Þþ v g
σð ! r ; !Þ v , where g
σð ! r ; !Þ v de fi nes the difference between the ground state population f
σ0ð !Þ v and the perturbed state population f
σð ! r ; !Þ v owing to the interfaces and the electric fi eld. It corresponds to only electrons involved in transport phenomena. For a static and uniform electric fi eld ! E
applied along the direction ! x of a multilayered system stacked along the direction ! z , the translational invariance in the plane of the layers (x,y) implies that the fi nal solution depends only the direction ! z and the Boltzmann equation becomes
∂
∂ z g
σ7ð ! r ; !Þþ v 1 τ
σv
zg
σ7ð ! r ; !Þ ¼ v eE mv
z∂
∂ v
xf
0ð !Þ v ð 1 Þ
leading to the solution g
σ7ð z ; v
zÞ ¼ eE τ
σm
∂ f
0∂ v
x1 þ F
σ7exp z τ
σv
zð 2 Þ where F is an arbitrary function of velocity v , determined by the boundary conditions, e and m denote respectively the electron
Fig. 1.Comparison of MR
calðtNiFeÞ(continuous curve) with MR
expðtNiFeÞ(symbols).
Fig. 2.
Variation of MR
calðtZrÞ(continuous curve) and MR
exp(t
Zr) (Symbols).
charge and electron effective mass and τ
σis the spin-dependent relaxation time. Once the Fs are known, and thus the g, the current density in each region may be given by I ð z Þ ¼ 2e ½ m = h
3R v
x½ g
↑ð v
z; z Þþ g
↓ð v
z; z Þ d
3v and then the current density in the whole structure is I ¼ R
I ð z Þ dz and thus the effective resistivity may be found.
Therefore, calculating the current in the two con fi gurations of magnetization (parallel (P) and anti-parallel (AP)), we can obtain the MR ratio for the entire structure by
MR
cal¼ ρ
Pρ
APρ
AP¼ I
PI
API
APð 3 Þ
ρ
APand ρ
P(I
APand I
P) are respectively the resistivities (electrical currents) in the antiparallel and parallel con fi gurations of magnet- izations.
The electronic mean free path (MFP) λ
σ, the relaxation time τ
σand the spin-dependent scattering asymmetry (SDSA) coef fi cient α ¼ λ
↑=λ
↓used to calculate MR ratio are strongly dependent on the nature and quality of the considered interface. It is therefore necessary to specify these interfaces.
3.3. The NiFe/Zr interface con fi guration proposed
In the present study, we supposed that the interfaces between the magnetic NiFe and non-magnetic Zr layers to be rough due to the intrinsic effects (possible extrinsic effects caused by impurities added to the interfaces are neglected). For this purpose, we consider that each interface NiFe/Zr constitutes a mixed zone which contains a disordered phase constituted by a mixture of aggregates or ‘ particles ’ of alloys MZr (M ¼ Ni, Fe, NiFe) formed through an interdiffusion of atoms from magnetic and non- magnetic layers. This disorder is probably caused by the diffusion of non-magnetic alloying metal Zr whose introduction, even in small contents, can lead to an amorphous state as observed experimentally [7]. Furthermore the low iron content in the studied samples, and the weak miscibility between zirconium and iron, in addition to a relatively very low mobility of Zr atoms [12], can suggest that the probability of existence of FeZr particle within the interface is negligible. Similarly, the two elements Fe and Zr both promote a reduction of Ni [13]. Thus, the NiFe/Zr interface probably contains a con fi guration consisting of a mixture of ‘ particles ’ NiZr, NiFe and NiFeZr alloys. Fig. 3 depicts a rough partition of the interface containing these ‘ particles ’ with a predominance of NiFeZr phase around the center of the interface.
On the other hand, the rate of diffusion of Zr atoms in the magnetic layer is very small; the formed alloy particles (NiZr and NiFeZr) correspond to very low contents of Zr promoting amor- phization of these particles [14] which is in fact revealed by interfacial texture measurements in studied multilayer NiFe/Zr [7]. Thus, the overall weakness showed by our measured magne- toresistence rate MR
expcan be explained by the existence of this
amorphization related to the reduced crystallinity of the interfaces when Zr atoms are introduced. The formation of such disordered alloying phase in the interfaces that we suggest seems to be a general characteristic of this type of multilayer [8,15 – 17].
As a fi rst approximation, we considered that the alloy phase NiFeZr can be regarded as playing the same role as that of a layer of impurities with a thickness ʻ t
impurityʼ ¼ t
alloyinserted in the mixed zone such that t
alloyo t
mx. The thickness t
mxis fi xed while t
alloydepends on magnetic layer thickness t
NiFe. If t
0mxis the thickness of the phase NiZr (i.e. is one of the interface in the absence of the disordered phase), we have t
0mxþ t
alloy¼ t
mx¼ cte.
