Journal of Magnetism and Magnetic Materials 5 (1977) 23-34 North-ltoUand Publishing Company

SPONTANEOUS RESISTIVITY ANISOTROPY IN Ni ALLOYS

O. JAOUL, I.A, CAMPBELL and A. FERT Laboratoire de Physique des Solids *, UniversitY"Paris-Sud, 9 ! 405-Orsay, France Received 28 September 1976, in revised form 4 November 1976 We present experimental results for the resistivity anisotropy of Ni alloys containing transition impurities, rrom these results and those of other authors, we show that the Smit spin mixing mechanism is dominant in all cases where there is no d virtual bound state at the spin t Fermi level. When such a state is present, an additional mechanism due t o the LzSz lYartof the spin-orbit interaction must be included in the analysis.

1. Introduction
The spontaneous anisotropy of the resistivity of ferromagnetic metals has been known for well over a century, but although it has been generally recognized that this is a spin-orbit effect, various types of mechanism have been proposed to explain the relation between the spin-orbit coupling and the conductivity. Recently, interest in the effect has been renewed because of the practical applications (bubble memory read-outs, tape readers). We will discuss the spontaneous resistivity anisotropy in Ni ba~ed alloys. In a ferromagnetic metal, and in particular in Ni, spin t and spin ~, electrons (i.e. spin parallel and antiparallel to the magnetization) carry current in parallel and one can define at T = 0 specific residual resistivities Pot and Po ~- The ratio = P0~/p0t for a given impurity in a given host can be estimated by measurements on the temperature dependence of alloy resistivities or by ternary alloy residual resistivity measurements [ 1 - 5 ]. In the present work we examine in detail the relation between the resistivity anisotropy and the two band character of the conduction. We have c0rried out experiments on a wider range of binary Ni based alloys than in previous work, together with certain ternary alloy systems. We have paid particular attention to the influence of texture and of parasitic impurities on the measured anisotropy. We find that for each impurity * Laboratoire associt~au CNRS. 23

there is a characteristic concentration independent value of the anisotropy; for low residual resistivity impurities the anisotropy does not saturate at a concentration independent value until ~the concentration is such that the residual resistivity is greater than about 2/a~2cm. We revise upwards previous estimates of the characteristic values of the anisotropy for NiCo and NiFe. For certain NiCo samples the anisotropies we have measured are the largest ever reported on any system. We find that for impurities with values of a greater than 1 the anisotropy is proportional to (a-I) confirming that a Smit [6] spin mixing type of mechanism is the dominant one in these alloys [7]. However, in alloys where a is less than 1, although the anisotropy is always small, there are deviations from the (a-l) rule. To explain these deviations we propose an additional intra-spin-band Lz Sz spin-orbit mechanism which plays a role in the presence of a virtual state at the spin t Fermi level. Results on the anisotropy of each spin band separately obtained from an analysis of ternary alloy data [8] support this approach.

2. Definition of tile spontaneous magnetoresistance

In addition to the well-known ordinary magnetoresistance effect observed in all metals, magnetic metals have an additional term depending on the relative orientation of the magnetization and the current. For a fully magnetized ferromagnetic polycrystal the resistivity is of the form
p(B, O) = -rio + ( cs20 - ~) Ap + So(B, 0 ) ,

(l)

2~

where 0 is the angle between the current direction and tile macroscopic magnetization of the sample. The last term represents the ordinary Lorentz force magnetoresistance which depends on the magnetic induction 8; the second term is the spontaneous magnetoresistance ~ . To separate the two terms experimentally, the sample resistance is measured as a function of applied ! . Then, the curves for p0(B) and field for 0 = 0 and ~ p~(B) above technical saturation are extrapolated back to B - 0. eliminating the Lorentz term, fig. 1. We define the spontaneous magnegoresistance parameter Ap/,~ by
ap = p,,(s o) - pi(B --, o) (2)

3. Experimental details
We prepared Ni based samples containing different elements at various concentrations. These alloys were prepared by induction melting in alumina crucibles or for the less resistive ones (N/Co, NiFe and NiCu) by induction melting on a cold copper hearth with weak levitation of the melt. The atmosphere was argon or argon/hydrogen. The alloys were usually cold rolled into the form of wires or long plates, and were generally annealed at 900C under vacuum. Sample resistances were measured at 4.2 K in applied fields up to 30 kG (in some cases 70 kG) for parallel and perpendicular orientations of the sample current relative to the applied field. As defined in eq. (2), the anisotropy AO/~ does not depend on the sample form factor. There are, however, possibilities of error due to texture or composition problems.

~PlI(B -* O) + }p(B -+ O)

in alloys, the extrapolation to B = 0 generally presents no great problem as the spontaneous effecl~ is much greater than the ordinary effect except for dilute samples at low temperatures. Only in this particular case is it necessary to know how 6p(B, 0) varies with B and 0. The ordinary magnetoresistance of Ni alloys has been studied by Schwerer and Silcox [9] who showed that the variations of pll(8) and pl(B) follow a Kohler's law which depends strongly on the type of impurity present. For most of the alloys with which we will be con. cerned, the extrapolations are negligible. Exceptions are alloys, particularly NiCo, where residual resistances are low even at quite high impurity concentrations and where the ordinary magnetoresistance is strong.

