JOURNAL OF APPLIED PHYSICS                                     VOLUME 85, NUMBER 8                                          15 APRIL 1999

Biquadratic coupling in sputtered Fe/Cr/Fe still in need
of a new mechanism
          S. M. Rezende,a) C. Chesman, M. A. Lucena, M. C. de Moura, A. Azevedo,
          and F. M. de Aguiar
          Departamento de Fi´sica, Universidade Federal de Pernambuco, Recife PE 50670-901, Brazil
          S. S. P. Parkin
          IBM Almaden Research Center, San Jose, California 95120-6099
          The bilinear (J1) and biquadratic (J2) exchange coupling constants were measured in sputtered
          trilayers of  100  Fe 40 Å /Cr s /Fe 40 Å  for several Cr spacer layer thicknesses in the range
          s 8­35 Å and as a function of temperature T, using magneto-optical Kerr effect magnetometry,
          Brillouin light scattering, and ferromagnetic resonance. In the samples in the range s 8­13 Å,
          corresponding to the first antiferromagnetic peak of J1 , J2 follows J1 with a room temperature ratio
          J2 /J1 0.1, while in the range 25­35 Å, corresponding to the second antiferromagnetic peak, J2
          also follows J1 but with a much larger ratio J2 /J1 1. This result, as well as the temperature
          dependence of J2 in all samples but the one with s 15 Å, cannot be explained by any of the intrinsic
          or extrinsic mechanisms that have been proposed for the origin of the biquadratic exchange coupling
          in Fe/Cr/Fe. © 1999 American Institute of Physics.  S0021-8979 99 68008-2 


INTRODUCTION                                                               some attributed to intrinsic properties of the spacer layer and
                                                                           others to extrinsic factors, such as the presence of impurities
     Magnetic multilayers, consisting of stacks of ferromag-               or interface roughness. Intrinsic mechanisms seem not to ac-
netic layers separated by nonmagnetic metallic layers, have                count for the observed coupling strengths and signs, nor for
attracted considerable attention due to their unique physical              its temperature dependence.18 On the other hand, if the
properties and potential for technological applications. Many              mechanisms based on extrinsic factors prevails in the BEC,
multilayer systems exhibit a coupling between the magnetic                 one expects the value of the coupling constant J2 to be quite
layers mediated by the nonmagnetic spacers, which oscillates               sensitive to details of the sample preparation conditions. In-
periodically between ferromagnetic  FM  and antiferromag-                  deed, there is a considerable spread in the values of J2 mea-
netic  AFM  as the spacer-layer thickness varies in the range              sured by different groups for nominally the same system,
of 5­50 Å.1­5 Due to its central role in the properties of                 indicating the dominance of extrinsic mechanisms. However,
magnetic multilayers, the coupling between the magnetic                    there are conflicting reports on the temperature and spacer
layers through the nonmagnetic metallic spacer has been the                layer thickness dependence of J2 and only in very few cases
subject of extensive investigations for nearly ten years. Ex-              there seems to be a reasonable connection between data and
perimentally this coupling is more conveniently studied in a               some specific extrinsic mechanism.22 The fact is that the
trilayer structure, formed by two magnetic thin films sepa-                whole question of the origin of the BEC is still quite
rated by a nonmagnetic layer, Fe/Cr/Fe being the most stud-                controversial23 and deserves further investigation. In this ar-
ied system.4­12                                                            ticle we present new data on the temperature dependence of
     The coupling between the magnetic layers is usually                   J1 and J2 in the prototype system  100  Fe/Cr/Fe for varying
dominated by a mechanism which can be modeled by an                        Cr spacer layer thickness and show that in only one sample
interaction energy of the form  J1m1­m2 , where m1and m2                   the exchange fluctuation mechanism accounts for the experi-
are the unit magnetizations of the two magnetic layers and J1              mental data.
is the bilinear exchange coupling constant. The origin of this
coupling lies in the interaction between the s electrons in the
metallic spacer and the d electrons in the magnetic
layers,13­15 and is currently well understood.16 However,                  EXPERIMENTAL RESULTS
more recently it was observed5,6,17 that under certain condi-                  The samples investigated are single-crystal trilayer struc-
tions the magnetic moments of the two layers tend to align at              tures of  100  Fe 40 Å /Cr s /Fe 40 Å  grown by magnetron
90° with respect to each other. This alignment may be ac-                  sputter deposition, as described in Ref. 25 on MgO  100 
counted for through an interaction energy described by a                   substrates. All samples have the same Fe layer thickness,
phenomenological biquadratic exchange coupling  BEC                        d 40 Å, and a thin Cr cap layer. Initial characterization of
 J2(m1­m2)2, where J2 is the biquadratic coupling con-                     the coupling was made by magneto-optical Kerr effect
stant. Over the last few years several mechanisms have been                 MOKE  with a Cr wedged sample, with 0 s 70 Å. Then
proposed for the origin of the biquadratic coupling,18­21                  a series of samples was prepared with uniform Cr thickness
                                                                           varying from 5 to 35 Å, a range that corresponds to the first
a Electronic mail: smr@df.ufpe.br                                          two antiferromagnetic peaks.

