# Oscillatory Exchange Coupling across Cr(1-x)Vx Alloy spacers

## Abstract

We have identified the pieces of the Fermi surface responsible for the long period oscillations of magnetic coupling across Cr and Cr<sub>(1-x)</sub>V<sub>x</sub> alloy spacers in metallic multilayers. Analysing experiments and results of KKR-CPA calculations we find that the periods are determined by the extremal wave vectors of the hole pockets centered on the N-point in the Brillouin zone.

The discovery that the magnetic coupling between two Fe layers separated by a Chromium layer, of thickness $`L`$(=1,100 Å), oscillates from ferromagnetic to anti-ferromagnetic as function of $`L`$ has lead to a veritable avalanche of observations of the same effect in similar metallic multi-layer systems. The interest in this surprising phenomenon derives from two sources. The first is its relation to the technologically important GMR effect. The second is the wealth of evidence which links the periods of the oscillations, $`P_\nu `$, to the Fermi surfaces of the bulk spacers. In this letter we shall be concern with the second aspect of the problem.

Whilst there are a variety of theoretical approaches for describing the above oscillatory magnetic coupling, each leads to the conclusion that one is dealing with a variant of the well known RKKY interaction between two impurity spins where the two point defects (spins) are replaced by two planar defects (the magnetic layers). Moreover, they all predict that the periods of oscillations, $`P_\nu `$, are determined by the extremal spanning wave-vectors, perpendicular to the layers, of the Fermi Surfaces of the bulk spacer metals. Reassuringly, there are now many cases where the calculated callipers vectors of the appropriate Fermi surfaces are in good quantitative agreement with measurements of the corresponding periods. Nevertheless, there is no consensus as to which piece of the Chromium Fermi surface is responsible for the long (18 Å) period of oscillation in the original, and since then much studied, experiments on the Fe/Cr/Fe system . In what follows we shall present conclusive evidence that these oscillations are due to the hole pocket centered on the N-point in the bcc Brillouin zone of bulk paramagnetic Cr.

Our arguments will be based on KKR-CPA calculations of the Fermi surfaces of Cr<sub>(1-x)</sub>V<sub>x</sub> alloys and a detailed, theoretical and experimental, investigation of the way the Fermi surface evolves as Vanadium is added to Cr. In short, we show that of all the possible candidate extremal vectors only these spanning the N hole-pockets change with concentration in a manner consistent with the experiments of Parkin et al.

A second, equally important point we wish to make, concerns the generic problem of the Fermi surfaces in random alloys of transition metals. As has been emphasised repeatedly, these fundamental features of the metallic state vary rapidly with changes in concentration and undergo interesting electronic topological transformations. Using the Cr-V system as an example, the first which features a non trivial topology, we shall demonstrate that measurements of the oscillatory exchange coupling across an alloy can be used as quantitative probe of subtle features of the Fermi surface. In fact, we suggest that they may provide comparable information to that extracted from results of Angular Correlation of (positron) Annihilation Radiation (ACAR) experiments.

To be specific, let us recall the general theoretical result that the exchange coupling between magnetic layers, across a pure metal spacer, is given by

$$E=\frac{1}{L^2}\underset{\nu }{}A_\nu \mathrm{cos}(\frac{2\pi }{P_\nu }L+\varphi _\nu )$$
(1)   
where $`A_\nu `$ is the amplitude, $`\varphi _\nu `$ the phase and $`P_\nu `$ is the period of the $`\nu `$-th oscillatory contribution. As was shown in Ref.  and is confirmed by our KKR-CPA calculations, the states near the Fermi Energy in the Cr<sub>(1-x)</sub>V<sub>x</sub> alloy case have sufficiently long lifetimes, as described by the Bloch Spectral Function (BSF) $`A(𝐤,E)`$, that the above formula can be used for these random alloys as well as for pure metals. Evidently, this means that spanning vectors are well defined by the sharp peaks in $`A(𝐤,E)`$. Taking this simplifying circumstance for granted we have carried out standard, self-consistent KKR-CPA calculations for a number of concentrations $`x`$ and determined both the Fermi surfaces and their extremal spanning vectors as described in Ref. . All the theoretical results which feature in the foregoing discussion will refer to these calculations.