3.1. Problem of textures

The dispersion of the experimental data on Ap/-~ for NiCo alloys found in the literature [6,8,10-13 and our own results] drew our attention to the possibility of textures in samples which we re supposed to be random polycrystalline. From data on NiFe single crystals [14,15] it can be shown that samples with certain textures could have apparent Ap/~ values considerably different (by a factor of up to 2) from the value characteristic of a randomly oriented polycrystalline sample of the same alloy. Some Ni based alloys, particularly NiFe and NiCo, are well known for having distinct textures which vary with casting, cold work and annealing procedures. We found a considerable spread of anisotropy values for different samples all coming from a single NiCo alloy but which had undergone different treatments. We therefore X.ray analysed our samples after etching and checking grain size. All our results refer to samples with no pronounced texture, and which we hope are close to random polycrystalline samples. For some samples we produced directly cast rods by sucking the molten alloy into an Humina tube (see, for example, [16]. This process corresponds to a rapid quench, and the grains grow inward radially in a dendritic form. X-rays show generally randomly oriented crystrJlites. Agreement between these samples and

/ P,CB,--0)

Y
r::~._---.O B.I.=OH=O

O,(BL=O)

l.ig. 1. Resistivity of a ferromagnetic sample as a function of applied field for Hlli and H I i geometries (schematic).With 8 = H + 4:rM and different demagnetizing factors for Hlland ttL, the spontaneous anisotropy of resistivity Ap is defined as plI(BII = O) - pl(Bj. = 0), where these values are obtained by extrapolation. Note that Po(H = O) depends on the magnetic history of the sample and is generally different f r o m ~ = 1 [pll(8 0) + 2 p I ( B I = 0)].

O. Jaoul et al. / Spontaneous resistivity anisotropy in Ni alloys

Table 1 The residual resist.city per percent, the values of a = po$/PO 1' , the saturation resistivity artisotropy a p / ~ and the estimzted anisotropies in each spin band for Ni based binary alloys Impurity

25

p(O)l%
/~2cm/% at.

AplK (%)

( A p / p ) t (~.)

(ZXp/p), (%)

Impurities with no VBS Mn Fe Co Pd Cu Zn A!

Si Sn

0.79* 0.37" 0.16" 0.14 * 0.77 * 1.01 a 3.05 a

3.6 a 3.5 a

11 to 17 c 15 to 23 c 23 to 35 c ~3 * 8 to 1 0 " ..-8 ~6
~4 ~4

9.5 0.5 * 19.5 1 * 28 3"

10.5

0.5

-1.20.4

20 30

2* 3*

-1.00.3" -1.2~0.3"

2.0 0.5 a 7.8 0.5 * 6.5 a 4.8 a

2.8 a 3.5 a

8.0

0.3"

-2.31.5"

0.5

-1.50.5

3.85 +- 0.3 8.0 0.5

- 1 . 2 0.6 - 2 . 5 1.3

Au Impurities with VBS V Cr Nb Mo Ru Rh W Re Os Ir Pt

0.62 *

6 to 8 *

7.9 0.7 *

5.0 * 4.8 * 5.3 b 6.0 b 5.26 b 1.81 b 4.9 b 6.2 b 5.9 b 3.9 b 0.8 b

0.55 to 0.65 c 9.35 to 0.5 c 0.5 b 0.35 * 0.14 * 0.3 ~ 0.50 *

0.18 *

0.6 * -0.28 * +0.15 * + 0.05 * -0.82 * + 0.05 * + 0.8 a -0.45 * +0.25 * -1.52 * + 0.4 *

+4.4 2"

-2.5

1 2"

+1.2 6"

-0.7

+-0.2"

0.5 0.5 +3.7 1

-1.0 -1.5

9.3 0.4

+4 +9 -4 +4

2 3" 2" 1.5

--1.5

0.5

0.12 * 0.17 * 0.213 *

- 0 . 7 5 +-0.3" -1.0 -0.3 0.3" 0.3

Note: (a) Ref. [ 11 ], (b) ref. [30], (c) ref. [5 ], and those m a r k e d * are from the present w o r k and ref. [ 15 ]. In the last two colunms, the vaiues n o t marked with * were o b t a i n e d from a reanalysis o f the results of ref. [8] in orde~ to show the influence of the choice o f the present a values. It should be noted that the uncertainties involved are m u c h greater lhan in the preceedtng columns.

26

O. .laoul et al. / Spontaneous resistivity anisotropy in At"alloys

conventionally prepared samples was good. The only truly satisfactory way to overcome the texture problem would be to make measurements on sets of monocrystals and take tile correct polycrystalline a,,emge from these values. However, this would be an extremely tedious procedure.
3. _." Parasitic impurities

We used 5 N or 6 N metals and tile principal pollution comes from the melting in the alumina crucibles and the annealing in quartz tubes. Principal residual parasitic impurities are AI and Si. A sample of pure Ni prepared in the same way as the alloys gave a residual resistivity ratio (RRR) "-- 800.

