Giant magnetoresistance in laser-deposited permalloy/Ag multilayers Jörg Faupel, Hans-Ulrich Krebs, Andrea Käufler, Yuansu Luo, Konrad Samwer et al. Citation: J. Appl. Phys. 92, 1171 (2002); doi: 10.1063/1.1489088 View online: http://dx.doi.org/10.1063/1.1489088 View Table of Contents: http://jap.aip.org/resource/1/JAPIAU/v92/i2 Published by the American Institute of Physics. Related Articles (001) textured L10-FePt pseudo spin valve with TiN spacer Appl. Phys. Lett. 99, 252503 (2011) Sign change of tunnel magnetoresistance ratio with temperature in epitaxial Fe/MgO/Co2MnSn magnetic tunnel junctions J. Appl. Phys. 110, 073905 (2011) Enhancement of magnetoresistance by ultra-thin Zn wüstite layer Appl. Phys. Lett. 99, 132103 (2011) Coexistence of exchange bias effect and giant magnetoresistance in a Ni/NiO nanogranular sample J. Appl. Phys. 110, 043922 (2011) Unusual magnetoresistance in a topological insulator with a single ferromagnetic barrier Appl. Phys. Lett. 98, 243112 (2011) Additional information on J. Appl. Phys. Journal Homepage: http://jap.aip.org/ Journal Information: http://jap.aip.org/about/about_the_journal Top downloads: http://jap.aip.org/features/most_downloaded Information for Authors: http://jap.aip.org/authors Downloaded 26 Feb 2012 to 59.162.23.73. Redistribution subject to AIP license or copyright; see http://jap.aip.org/about/rights_and_permissions JOURNAL OF APPLIED PHYSICS VOLUME 92, NUMBER 2 15 JULY 2002 Giant magnetoresistance in laser-deposited permalloyÕAg multilayers Jörg Faupel and Hans-Ulrich Krebsa) Institut für Materialphysik, University of Göttingen, Hospitalstrasse 3-7, 37073 Göttingen, Germany Andrea Käufler, Yuansu Luo, and Konrad Samwer I. Physikalisches Institut, University of Göttingen, Bunsenstrasse 9, 37073 Göttingen, Germany Satish Vitta Department of Metallurgical Engineering and Materials Science, Indian Institute of Technology, Bombay, Mumbai 400076, India 共Received 18 January 2002; accepted for publication 6 May 2002兲 Giant magnetoresistance 共GMR兲 of 3.5% in low fields of about 10 Oe was observed at room temperature in as-prepared laser-deposited Ni80Fe20 /Ag 共permalloy/Ag兲 multilayers. Strong columnar growth in combination with preferential sputtering of Ag from the film surface during deposition of Ni80Fe20 layer helps to directly create a discontinuous multilayer structure necessary for high GMR values. The magnetoresistance was found to increase to 5.1% after annealing for just 10 min at 275 °C. This increase is attributed to structural relaxation processes such as demixing of the intermixed interfaces, preferential diffusion of Ag to the column boundaries and reduction of structural defects. Pulsed laser deposition appears to be a suitable technique for the preparation of permalloy/Ag films with considerable GMR in a one-step process. © 2002 American Institute of Physics. 关DOI: 10.1063/1.1489088兴 Multilayers of Ni80Fe20 /Ag 共Ni80Fe20 , permalloy, Py兲 are well known for a low field giant magnetoresistance 共GMR兲 effect of the order of 5%– 6% in saturation fields of about 10 Oe at room temperature.1 These are of special interest because they can be used as highly sensitive magnetic field sensors. Py/Ag multilayers prepared at room temperature by magnetron sputtering1 or molecular beam epitaxy2 共MBE兲 show negligible GMR in the as-prepared state. The multilayers prepared by sputtering exhibit the GMR values mentioned above only after annealing at 315 °C for 10 min while those prepared by MBE require annealing at 400 °C for 40 min to show similar GMR values. The presence of magnetic Py islands in the Ag matrix in a quasimultilayer configuration is known to promote magnetostatic antiferromagnetic ordering leading to the GMR effect.3,4 Here it is reached by the destruction of the continuous multilayer to form a discontinuous structure. The idea of the present work was to obtain a similar discontinuous state of the Py/Ag multilayers essential for observing the GMR effect already in the as-deposited state itself. This is made possible using pulsed laser deposition 共PLD兲 because of the columnar growth tendency in many systems.5 To attain a discontinuous