0021-8979/99/85(8)/5892/3/$15.00                                   5892                                © 1999 American Institute of Physics



J. Appl. Phys., Vol. 85, No. 8, 15 April 1999                                                                               Rezende et al.         5893























FIG. 1. Room-temperature exchange coupling constants measured in sput-    FIG. 2. Temperature dependence of the exchange coupling constants in
tered  100  Fe 40 Å /Cr s /Fe 40 Å  by MOKE, BLS, and FMR.                Fe 40 Å /Cr s /Fe 40 Å . The symbols represent the data for the samples
                                                                          with s 11  circles , 13  squares , and 15 Å  triangles  and the solid lines are
                                                                          fits with theoretical predictions.

       In order to obtain reliable values for J1 and J2 , we have
used three independent techniques, namely, MOKE magne-                         Figure 2 shows the temperature dependence of J1 and J2
tometry, Brillouin light scattering  BLS , and ferromagnetic              measured in three samples with Cr layer thickness s 11, 13,
resonance  FMR . The data were fitted with a phenomeno-                   and 15 Å. Qualitatively the data are similar to results previ-
logical energy model including bilinear and biquadratic ex-               ously obtained in several systems, both exchange constants
change couplings, as well as surface and crystalline cubic                decrease with increasing temperature. However, a detailed
anisotropy contributions. Details of the measuring techniques             analysis of the temperature dependence contains important
and the procedures used to extract the values of J1 and J2 are            clues on the mechanisms responsible for the coupling be-
presented elsewhere.24,25                                                 tween the magnetic layers.
       Figure 1 shows the room-temperature values for J1 and
J2measured in 14 samples with varying Cr spacer thickness.                DISCUSSION
The vertical bars represent the uncertainties due to the esti-
mated errors in each fitting plus the spread in the values                     In order to discuss the origin of the biquadratic coupling
obtained with the various techniques. Two AF peaks alter-                 in our Fe/Cr/Fe samples, we start looking at the behavior of
nating with one FM peak are observed in J                                 the bilinear coupling J
                                                   1 in the thickness                                    1 . There is general agreement today
range 5 Å s 35 Å, a well known result which has been                      that the bilinear coupling originates in the interaction be-
obtained by many authors. The maximum  absolute  value of                 tween the s electrons in the Cr layer and the d electrons in
J                                                                         the Fe layers, the so-called intrinsic mechanism. Calculations
     1 in the first AF peak is 0.59 erg/cm2, for s 9.5 Å, a value
somewhat smaller than J                                                   taking into account the full electronic structure of the metals
                               1 1 erg/cm2 reported for some mo-
lecular beam epitaxy  MBE  grown samples,3,4,9 but similar                show26,27 that for perfectly sharp interfaces the behavior of
to those reported for other MBE7 and sputtered11  100  Fe/                J1 with the spacer layer thickness is entirely dominated by
Cr/Fe trilayers.                                                          short period oscillations with amplitude decaying with in-
       The result for J                                                   creasing thickness. The maximum negative value of J
                           2 is not so well known. In fact, to our                                                                              1is ap-
knowledge, this is the first measurement of J                             proximately 7 erg/cm2, which is an order of magnitude larger
                                                        2 vs spacer-
layer thickness in the second AF peak. The data show that J               than the measured values. This discrepancy is accounted for
                                                                    2
is negative in the whole range, and that its ratio to J                   by the existence of roughness, interdiffusion, vacancies, and
                                                              1 varies
considerably with s. In most of the first AF peak, J                      steps in the real sample, which smooth out the short period
                                                           2 follows
a dependence with s similar to that of J                                  oscillations and drastically reduce the peak value.27 While
                                                 1 , with J2 /J1 0.1.
However, near the crossing from AF to FM  s 15 Å , this                   comparison between theory and experimental data for the
ratio increases to J                                                      strength of the coupling is not satisfactory, the same is not
                        2 /J1 0.3, which is similar to that mea-
sured in a structure Fe 28 Å /Cr 15.8 Å  grown by MBE on                  true for the temperature dependence of J1 . Consider the the-
a  100  Fe whisker.8 Throughout the Cr thickness range                    oretical prediction for the intrinsic mechanism21 J1(T)
s 16­24 Å, corresponding to the second FM peak, the ratio                  J1(0)f1(T), where f1(T)  (T/T0)/sinh(T/T0) .
 J2 /J1 remains in the range of 0.2­0.3. Surprisingly, in the                  The solid lines in Fig. 2 a  represents the fits of this
second AF peak the ratio increases to J2 /J1 1, so that the               function to the experimental data, obtained with T0 390,
antiferromagnetic phase ceases to exist.24,25                             214, and 122 K for the samples with Cr layer thickness