Thus, in the limit of low concentrations of these ‘ impurities NiFeZr ’ , the resistivity of each canal of spin ( σ ¼ ↑ or σ ¼ ↓ ) in the mixed zone, due to the ‘ particles ’ NiZr and impurities NiFeZr diffusing into NiFe is given by the Matthiessen rule ρ
σmxðμ
0mx; μ
alloyÞ ¼ μ
0mxρ
0mxσþμ
alloyρ
σalloy, where μ
alloyand ρ
σalloyare respectively the weight and the resistivity of the alloying phase
‘ NiFeZr ’ , while μ
0mxand ρ
0mxσare respectively the weight and the resistivity of NiZr alone in the mixing zone. Then, the facts that μ
0mxþμ
alloy¼ 1 and t
0mxþ t
alloy¼ t
mx¼ cte allow us to de fi ne μ
alloyand μ
0mxas μ
alloy¼ ð t
alloy= t
mxÞ and μ
0mx¼ ð t
0mx= t
mxÞ . Therefore, substituting in the Matthiessen rule above, we have for each spin σ : ρ
σmxðμ
0mx; μ
alloyÞ ¼ ð t
0mx= t
mxÞρ
0mxσþð t
alloy= t
mxÞρ
σalloy. The SDSA coef fi cient α
mx, de fi ned by α
mx¼ ðρ
↓mx=ρ
↑mxÞ , is then given by α
mx¼ ð t
alloyρ
↓alloyþ t
0mxρ
0mx↓= t
alloyρ
↑alloyþ t
0mxρ
0mx↑Þ Eliminating t
0mxby t
0mx¼ t
mxt
alloy, we have the expression
α
mx¼ t
alloyt
alloyα
alloyþα
alloyKðt
mxt
alloyÞ þ t
mxt
alloyðt
alloyα
0mx=KÞþα
0mxðt
mxt
alloyÞ
1
ð 4 Þ with K ¼ ρ
0mx↓=ρ
↓alloyand α
alloy¼ ρ
↑alloy=ρ
↓alloy. Similarly, the mean free path in the mixed zone λ
mxcan be obtained by assuming that the contribution of the resistivity term to the mean free path inverse ρλ is constant. So λ
0mxρ
0mx¼ λ
mxρ
mxand λ
mx¼ ðρ
0mx=ρ
mxÞλ
0mxwhere ðρ
0mx=ρ
mxÞ ¼ ð t
0mxðρ
0mx↑þρ
0mx↑ÞÞ=ð t
0mxðρ
0mx↑þρ
0mx↑Þþ t
alloyðρ
↑alloyþρ
↓alloyÞÞ is the ratio of arithmetic means of the resistivities in the mixed zone without and with impurities. Then we have
λ
mx¼ ð t
mxt
alloyÞð 1 þα
0mxÞ
ð t
mxt
alloyÞð 1 þα
0mxÞþð t
alloyα
0mx= K Þð 1 þð 1 =α
alloyÞÞ λ
0mxð 5 Þ Moreover, the extent of phase alloy t
alloyis directly related to the thickness of the magnetic layer. We assumed that t
alloyvaries inversely with t
NiFe. As t
NiFedecreases, more t
alloyextends in the mixed zone follows as:
t
alloyd t
NiFeA ð 6 Þ
The constant A is an adjustment parameter. The formed alloying phase can be characterized by concentration c de fi ned by 0 r c ¼ t
alloy= t
mxr 1. The zero value of c describes a smooth inter- face, while c ¼ 1 (or c ¼ 100%) means that the disordered alloying phase extends over the entire mixed zone. The interface properties α
mxð c Þ , λ
mxð c Þ and λ
σmxð c Þ can then be obtained as functions of the alloy concentration c using Eqs.(4) – (6) follows as:
α
mxð c Þ ¼ c
c α
alloyþα
alloyK ð 1 c Þ þ 1 c ð c α
0mx= K Þþ α
0mxð 1 c Þ
1
ð 7 Þ
λ
mxð c Þ ¼ ð 1 c Þð 1 þα
0mxÞ
ð 1 c Þð 1 þα
0mxÞþð c α
0mx= K Þð 1 þð 1 =α
alloyÞÞ λ
0mxð 8 Þ Using λ
mxas an arithmetic mean of λ
σmx, i.e. λ
mx¼ ðλ
↑mxþλ
↓mx= 2 Þ , and α
mx¼ ðλ
↑mx=λ
↓mxÞ ¼ ðτ
↑mx=τ
↓mxÞ , we have
Fig. 3.
The proposed representation of NiFe/Zr interface.