4. Experimental results Our experimental results for binary samples at 4.2 K together with some results by other authors at low temperature are given in table I. For each alloy series N i X there is an anisotropy value (Ap/~-) which is characteristic of the impurity X. For most impurities this anisotropy is easy to determine, as we find little concentratio~; dependence at concentrations of the order 1% and gc~od agreement with values reported by other

authors where these exist. However, the case of impurities which have both high anisotropies and low specific resistivities are more complicated; we show the details of the concentration dependence of the an. isotropy for NiCo, NiFe and NiCuin figs. 2 and 3. For NiCo our results are in reasonable agreement with those of Dorleijn and Miedema [8] over the concentration range up to 5% which they investigated, but are considerably above those of Smit [6] and McGuire [13] (except that McGuire also finds quite a high anisotropy for a NiCo 30% alloy). For NiFe and NiCu there is much better agreement between tbe results from different groups. The disagreement for NiCo can partially be ascribed to the influence of uncontrolled texture, but the effect of parasitic impurities in the samples giving low values is probably also important. As the residual resistivity of NiCo is particularly low, these alloys are extremely sensitive to the presence of uncontrolled impurities such as W introduced during arc melting. it can be seen from fig. 3 that for each of these three alloy series there is a continuous variation of the anisotropy with concentration until a plateau is reached. We have already pointed out [17] that the condition for saturation appears to be that the residual resistivity of the alloy must be greater than about
ao A ,l si% ....
G

25
I, 1,

Ni Co

,o.
20
a
oo, o

i t

to
15

lo

-2

5[,"
II

"

5i/

5t/

NCu

2 4
~ %,, o~

6 "

~' 2 4 ~

2 4

8 10

20

40 60 80 Impur i ty concentrotion,ot %

Fi~. 2. Concentration dependence of the resistivity anisotropy for three Ni based series showing slrong effects at T = 4.2 K. A NiCo, =~NiFe, NiCu. Crosses and full symbols: present results. Fmpty symbols: 3mit [6].

0 " Conc---c-~ ca t ion, % Fig. 3. Concentration dependence of the resistivity anisotropy for NiCo, NiFe and N;Cu in the low concentration region. NiCo: A present results, A Dorleijn and Miedema [8J, VMcGuire [13], n Smit (6). Nil:e: present results, o Dorleijn and Miedema [81,@ Smit [61. N/Cu: x present results, +Stair [61; Dorleijn and Miedema [8 ], In each case, arrows indicate the concentration where P0 = 2 ufZcm.

O. Jaoul et ai. / Spontaneous resistivity anisotropy in Ni alloys

27

2 #12cm. The concentration corresponding to this criterion is indicated for each case in fig. 3. For Fe and Cu the anisotropy remains unchanged from this concentration up to about 25%, and for Co up to about 50%. The initial approach to the plateau value appears as an intrinsic effect rather than, for instance, a gradual change of character of the impurity with concentration, because for each of the three alloy series the anisotropy increases regularly and in the same fashion with concentration until the residual resistivity reaches about 2/a~cm. We have discussed this effect and associated concentration dependent changes in the deviations from Matthiessens rule, in the ordinary Hall effect and in the ordinary magnetoresistance [17]. For the various alloy series the plateau value of Ap/p persists until a drop is observed only at concentrations so high that interactions between impurities are certainly important. It seems that Ap[p is only sensitive to quite major changes in the alloy structure. Thus for instance for NiCu alloys the anisotropy begins to be affected by the change in electronic structure and the lowering of T~ only when the concentration increases above about 25% (cf. calculations by Brouers et al. [18]) and for NiFe alloys Ap/~ falls dramatically at the concentration corresponding to the Ni 3 Fe compound. In NiCo a similar drop occurs above 50% concentration. We should perhaps point out that the anisotropies we obtain for certain NiCo samples are the highest ever reported on any system up to now. This suggests po:~sible technological applications, but for these samples at room temperature the anisotropy has dropped to 6%, which is little more than the anisotropy for NiFe near the permalloy concentration.

apt? "1.

Ni Os Fe

o[
.1

0.'2

'

o14 ' o:6

'

Ni Ir Fe

-2

Fig. 4.The residual resistivity anisotropy of ternary Ni based alloys Ni I _x_yFexBywith B = It, Os as a function of the relative concentration t = x/x + y. The curves are fits using the technique described in the Appendix and correspond to the parameters for Fe, lr and Os given in table 1.

5. Ternary alloys We have also inade measurements on a number of ternary alloys, NiCuCr, NiCoV, NiFelr, NiFeOs (fig. 4). Residual resistance measurements on ternary alloys can be analysed to give the values of a = Po $/Po t for the impurities present [ 1-5]. Similarly, spontaneous anisotropy results on sets of ternary alloys can be used to obtain the anisotropies within each spin subband (Ap/p)t and (Ap/p)$ separately for each impurity. This idea has been exploited

by Dor!eijn and Miederr, a [8] who obtained estimates for a number of impurities in Ni. A!':!hough this work is interesting, we do not consider it definitive for three main reasons" (1) For a number of the samples measured in this work, tae residual resistivity is significantly higher than values obtained by ourselves or by other groups [2, 19]. This suggests inadvertent introduction of parasitic impurities into the alloys, which could ser. iously affect Ap/~. (2) ~,ome of their ternary alloys do not seem to be sufficiently concentrated (especially those containing Co) to avoid the low concentration effect described before. (3) The final set of t~ values [8] differs considerably from most of the values estimated from individual sets of ternary alloys, using the same samples [4]. This appears to be because a global computer treatment is not the ideal technique for analysing; the data. We have discussed the ternary alloy residual resistivity results [5], and we find a set of final "best 'values" for a different from those of ref. [8] but compatible with the experimental data of ref. (4) and in agreement with previous work [20]. The method we have used for determining (Ap/~)l'