structure the growth behavior of Py on Ag and Ag on Py had to be studied in detail so that the critical value for the thickness at which a discontinuous to a continuous layer formation transition occurs was determined. The GMR effect could be optimized on annealing at relatively low temperatures of 275 °C, when compared to those made by sputtering or MBE. The structural and magnetoresistive properties of the as-deposited and annealed multilayers are discussed and compared with those of conventional deposition techniques. The multilayers were prepared by PLD at room temperature in ultrahigh vacuum (⬍10⫺9 mbar) using a KrF excimer laser 共wavelength of 248 nm, pulse duration of 30 ns, laser fluence of 5– 6 J/cm2兲. Details of the exact geometry are published elsewhere.6 The multilayers were deposited onto clean Si共111兲 substrates kept at room temperature. A typical multilayer consists of 20 bilayers of Ag/Py with a Ag capping layer and is denoted as 关 Ag(x)/Py(y) 兴 20 . The thicknesses x and y 共given in nm兲 of the Ag and Py layers, respectively, were varied but were always less than 7.0 nm as thicknesses larger than this value would not result in coupling of Py needed for GMR. High purity Ag foil and a Ni80Fe20 alloy target were used for the deposition of the multilayers. GMR measurements were performed at room temperature using a four-point in-line geometry of contacts with the current flowing in plane and the magnetic field applied parallel to the film plane. For each sample two measurements were performed with the applied magnetic field parallel and perpendicular to the current flow. The maximum GMR value is given by (R 0 ⫺R S )/R S , where R S is the resistance in saturation field and R 0 is that in zero field. The microstructure of the multilayers was studied by wide-angle x-ray diffraction in Bragg–Brentano geometry using Co K␣ radiation and by low-angle 共below 3°兲 x-ray reflectometry using Cu K␣ radiation. Simulations were performed using interface and surface roughnesses as well as bilayer periodicity as fit parameters. On some samples, hot-stage wide-angle x-ray measurements were performed in UHV ambient using a constant rate of 0.5 °C/min and taking scans every 10 °C. Other multilayers were annealed at different temperatures in the range 250– a兲 Electronic mail: [email protected] 0021-8979/2002/92(2)/1171/3/$19.00 1171 © 2002 American Institute of Physics Downloaded 26 Feb 2012 to 59.162.23.73. Redistribution subject to AIP license or copyright; see http://jap.aip.org/about/rights_and_permissions 1172 Faupel et al. J. Appl. Phys., Vol. 92, No. 2, 15 July 2002 FIG. 2. 共a兲 GMR vs magnetic field H curves and 共b兲 maximum GMR values for 关 Ag(x)/Py(1.4) 兴 20 samples with different Ag-spacer thicknesses x as a function of annealing temperatures. FIG. 1. In situ rate measurement at the Ag/Py interface shows that the film thickness is reduced due to strong sputtering of the heavier Ag atoms by the impinging Ni and Fe ions until an equilibrium rate is observed after about 170 laser pulses, 1.5 nm. 375 °C for 10 min to study the effect of annealing both on the structure as well as the GMR effect. The discontinuous to a continuous layer formation transition was determined by monitoring the deposition rate during growth of Py on Ag. The results are shown in Fig. 1. At the Py/Ag interface the mass, as observed by the quartz crystal balance, is reduced first and an equilibrium rate is observed after about 170 laser pulses. The reduction of mass is due to a combination of sputtering as well as ion implantation effects as discussed in detail in Ref. 7. The energetic Fe and Ni ions 共100 eV兲8 present in the laser plasma plume sputter the heavy Ag atoms from the underlying layer and also get implanted. The equilibrium deposition rate for Ni80Fe20 is observed as soon as the Ag film surface is completely covered by Fe and Ni atoms. At this thickness the Py film undergoes a transition from a discontinuous state to a continuous state. This critical thickness was determined both from the thickness monitor and x-ray diffraction measurements and is found to be about 1.4 nm. Hence in the present work the thickness