In fig. 1 we display a three dimensional, schematic picture of the Fermi surface of Chromium. Clearly, for such a complex Fermi surface there are many extremal spanning vectors for each direction of the layer growth. Indeed, Stiles find no less than 6 candidates for explaining the long (18Å) period observed on (110) Fe/Cr/Fe multilayers and the controversy as to which of these, if any, is relevant continues unabated. Of course, a parameter free, reliable calculation of the amplitudes and the phases of the oscillatory exchange coupling could differentiate among these candidates. However, such calculations, at the moment, are still very difficult. Model amplitude calculations have been done for Fe/Cr systems either using the reflection probabilities for Fe/Cr interface or employing a Tight Binding model with spin orbit interaction. Whilst they point towards the conclusion that the long oscillation period for pure Cr spacers originates from the N-centered hole pockets, they are not wholly convincing since the size of the periods calculated agrees with the experiments only roughly. In this letter we wish to advocate a much more effective procedure: Namely, we determine the periods $`P_\nu `$ as a function of the Vanadium concentration $`x`$ by the KKR-CPA calculations mentioned above and compare them with these deduced from measurements of the oscillatory coupling. As will be seen presently, only a small set of interrelated periods show the observed dependence on $`x`$.

In fig. 2a we show cuts across the Fermi surfaces of pure Cr and the Cr<sub>0.85</sub>V<sub>0.15</sub> alloy parallel to the growth direction, (110), of the multi-layer system. Evidently, the ‘hole like’ pieces of the Fermi surface increase and the ‘electron-like’ ones decrease as $`x`$ changes from $`0`$ to $`0.15`$. Consequently, some of the spanning vectors, identified by arrows, increase or decrease with $`x`$ depending on whether they span electron or hole like pieces of the Fermi surface. The behaviour of the corresponding periods $`P_\nu `$ with increasing V concentration is depicted in fig. 2b. Evidently, only the periods related to the N hole pockets decrease as in the experiments. Thus we conclude, in agreement with the amplitude model calculations of Stiles and Tsetseris et al, that it is these N pockets that are responsible for the observed long period.

To generate further evidence in support of the above conclusions all the different N-related spanning vectors, which can be probed by measurements on samples with (110), (100) and (211) growth directions, have been studied. These investigations are summarized in fig. 3. The Fermi surface cross sections in figs. 3a and 3b are well known and correspond to paramagnetic Cr. Evidently N-pocket is not spherical for pure Cr. According to our KKR-CPA calculations as V is added this pocket shrinks without a change in shape or orientation. As a reflection of this fact, the concentration dependences of the N-pocket related extremal wave vectors N<sub>1</sub>, N<sub>2</sub> etc, shown in fig. 3c, are very similar.

Clearly, having eliminated the electron pieces of the Fermi surface, like the ‘lens’ or the ‘knob’ as possible contenders for the role of causing the long period oscillation the new issue becomes: the shape and orientation of the N hole pocket. This is important since agreement between theory and experiments should establish the measurement of the oscillatory coupling as novel and powerful probe of the Fermi surface. However such agreement will require further refinement of the experiments. A hopeful sign in this direction is that although Fullerton et al find the oscillations to have the same periods, and even the same amplitude and phase for all three of the growth directions (100), (110) and (211), Tomaz at al reports small differences. Our predictions for the corresponding periods are N<sub>1</sub>, N<sub>5</sub> and N<sub>9</sub> shown in fig. 3c. Clearly, whilst the differences are small, and hence the periods can be said to be roughly the same, in a more discerning experiment, they should be observable.

In conclusion, our calculations on the evolution of the Fermi surface of Cr<sub>(1-x)</sub>V<sub>x</sub> with concentration identifies the N-hole pocket as the source of the long period oscillation of the Exchange Coupling across Cr and Cr<sub>(1-x)</sub>V<sub>x</sub> spacers. The N-hole pocket is fairly isotropic but there are little differences in the spanning vectors in different directions which could be measured by measuring the differences of the oscillation periods for different growth directions. Interestingly, the shape and orientation of the N-hole pockets can also be determined by 2-dimensional ACAR experiments. Clearly, a quantitative agreement between the KKR-CPA theory and the two above, very different, experiments would be a significant step towards establishing the measurement of the above discussed periods as a quantitative probe of topologically complex Fermi surfaces such as those which are host to Electronic Topological Transitions in transition metal alloys.   
Note Added: After submitting the present letter for publication we became aware of the work of D. Koelling  who has drawn similar conclusion to us on the basis of the Rigid Band Model calculations.

One of the authors (NNL) was supported by the TMR network on ‘Interface Magnetism’ (contract ERBFMRXCT960089) of the European Union. Also two of us (BG and EB) acknowledge financial support by INFM and the use of the facilities at CECUM (Univ. of Messina).