28

O. .laotd et at. / Spontaneous resistivity anisotrop), in Ni alloys

and (Ap/p)$ values from ternary alloy ~ . ~ o / ~ data when the a values are known is discussed in the appendix. We have applied this analysis to our ternary alloy data on NiCoV, NiCuCr and NiFeir, NiFeOs alloys and to the data of ref. [8]. Values, with associated uncertainties, are given in table 1, although the rough qualitative conclusions are similar to those that can be drawn from the equivalent table in ref. [8], the individual paramete~ are sensitive to the choice of the a values. it should be noted that (Ap/p)~ is equal to --1% within the experimental incertainty for all the impurities in the table (with the possible exception of Pt~. On the other hand, for impurities with 0t greater than I (Ap/p)t varies from +30% to +4% and is closely proportional to the value of a, while for impurities with a less than I (Ap/p}? varies from +9% to - 4 % and seems unrelated to ct. (We do no~t agree with the statement in ref. [8] that the (Ap/p)t values are approximately the same for all impurities.) Explanations for this behaviour will be discussed in the next sections.

~cm

~IiFe

Impurl ly concentrQlion (<at.%)

10 20

3r

.......

,'o

5'0

Fig. 5. Residual resistivity as a function of concentration for NiCo and Nil:e.

6. Basis of the model for the resistivity anisotropy Quite generally, in a ferromagnetic metal such as Ni spin ? and spin $ electrons carry current in parallel. ~,~,'ecan define at T = 0 intra-spin residual resistivities Po ~ a:ld Pc, ~. For a given impurity in Ni the ratio a = p0,t/pot is estimated by measurements on the temperature dependence of binary alloy ~resistivities or by measurements on ternary alloy residual resistivities (see. e.g. [5]). In table 1, we list the values o f p o per atomic percent, of a values and of Ap/~ for different impurities in Nf. We will discuss the interpretation of these values in terms of the well-known s - d model.
6.1. The s - d model

atively high density of states at the Fermi energy. From measurements of the magnetic moment on and around the impurity site (see, for example, Low [21 ]) and using the picture developed by Friedel [22], Kanamori [23] and Campbell and Gomes [24,25], one concludes that: (1) For some transition impurities in Ni (Mn, Fe, Co, Cu, Pd, Au), the screening is done entirely by the d~ band so that there are no dt states at the Fermi level. For s - p impurities, the potential is attractive so again there are no dt states at the Fermi energy (2) For other impurities (Cr, Rh, Ru, Ir, Os, Re) a spin t virtual bound state (VBS) overlaps the Fermi energy, fig. 8. This VBS corresponds to a resonant d state with more or less strong s - d hybridization giving it an energy width A. Many experimental results on the resistivities [20], thermoelectric pow,~r [26], electronic specific heat [27], and Hall effect [15] of such alloys give information about this VBS. (3) Finally, for strongly repulsive imp~arities at the beginning of a tranmion series, there is f~drly strong screening with considerable s--d mixing for both directions of spin.

I., ,,, this-"'~-' , , , u ~ = t , the host meta~ . . . . . . is represented as having a tight binding d-band and a free-electron-like conduction band. For the ferromagnetic metals, the d-band is polarized but the s-band can be taken for present purposes as unpolarized. A tr~msition impurity is screened essentially by the d-electrons. Nickel is a strong ferromagnet. The d? electrons lie completely below the Fermi energy, while the d$ band has a rel-

7. Resistivity anisotropy mechanisms If we assume the spin-orbit effect is a weak perturbation on the electronic structure of the metal, then the lowest order mechanisms which can lead to a spontaneous resistivity anisotropy are second order

o. Jaoul et al. ] Spontaneous resistivity anisotropy in Ni alloys

in the s p i n - o r b i t interaction *. We will describe these lowest order mechanisms within the s - d model.

29

7.1. Spin mixing or Smit mechanism ( L - S +)

Using the s - d framework, the most important mechanism leading to spontaneous magnetoresistance has already been proposed and tested experimentally [6,7]. In the presence of spin-orbit coupling in the d-band, a certain a m o u n t of d t character is mixed into the d$ states at the Fermi energy through the influence of the L - S * operator. This permits s scattering into the d$ part of the mainly d$ Fermi surface. The d t - d $ mixing is not isotropic because the magnetization direction provides a privileged axi.s for the s p i n - o r b i t perturbation, so it provides a mechanism for the resistance anisotropy. The anisotropy may be seen as an anisotropic transfer of a certain amount of spin ,I, resistivity into the spin t band. On this model, at low temperature

.-L_

..........

10

20

30

ot

Fig. 6. The characteristic value of Ap/~at 4.2 K for various impurities in Ni as a function of ~:: pO/p~ (see text and table l). The straight line is &p/~ = 0.01 (~ - 1).