of the Py layer is kept around this value in all the different multilayer combinations. The maximum GMR effect of 3.5% with a full width at half maximum 共FWHM兲 of 10.7 Oe and a sensitivity of 0.52% Oe⫺1 at room temperature was observed in asdeposited 关 Ag(6.2)/Py(1.4) 兴 20 multilayers and is shown in Fig. 2共a兲. It should be mentioned here that this GMR value is similar to that observed in Py/Ag multilayers prepared by sputtering and MBE. The main difference however is that in the present work these values are observed in as-deposited multilayers while those prepared by the more conventional methods exhibit these values only after annealing at relatively high temperatures. The GMR value in multilayers with thicknesses other than 1.4 nm for the Py layer and 6.2 nm for the Ag layer is found to be ⬍3.5% as shown in Fig. 2共b兲. All the samples show anisotropic magnetoresistance effects 共AMR兲 of 0.2%–0.4%, a large region, where the resistance linearly changes with the applied magnetic field, and very low hysteresis. Thus, the resistance values are independent of the history of the sensor which is important for applications. The GMR value of the as-deposited multilayers was found to increase on annealing for 10 min in the temperature range 275–300 °C. A maximum GMR value of 5.1% was obtained after annealing at 275 °C, while the maximum sensitivity of 0.66% Oe⫺1 was observed at 250 °C. It should be mentioned that the mean resistivity of the multilayer remains almost constant during annealing. The increase of GMR is therefore based on an increment of (R 0 ⫺R S ). In Fig. 2共b兲 the maximum GMR values are shown as a function of annealing temperature for multilayers with different Ag spacer layer thicknesses. It can be seen that the GMR value increases systematically with increasing spacer layer thickness and for thicknesses ⬍2.2 nm no GMR was observed even after annealing. Notice however the rate of increase of GMR is low compared to that observed in conventionally grown multilayers.2,3 This is because the multilayers in the asdeposited state already exhibit considerable GMR effect due to the special deposition conditions adopted for growth during PLD. The structural changes accompanying annealing of the multilayers have been studied using both low angle x-ray reflectivity and high angle x-ray diffraction. The low angle x-ray reflectivity scans from the 关 Ag(4.4)/Py(1.4) 兴 20 multilayer as a function of annealing temperature are shown in Fig. 3. The presence of a clear first order bilayer period peak together with total thickness oscillations in the asprepared multilayer indicates that the layers are well formed and ordered along the growth direction. On annealing however the first order peak shifts to higher angles or lower bilayer periods, decreases in intensity and becomes broad indicating that the layered structure becomes weak. At the same time the total thickness oscillations disappear due to increasing surface roughness. The rms roughness at the two interfaces, Py on Ag and Ag on Py has been determined from a simulation of the reflectivity of the multilayer. The Py on Ag interface roughness is found to increase from about 2.5 to 4.0 nm due to annealing at 275 °C while the Ag on Py interface roughness is found to be constant at about 1.5 nm. This clearly shows the asymmetric growth behavior of the two components, Py and Ag as well as the asymmetric annealing response at the two interfaces. The high angle x-ray diffraction spectrum as a function of temperature from the 关 Ag(2.7)/Py(1.8) 兴 20 multilayer is Downloaded 26 Feb 2012 to 59.162.23.73. Redistribution subject to AIP license or copyright; see http://jap.aip.org/about/rights_and_permissions Faupel et al. J. Appl. Phys., Vol. 92, No. 2, 15 July 2002 FIG. 3. Low angle x-ray reflectivity as a function of annealing temperature shows that the layered structure becomes weak and discontinuous. The clear first order peak observed in the as-deposited multilayer indicates the presence of good layering along the growth direction. obtained using a high vacuum (⬍10⫺6 mbar) hot stage attachment and is shown in Fig. 4共a兲. The presence of clear satellite peaks up