An analysis of both magnetic and magnetotransport properties is presented for electrodeposited multilayers prepared intentionally under conditions to make the superparamagnetic (SPM) magnetization contribution comparable to or larger than the ferromagnetic term. Based on a model elaborated for the giant magnetoresistance (GMR) of granular metals [N. Wiser, J. Magn. Magn. Mater. 159, 119 (1996); B. Hickey et al., Phys. Rev. B. 51, 667 (1995)], it is shown that in such multilayers both the magnetization and the GMR can be decomposed into ferromagnetric and superparamagnetic contributions where the latter term is described by a Langevin function. The size of the SPM regions estimated from the experimental data is in the nanoscale regime. It is believed that the method applied here gives a quantitative answer to the problem of the often observed nonsaturating behavior of GMR in multilayers. Electrodeposited multilayers are particularly prone to this feature although the occurrence of SPM regions is quite common in multilayers prepared by any technique. Therefore, this type of analysis should help better understanding of the factors influencing the GMR of multilayer films.
The giant magnetoresistance ͑GMR͒ effect was studied on electrodeposited Co-Cu/Cu multilayers of 300 bilayer repeats which were produced in an electrochemical cell with homogeneous current distribution from a bath with two solutes (CoSO 4 ,CuSO 4 ). The preparation employed the conventional potentiostatic/potentiostatic and galvanostatic/galvanostatic, as well as an unprecedented galvanostatic/potentiostatic ͑G/P͒ control. We find that the specific deposition parameters rather than the deposition mode itself are decisive for the magnitude of the GMR which could be as high as 10% measured at 1 kOe on substrate-free multilayers in optimized G/P conditions. For this new deposition mode, detailed studies on the dependence of GMR on Co and Cu layer thicknesses as well as the bath pH were performed. No oscillatory behavior of the GMR as a function of the Cu layer thickness could be observed. The results suggest the importance of a Co-dissolution and/or a Co vs. Cu exchange reaction after completing the deposition of each magnetic layer. These reactions lead to the formation of a Cu or Cu-rich interface layer prior to the electrochemical deposition of the actual Cu layer during the subsequent pulse in either deposition mode. It turned out that the properties of this interfacial layer ͑thickness, degree of chemical intermixing͒ strongly influence the resulting GMR behavior of the multilayer.
─ The electrical resistivity and the anisotropic magnetoresistance (AMR) was investigated for Ni-Co alloys at and below room temperature. The Ni-Co alloy layers having a thickness of about 2 m were prepared by electrodeposition on Si wafers with evaporated Cr and Cu underlayers. The alloy composition was varied in the whole concentration range by varying the ratio of Ni-sulfate and Co-sulfate in the electrolyte. The Ni-Co alloy deposits were investigated first in the as-deposited state on the substrates and then, by mechanically stripping them from the substrates, as self-supporting layers both without and after annealing.According to an X-ray diffraction study, a strongly textured face-centered cubic (fcc) structure was formed in the as-deposited state with an average grain size of about 10 nm. Upon annealing, the crystal structure was retained whereas the grain size increased by a factor of 3 to 5, depending on alloy composition. The zero-field resistivity decreased strongly by + Ph.D. student at
─ A detailed study of the evolution of the magnetoresistance was performed on electrodeposited Co/Cu multilayers with Cu layer thicknesses ranging from 0.5 nm to 4.5 nm. For thin Cu layers (up to 1.5 nm), anisotropic magnetoresistance (AMR) was observed whereas multilayers with thicker Cu layers exhibited clear giant magnetoresistance (GMR) behaviour. The GMR magnitude increased up to about 3.5 to 4 nm Cu layer thickness and slightly decreased afterwards. According to magnetic measurements, all samples exhibited ferromagnetic (FM) behaviour. The relative remanence turned out to be about 0.75 for both AMR and GMR type multilayers. This clearly indicates the absence of an antiferromagnetic (AF) coupling between adjacent magnetic layers for Cu layers even above 1.5 nm where the GMR effect occurs. The AMR behaviour at low spacer thicknesses indicates the presence of strong FM coupling (due to, e.g., pin-holes in the spacer and/or areas of the Cu layer where the layer thickness is very small). With increasing spacer thickness, the pin-hole density reduces and/or the layer thickness uniformity improves which both lead to a weakening of the FM coupling. This improvement in multilayer structure quality results in a better separation of magnetic layers and the weaker coupling (or complete absence of interlayer coupling) enables a more random magnetization orientation of adjacent layers, all this leading to an increase of the GMR. Coercive field and zero-field resistivity measurements as well as the results of a structural study reported earlier on the same multilayers provide independent evidence for the microstructural features established here. A critical analysis of former results on electrodeposited Co/Cu multilayers suggests the absence of an oscillating GMR in these systems. It is pointed out that the large GMR reported previously on such Co/Cu multilayers at Cu layer thicknesses around 1 nm can be attributed to the presence of a fairly large superparamagnetic (SPM) fraction rather than being due to a strong AF coupling. In the absence of SPM regions as in the present study, AMR only occurs at low spacer thicknesses due to the dominating FM coupling.
Direct current plating, pulse plating, two-pulse plating, and reverse pulse plating were used to produce electrodeposited Co-Cu alloys and Co-Cu/Cu multilayers under galvanostatic control from an electrolyte containing CoSO 4 and CuSO 4 . Atomic force microscopy, X-ray diffraction, and transmission electron microscopy were used to study the sample structure and morphology. Direct current plating resulted in a Co 95 Cu 5 alloy with nearly equal amounts of face-centered cubic ͑fcc͒ and hexagonal close packed phases, while all pulsed current methods yielded multilayers with fcc structure. Giant magnetoresistance ͑GMR͒ behavior was observed in the multilayers with a maximum magnetoresistance ͑MR͒ ratio of about 9% as measured at 8 kOe. The shape of the MR curves and the magnitude of the GMR were very similar, regardless of the sign of the current between the Co deposition pulses. The results of structural studies also confirmed the formation of a multilayer structure for each pulsed electrodeposition mode. The conclusion was that the spontaneous exchange reaction between Co and Cu 2ϩ is responsible for the formation of a pure Cu layer even under reverse pulse plating conditions. The GMR of the multilayer deposits decreased with increasing bilayer number, due to the deterioration of the microstructure as the deposit grew.
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