Ap/-fi = 3,(a - 1 ) ,

(3)

where a = Po $/Po t and 7 is a constant appreximately equal to (k/Hex) 2 and which can be estimated a priori as being about 10 -2. k is the s p i n - o r b i t average value in the spin $ band of nickel, and Hex is the exchange energy which splits the d t and d$ bands. We can compare the Ap/-~ characteristic of each NiX system with the et values, fig. 6. Eq. (3) provides a good fit to experiment with 3' ~ 0.01 (this value is slightly different from the one adopted by Campbell et al. [7] mainly because of the revised estimates of the characteristic Ap/-~ values for NiCo and NiFe). The spin t band for alloys such as NiCo or NiFe is almost purely of sp conduction character and so should be almost uninfluenced by the spin- o r b i t interaction, thus giving no resistivity anisotropy. The fact that in practice the largest anisotropies are observed for precisely thoo ~llc,y~ ,,,h~,-,- ,h,~,,~ sp *. . . . spin t "' . . . . . . . . are carrying almost all the current shows without any doubt that the dominant effect must be due to a Smit type of mechanism where the s p i n - o r b i t acts to mix spin t character into the spin $ d band. The good agree~lUtd 1.1 U I I ~

ment between the experimental results and eq. (3} confirms tha~t this mechanism dominater,, particularly for impurities having a > 1. However, if we look in detail at the results for impurities with low values of Ap/~6, fig. 7, there is an apparently random scatter of values of about - 19~ around t!'c 7(a -- 1) line. For these impurities this scatter is much greater than the experimental errors. It is ob-

0
/ M---~do ~ Rh . ~ ~.5

_l

Ru

* The relation between the order of the perturbation and the .symmetry of the physical effect was pointed out to us by P. Lenglart.

Fig. 7. An enlargement of the part of fig. 6 corresponding to impurities with low resistivity anisotropies. The line Ap/ff = 0.01 (a -- 1) (Smit mechanism) does not fit the resuits well for alloys with ot < 1.

30

O. daoui ei al. / Spontaneous resistivity anisotropy in Ni alloys

,dous that a is not the only relevant parameter which determines ..k0f~i. The details of the electronic structure of the impurity are important. In the next section, we will discuss a different mechanism in order to explain these deviations.

The 5d 1' resonant states are assumed to have ener. gies

b.~ t : E~+ ~X'rn ,

Z Z lntraband or L=S, m e c h a n i s m
So tar we have ignored the LzSz term in the s p i n orbit interaction. However, this term can also lead to an anisotropic resistivity by lifting the degeneracy of the d states for a given direction of spin. Because the scattering into each rl state taken separately is anisotropic, this lifting of degeneracy leads to anisotropic resistivity. Suppose there is a set of degenerate d 1' VBS near the Fermi level, fig. 8(a). When we introduce spin-orbit, the different d states will split, fig. 8(b), (c). For the case of fig. 8(c), there will be relatively more I0) states than the others at the Fermi level. For fig. 8(b), there will be relatively more 12) states. Now, for a spherical scattering potential, a free electron with k vector parallel to the magnetization can only be scattered into Im= 0) state whereas an electron with k vector perpendicular to the magnetization is scattered into a state { v - , - v - ) ( ~ - ~ + I ....:'.}) + ~ I0). The situation of fig. 8(c) will favour the scattering of the electron parallel to the magnetization giving p, > p, whereas the situation of fig. 8(b) will lead to p~ < p~.. We can calculate the size of the effect to be expected from this mechanism.

where fi~t is the energy of the d impurity level submitted to a local spin-orbit coupling ~,', (--2 < m < +2). Each of these states is then mixed with an l = 2 part of the plane wave states, leading to a phase shift 11~ nt given by tan r ~ n t = A/(E~ t - E F ) , (6)

where A is the virtual bound state width and E F the Fermi energy. Then, the scattering amplitude developed in spherical harmonics f(0, O)
o~ +!

f(o, o )

4,r z~ ~ (ein? _ l ) =o,,,=-z

(7)

x Y;"(OkOk) Y (Ok, %)

may be directly calculated from eqs. (5) and (6) and put in the expression of the diagonal part of the scattering cross section tensor

~Ouu= ~ 2 I(Ok--Ok')Ul 2 d ~ g d ~ k ' , I(o k - Ok,)Ul 2 d~2kd~ k,

(8)

n(E);

d',

EF

n (oE)~

EF

n(E)l

EF

l"X.
E~ E
6

where k and k' denote the incident and scattered wave vectors, respectively, in directions (0g0k), (0g, 0g') with respect to the magnetization direction, u is a unit vector in the direction of the current. Rapidly the calculation of Ouu shows that the five d phase shifts r/~ n are weighted very differently. The symmetry breakdown is sufficient to avoid calculation on other partial waves than l = 2 and also an averaging of the cross sections over all the k' scattered wave vectors. Then, within this simplification - otherwise the restilt does not differ greatly - the two cross sections can be written

a)

n(E )~

b)

c)

fig. 811( a ) Schematic picture of a virtual bound state near the spin r Fermi surface. (b), (c) local s p i n - o r b i t coupling on the impuritty site lifts the ,degeneracy of the different m z states making up the VBS. &p/~ will depend on the position of E O with respect to the Fermi energy El...