λ
↑mxð c Þ ¼ 2 α
mxð c Þλ
mxð c Þ
α
mxð c Þþ 1 ð 9a Þ
λ
↓mxð c Þ ¼ 2 λ
mxð c Þ
α
mxð c Þþ 1 ð 9b Þ
(9a) and (9b) are different if α
mxð c Þa 1. The corresponding relaxa- tion times τ
σmxð c Þ are then deducted using λ
σmx¼ τ
σmxv
Fwhere v
F, is the velocity of electrons at the Fermi level, as follows
τ
↑mxð c Þ ¼ λ
↑mxð c Þ v
F¼ 2
v
Fα
mxð c Þλ
mxð c Þ
α
mxð c Þþ 1 ð 10a Þ
τ
↓mxð c Þ ¼ λ
↓mxð c Þ v
F¼ 2
v
Fλ
mxð c Þ
α
mxð c Þþ 1 ð 10b Þ
This allows us to express the solution g
σ7ð z ; v
zÞ (Eq. 2) of the Boltzmann equation (Eq. 1), used to calculate the MR, in terms of the properties of the interface as
g
↑7ðz; v
z; α
mx; λ
mx; cÞ ¼ 2eE m v
F∂ f
0∂v
xα
mxð c Þλ
mxð c Þ
α
mxðcÞþ1 1 þF
↑7exp z 2
v
Fv
zα
mxð c Þþ 1 α
mxðcÞλ
mxðcÞ
ð 11a Þ g
↓7ð z ; v
z; α
mx; λ
mx; c Þ ¼ 2eE
m v
F∂f
0∂v
xλ
mxðcÞ
α
mxðcÞþ1 1 þ F
↓7exp z 2
v
Fv
zα
mxðcÞþ1 λ
mxðcÞ
ð 11b Þ 4. Analysis and discussion
4.1. Obtained MFP and SADS coef fi cient of mixed zone
The description of the MR effect in alloys can be qualitatively made taking into account both the mechanisms of electron diffusion in inhomogeneous medium and the magnetic properties of small ‘ particles ’ that are very different from those of bulk ferromagnetic. In the present study, the dependence of magneto- transport properties on the evolution of impurity ‘ particles ’ (con- centration c, α
mx, λ
σmxand τ
σmx) in the mixed zone is discussed phenomenologically assuming that the effect of introducing of Zr atoms is the parameter most in fl uencing the mechanisms of electronic diffusions. We assumed indeed, that the insertion of Zr atoms even in very small quantities causes amorphization of
‘ particles ’ alloy FeNiZr in the mixed zone. This effect, in addition to the alloying effect, could induce signi fi cant change in the electro- nic structure. It is also known for this type of transition-metal base amorphous alloys that the main contribution to the Fermi level still arises from d electrons in spite of the important reduction which may be due, among other things, to the effects of charge transfer and/or hybridization. The problem of NiFeZr impurity in the mixed zone can be approximately discussed by analogy with that of a magnetic impurity state in transition-metal base amor- phous alloys treated basically in d-band hosts.
Qualitatively, the main contribution to perturbation potential V
mxs ddue to Zr atom introduction causes a mixture of states ‘ s ’ of Zr and ‘ d ’ of the transition metal. This may induce signi fi cant changes in the topology of the Fermi surfaces. The transition probabilities W
mxs-d, the relaxation times τ
σmx, the mean free path λ
σmxand densities of states D
σdð E
FÞ in the vicinity of these Fermi surfaces can also undergo signi fi cant distortion following the introduction of Zr atoms. These quantities can be linked roughly by a relation- ship type Fermi rule:
mxW
smxdV
s dmxD E
d Fh . Thus, the
reduction in the mean free path in the mixed zone λ
σmx(ie the resistivity ρ
σmxincreases) when the concentration c of the dis- ordered phase NiFeZr increases could mean that the mixture of states (V
mxs d) and or the density of states D
dð E
FÞ increased with increasing c.
In Fig. 4, we report the variation of the SDAS coef fi cient α
mxversus alloying phase concentration c. It emerges that α
mxð c Þ shows drastic decrease inside the interval 6 : 7 rα
mxð c Þr 1. Indeed, it drops by 83.5% at c ¼ 46%. This concentration is related to the magnetic layer thickness t
NiFe¼ 30 A ̊ beyond which important modi fi cation in MR behavior and structure can be expected.
Indeed the XRD results show an absence of crystalline structure for t
NiFeo 30 Å [7] which re fl ects a maximum disorder and con- sequently a very weak MR ratio. Therefore the spin dependent scattering asymmetry process – directly responsible for the GMR phenomena – is strongly distorted as soon as the proportion of disordered phase increases in the mixed zone, leading to very weak MR ratio, con fi rming the weakness of MR measured values.
The highest value of α
mxð c Þ is obtained for c ¼ 0 and it is equal to:
α
mxð c ¼ 0 Þ ¼ α
0mx¼ 6 : 7. It can be related to a con fi guration where the interface contains a mixture composed only of binary alloys NiFe (in majority) corresponding to α
NiFe9 : 5[18] and NiZr (in minority) with α
NiZr7 : 5[19]. The lowest value α
mxð c ¼ 1 Þ ¼ α
1mx1, describes the important modi fi cation of the interface magnetic state caused by the introduction of Zr atoms leading, even for weak contents of Zr atoms, to a paramagnetic state with
Fig. 4.
Variation of
αmx(c).
Fig. 5.