to about 300 °C indicates the presence of a layered structure which breaks down for T⬎300 °C as seen by the disappearance of satellite peaks. These results are in close agreement with the low angle reflectivity studies. Concurrent to the disappearance of the satellite peaks the intensity of the Ag共111兲 peak increases and sharpens indicating a grain growth phenomenon. In order to understand the structural changes accompanying annealing in detail the Ag planar spacing d of the strongest peak corresponding to Ag共111兲 plane reflection is plotted, corrected for linear thermal expansion, as a function of temperature in Fig. 4共b兲. Also the planar spacing of the multilayers from the annealing series depicted in Fig. 2共b兲 shows the same salient features. The planar spacing decreases with increasing temperature and reaches, independent of the initial value, a quasi-steady-state value in the temperature range 250–300 °C. This indicates that the struc- ture reaches a state of relaxation. At this state the annealed samples posses the highest GMR values as shown in Fig. 2共b兲. The presence of pronounced GMR effect exhibiting structure in the as-deposited Py/Ag multilayers prepared by pulsed laser deposition can be understood by considering the energetics of the deposition process. The laser generated plasma plume has energetic ions, of the order of 100 eV, which help in increasing the surface roughness, sputtering at the interfaces and ion implantation. Because the sputter yield of Py is much lower than that of Ag, in the early stages of Py growth on Ag the interfacial roughness is increased by preferential sputtering of Ag by the impinging Fe and Ni ions.7,9 The growth of Py columns however is unhindered because of the low sputter yields for Fe and Ni. This model accounts for the asymmetric interface roughness observed at the two interfaces, Py on Ag and Ag on Py. The high interfacial roughness requires that the Ag layer has a certain minimum thickness so as to avoid bridging of the Py islands and thus ferromagnetic coupling. Then, a magnetostatic coupling favors antiferromagnetic alignment which is needed for a high GMR value and this is why the multilayers exhibit a high GMR for a Ag layer thickness of 6.2 nm. The high kinetic energy of the ions which is a characteristic feature of high fluence PLD results in considerable intermixing at the interfaces, a residual compressive stress in the films, and a large density of defects.8 Annealing results in an increased diffusion of Ag into the boundaries between Py columns and also agglomeration of Ag within the Py layers. This reduces direct coupling of the Py islands and promotes magnetostatic antiferromagnetic ordering. The decrease in overall defect density increases spin dependent electron scattering contribution to the resistivity and thus aids in GMR. In conclusion, Py/Ag multilayers which exhibit room temperature GMR of 3.5% in the as-deposited state have been prepared by PLD. The discontinuous growth mode of Py together with sputtering of Ag by energetic Fe and Ni ions result in a structure which is ideally suited for GMR effect. Annealing the preexisting discontinuous layered structure enhances the GMR effect to 5.1% due to a combination of Ag diffusion to isolate the Py layers and reduction of structural defects. It should be possible to produce multilayer structures with higher GMR value in the as-deposited condition by a further optimization of the PLD process. 1 FIG. 4. 共a兲 High angle x-ray diffraction patterns from hot-stage measurements at elevated temperatures 共spectra were taken in steps of 10 °C兲 and 共b兲 the planar spacing d of the highest peak as a function of annealing temperature from 关 Ag(x)/Py(y) 兴 20 multilayers corrected for thermal lattice expansion. The maximum GMR values are found in the marked area, when the multilayers are in a relaxed state. 1173 T. L. Hylton, K. R. Coffey, M. A. Parker, and J. K. Howard, J. Appl. Phys. 75, 7058 共1994兲. 2 R. F. C. Farrow, R. F. Marks, T. A. Rabedeau, M. F. Toney, D. Dobbertin, R. Beyers, and S. S. P. Parkin, J. Appl. Phys. 76, 3688 共1994兲. 3 M. A. 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