Oztz cc I/']2 cos 2 0 sin 0 dO dO,

r o: Ijq2 sin 2 0 cos 2 0 dO d 0 , Oxx

(9)

O. Jaoul et al. / Spontaneous resistivity anisotropy in/~i alloys

where z and x denote directions parallel and perpendicular to the magnetization. The anisotropy of the cross section tensor comes from the fact that the scattering amplitude f(O, ~) is anisotropic, like the I(kldm)l 2 integral as we showed in the simple example above. Finally, this mechanism induces an intra-spin transfer of resistivities from parallel (11 or zz) to perpendicular (1 or xx) directions of the current with respect to the magnetization. Then

31

K=.3

-'

~/2

p~ = (1 + 2/3) P~o+ 27 p~,

Fig. 9. The function Y(r/O~ ' , K) representing the calculated

LzSz effect anisotropy for the spin ~ resonant diffusion, l'or

p~=(l-2"y)p~,

PI=(I-3')P~,

(10)

a given impurity not can be evaluated from the resistivity oOK = MA, will be equal to about 0.3, 0.5 and I for first, second and third series transition impurities in Ni. The approximation (~,'/A) 2 < < 1 is not valid for second and third series impurities. To obtain numerical estimates, we take A = O. 15 eV, 0.25 eV, 0.5 eV for VBS widths of first, second and third series impurities, respectively (values estimated from specific heat [27] and thermoelectric power [26]*). For the local s p i n - o r b i t coupling ;~', we take the atomic values 4 X 10 -2, 0.12 and 0.5 eV, respectively. for the three series of elements. LJsing these parameters we estimate LzSz anisotropies as shown in fig. 9, where we plot the function Y(r~t, X'/A) as a function of r/~ for various values of X'/A. The simple explanation given initially is still 'valid qualitatively O > P: for phase shifts near g rr (i.e. when the VBS is centred near the Fermi level) and Oil < P t for nearly full or nearly empty VBS. An exactly equivalent term should exist in the spin ~, band, but can be expected to be much weaker, as in the factor (X'/,~):' the VBS widtl'~ A would be replaced by an energy of the order of the d band width. Deviations from the Smit term can be expected to be small for the spin ,I, band. We can compare the predictions of this modified model with the experiments, sections 4 and 5 and table 1. First, for no impurity does the value of (Ao/p)~ deviate greatly from - 1%, that is to say (Ap/p)$ ~ 7 in agreement with eq. (14). For spin l, firstly (Ap/f,)t 7a for all impurities where there is no VBS in the spin I' band (Mn, Fe, Co, Cu, Au, Sn, AI, Pd). This is * In fact, the VBS width should increase as the Z difference between host and impurity increases.

where p~ and pro are resistivities without spin orbit and 7 is the Smit mechanism parameter. We find

~= ~(rlt2,K) = A r(rl~,K)/sin2 rlt ,

with

(11)

Y(,fi, K) - 2

,rio

+ si.2
(12)

_ 2(sin:~ r/t2 + sin 2 ~ - 2 ) and

pro s si, ,rio,

(13)

where y ( ~ , K) is a function of the phase shift ~ and is related to the position in energy of the VBS relatively to the Fermi level, and depends also on the local spinorbit coupling ~' and the width A. A is connected witil the s - d hybridization around the impurity potential. More precisely, Y depends on the ratio K = k'/A. Finally, the resistivity anisotropy may be rewritten
as

(Ap/p) t ='y(x + 3/3;

or

(Ap/p)$ = - , y

(14)

A p / p = ' r ( a - 1)+ 3[a/(a + 1)]/3.

When X' < < A (first series transition impurities) /3 = - ~ 7 ( ~ , ' / A ) 2 (1 -- 4 cosZr/t:)sin 2 r~ .

(t5)

(16)

Notice that this involves a second power of the spinorbit interaction, in agreement with the general rule.

32

O. .laoui et ai. / Spontanc,gus rcsistirit.v anisotropy in Ni alloys

stron~ support for ti~e dominant influence of the Smit mech:~,nism m these cases. The rule for the total anisotropy Aptp = 7(a - I ) is well obeyed. On the other hand, for inlpurities with VBS in the spin ? band, an extra/3 term must b,e invoked. This term can be of either sign, and is roughly of the order of magnit ude estimated on the Lz Sz mechanism above. I It~wever, it is difficult to recognize in the experimental results the detailed variation of the fl term as a function of r/~ predicted by this model and shown in fig. t). The oscillating deviation from the Smit value shown by the third series transition impurities, fig. 10, does seem to show roughly this behaviour but, as we take a very simplified description of the electronic s~ructure of the VBS, we cannot really expect precise agreement with the model. Nevertheless, for impurities such as It, Os, Re, or Ru, the fit between experimenltal and calculated values of Ap/~ (Smit +/3 term) seems to be quite good based on the r/~zvaltues taken from table 1. Notice that this type of impurity does not a~'feet the spin ,L band by extra spin 4, screening charges. The main point is that the deviation from the Smit

value is due mainly to an effect in the spin t VBS, and is strongest for third series transition impurities where the local spin-orbit coupling is strongest. This indicates that the origin of the deviation from the Smit value is indeed the LzSz effect in the VBS. However, the prediction for W is bad, so we must be cautious about using the detailed quantitative predictions of this simple model. it is interesting to remark that the LzSz term can be regarded as introducing a local electronic quadrupole moment on the impurity site, which gives the impurity an anisotropic cross section (cf. Friederich and Fert [28] who consider the case of rare earths). This electronic quadrupole should be related to the nuclear quadrupole splitting observed at third series transition impurity sites in ferromagnetic hosts ([29] and references therein).

8. Conclusion We have refined the model presented in an earlier article [7] to explain the spontaneous resistivity anisotropy of ferromagnetic metals, and in which we showed that the Smit spin mixing mechanism explained the anisotropy of a number of Ni based alloys. We can summarize the conclusions we can draw from the analysis given here. (1) For impurities for which there are no d states at the spin 1' Fermi surface (non-transition impurities, Co, Fe, Mn, Pd), the Smit mechanism alone provides a good description of the anisotropy with A p ~ = 7(~ - 1), where 3' is a spin-orbit parameter which we find equal to about 0.010. Alternatively, if separate values of (Ap/p)t and (Ap/p)~ have been obtained from an analysis of ternary alloy data, then for these impurities
( A p / p ) t ~ 7a , (Ap/p)~ " . - 7 ,

~L

!
: : ?
,

'I
0 L

.,

L
~,,,
i

Au t i,.:. 10. I xperimental resistivity anisotropies lk)r third series impurities in Ni points. Values calculated from O.01 (~ - 1): dashed line. Values calculated including I.::S z mechanism: full line. ~O values used in the calculation are estimated from resistivity values o~). Similar values would bc obtained from mag.elic mom,:nt data, except for the case of W {Durand [31)]).

so that Ap~ = --Apt. (2) For other transition impurities where there is a VBS at the spin 1' Fermi surface, it is necessary to introduce an additional anisotropy in the spin 1' band resistivity, so that we write (Ap/p)t = 7or + 3/3. llere, as determined experimentally/3 varies from impurity to impurity and can be either sign. We have suggested that the 13term can be identified with an LzSz spin-orbit mechanism acting within the

O. Jaoul et ai. / Spontancous resistivity anisotropy in Ni alloys

33

spin t VBS. We have developed a simple model which gives the correct order of magnitude of the effect, together with an indication of how the effect can be expected to vary from impurity to impurity across a transition series. Judging from the experimental results, there appears to be no need to introduce an analogous spin 4, term, so that for these impurities also (Ap/p)~, ~ -"7. Froth symmetry arguments, if the resistivity anisotropy is due to a weak spi~--orbit perturbation of the structure of the metal, the leading terms must be second-order in s p i n orbit, that is to say of the type (M,+S_) 2 or (M, r Sz) 2. The former is the Smit mechanism term, and the latter the additional anisotropy in a spin 1' VBS. Even though we have used a very simple model of the electronic structure of ~he alloys, the identification of the type of mechanism leading to the anisotropy in various cases seems clear, A further analysis on single crystals should give more detailed information about these mechanisms in relation to a realistic band structure scheme including spin orbit.

~I ~9/~ ('/.)

8L
6;
t-

oE
0

;t

..,..._-..-......--.

112 0.4

0.6

0.8

,,t

__

I"ig. A I. The resistivity anisotropy of Nit_.,: vMnxCr v alloys at 4.2 K as a function of the relative conccnltation t = x x + r The curve is based on data by Dorleijn and \liedcma 181 and Jaoul [ 151.

can use the four experimental parameters

(AP/o)A'

(AP/p)B"

~W]:--.O

-d-t~ p l , - t

(see fig. AI). It can be shown by a little algebra that we have the four simultaneous equations: (i) u A + ( l / a A ) d A = (o~A + i/0ta) (Ap/p) A .

Acknowledgements (ii) uu + (I/oq~) dB = (o~u + l/ate) We would like to thank Professor Perio and Drs. Lauriat and Dixmier for kindly guiding us in the texture problem.
(AP/P)B ,

(iii) UA [~3(q~ + 1 )l + ul~ [aA + 1 - au(aj3 + 1 )2 ] + dA(a B + I ) ~A dB(CtA(20~B+ 1 ) P~ d Ap)

dt ,-o

Appendix Suppose we have a set of ternary Ni based alloys Nit_x. yAxBy, where a A = (Oo~/Pot)~ and % = { p o U P o t ) , are known. We will assume that all the alloys are sufficiently concentrated for the effects discussed in section 4 to be unimportant. Tile resistivity anisotropies on these alloys can be plotted against the relative concentrations of B to A, expressed by t,,,~ l. ^ pa ...... '- = C A / (Ca + Cu ) which varies from 0 to I as x/y varies from 0 to oo. We define
I dt I I I~., I ~., I t

=(aa+l)3

( ~A

(iv) UA [0~A(a A + [)2 _(Ct B +

1)1- UBIe2(C~A + 1)!

- d B ( O t B ( e A + 1))

- d A [ 0 t 2 - - ( 2 0 t A + l)OtB]

u
-

l&tA

[,,~,

'

''~aa +1 pO dt plt__,

.A=(aolp)
uB = (

,
xp/o)P ,

dA = (Ap/p)'~ ~'

dn = (AP/P)~

To determine these four parameters separately, we

where O~,, O are the specific resistivities per percent impurity for impurities A, B. These four equations can be solved immediately for the four unknowns, it is instructive to put in the numerical factors for the case shown in ig. A l, where A is Mn, B is Cr. Let us take as given for instance aMn = 11, act = 0.35. This

34

O. .laoul ctal, / Spontatu'ous resistivity anisotropy in ,Vi alko,s

is a typical case wltere eA ~' 1, oq~ < I. We have (i) u.x + O.Oq 'IA = !.! (Ap/p) A = 10.5 ,

d A = OtA/(C~A -- 0tB) 3 [{a A + a B ) K0 - 20lBKI ] ,

d B = 0tB/(OtA -- OrB)3 ( 2 a A K o - (C~A +ORB) K I ) ,

(ii) tt B + '.85 d B = 3.9 (Ap/p) u . . . . 0 . 8 , where UA and u u can then be determined from eqs. (i) and (ii). Application of either o f these methods shows that the accuracy of the final estimates requires points very close to the t = i side o f the fig. AI.

{iii~ { 10)UA + t ! I .35)UII + ( ! 4.9)d A -- ( 1 8 . 6 ) d (.._6116.8t d Ap --*o (iv ~, 15t)0ua 1 4 5 0 u B -li3d A - - 4 d B

References
[ 1 ] I.A. Campbell, A. l:ert and A.R. Pomeroy, Phil. Mag. 15 (1967) 977. 121 P. Leonard, M.C. Cadeville, J. Durand and I:. Gautier, J. Phys. Chem. Solids 30 (1969) 2169. 13 I.'.C. Schwerer and J. Conroy, J. Phys. !"1 (1971) 877. [4 J.I.'.W. Dorleijn and A.R. Miedema, J. Phys. i"5 { 1975) 487. [5 A.l.'ert and i.A. Campbell, J. I'hys. 1'6 (1976) 849. [61 J. Smit, Physica 16 (1951) 612. [7 i.A. Campbell, A. I:ert and O. Jaoul, J. Phys. C3 (Met. Phys. Suppl.) 119.70) $95. [8 J.I .W. Dorleijn and A.R. Micdema, J. I'hys. 15 (1975) 1543. 19 I".C. Schwcrer and .I. Silcox, l'hys. Rcv. BI (1970) 2391. 101 J.i.. Snoek, Nature 163 (1949) 411. ! !1 il.C. Van Elst, I'hysica 25 (1959) 708. 121 Y. Shirakawa, Sci. Rep. Tohoku Univ. 27 (1939) 485. 131 I".R. Mc (;uire, All' Conf. Proc. 24 (1975) 435. 141 L. Berge~ and S.A. i:riedberg, Pl~ys. Rev. 165 (1968) 670. I151 O. Jaoul, Thesis, Orsay (1974). 1161 P.L. Maitrepicrre, J. Appl. l'hys. 40 (1969) 4826. ! 17] O. Jaoul and I.A. Campbell, J. Phys. 1'5 (1975) L 69. I 18 ] !:. 13rouers, A.V. VeJyaver and M. (;iorgino, Phys. Rcv. B 7 (1973) 380. I i 91 T. I.arrell and D. (;reig, J. Phys. C 1 (1968) 1359. 1201 A. I:ert and I.A. Campbell, Phys. Rcv. Lctt. 21 (1968)

= -67s-~'-ai - 7 -

---!

It can be seen that solving equations (i), (iv), (ii) and tiii) successively gives essentially the parameters UA, u B, d B and ,t:x in that order. The errors arise mainly from zhe undertainties in the estimates o f the limiting slopes. Itere we find u A = 10.5" UB = !.2" d A = -1.6; d B = -0.7.

An alternative but equivalent method which has the advantage of t,sing all the measured points is the following. Define k = P A t /(P A t + p tB) . do that o~ = '~'0:A + ( 1 -- Me u. and X goes from 0 to 1 as t goes from 0 to 1. Then
-..&p _

~+['~:A

+(l -X)UB+

XaAd A + (1 -- ;k) aBd B

0:2

This can be rewritten e:: a + 1 Ap

p

x ( 1 -- ~ ) - - -

1109.
11--X)aB + 1(~ 1211 (;.(;.I'L Low, J. Appl. Phys. 36 (1965) 1174. [221 J. l"riedei, Nuovo CmL 7, Suppl. 2 (1958) 287. 1231 J. Kanamori, J. Appl. Pl',ys. 36 (1965) 929. . . . . . '~. t t t t l t , u ~ a t l i_llltl t~t.l'~. ( J t ) l l i C S , P r o c . Pilys. Soc. 9i (1967) 319. [251 A.A. (;omcs and 1. ~,. Campbell, J. I'hys. ('3 (1968) 1312. 1261 M.C. Cadeville, i:. (;autier, C. Robert and J. Roussel, Solid State Comnmn. 7 (1969) 1701. 1271 R. Caudron, R. Caplain, J.J. Meunier and P. Costa, Phys. Rev. 68 (1973) 5247. 1281 A. I:riederich and A. l.'ert, Phys. Rev. Lctt. 3"1 (1974) 1214. [:]91 G.A. (;ehring, Phys. Scr. I i (1975). 1:301 J. Durand, Thesis, Strasbourg (1973).

aA + I ( ~ Q

= CtB{-' -,~)

2}, CtB

(1

X)(Ct2/~A)dA
~k(O~2/O~B)dB

+aB(2

h)

2(1

~)0:A

T!~,~ expcdmental!y determined function on the lefthand side is linearly dependent on X, with intercepts K o w h e n k = O, Kl when ?~ = !. F ' r o m these intercepts