5894         J. Appl. Phys., Vol. 85, No. 8, 15 April 1999                                                                                        Rezende et al.

s 11, 13, and 15 Å, respectively. Note that T0 decreases                        This yields an exponent a 0.25 0.10, implying that the
with increasing s, and although it does not follow the 1/s law                  temperature dependence of J2 for the s 15 Å sample is con-
of the simple theory, the good fits indicate that the intrinsic                 sistent with the prediction of the exchange fluctuation
mechanism accounts for the origin of the bilinear exchange                      mechanism. However none of the proposed mechanisms for
coupling.                                                                       the BEC12,18 can account quantitatively for the data in the
    Regarding the origin of the biquadratic coupling J2 , we                    other Fe/Cr/Fe samples. Therefore, the present results add
first note that it cannot be attributed to intrinsic mechanisms                 evidence to previous12,23 conclusions that further theoretical
for two reasons: the predicted oscillation period for J2 is                     and experimental work is necessary to fully explain the bi-
smaller than for J1 , whereas the data of Fig. 1 shows J2                       quadratic exchange coupling in magnetic multilayers.
following J1 ; theory21 predicts a rapid decay of J2 with in-
creasing s, which is certainly not the case of the data. For the                ACKNOWLEDGMENTS
samples under investigation here, among the various extrin-
sic sources proposed for J                                                               This work has been supported by the Brazilian federal
                                     2 , the most plausible one is the
Slonczewski's exchange fluctuation mechanism18 caused by                        agencies CNPq, FINEP, PADCT, and CAPES and the Per-
interface roughness. According to the model, J                                  nambuco state agency FACEPE. The work at IBM was par-
                                                              2 arises from
the combined effect of the rapid oscillation in the intrinsic J                 tially supported by the Office of Naval Research.
                                                                           1
and the variation in spacer layer thickness in the form of
terraces. If J                                                                   1 P. Gru¨nberg, R. Schreiber, Y. Pang, M. B. Brodsky, and H. Sowers, Phys.
                  1 varies in steps of  2 J1 , the first order con-
tribution of this mechanism to the BEC is18                                           Rev. Lett. 57, 2442  1986 .
                                                                                 2 S. S. P. Parkin, N. More, and K. P. Roche, Phys. Rev. Lett. 64, 2304
                4  J                                                                   1990 .
                                                                                 3
    J                   1 2L                                                          See, for example, B. Heinrich and J. F. Cochran, Adv. Phys. 42, 523
         2                      coth  d ,                                 1 
                    3A                   L                                             1993 ; Ultrathin Magnetic Structures, edited by B. Heinrich and J. A. C.
                                                                                      Bland  Springer, Berlin, 1994 .
where A is the exchange stiffness constant of the Fe layer, L                    4 J. J. Krebs, P. Lubitz, A. Chaiken, and G. A. Prinz, Phys. Rev. Lett. 63,
is the terrace width, and d is the Fe layer thickness. Equation                       1645  1989 ; J. Appl. Phys. 67, 5920  1990 .
                                                                                 5 J. Unguris, R. J. Celotta, and D. T. Pierce, Phys. Rev. Lett. 67, 140  1991 .
 1  predicts that J2 is always negative, favoring the 90°                        6 M. Ruhrig, R. Scha¨fer, A. Hubert, R. Mosler, J. A. Wolf, S. Demokritov,
alignment, as observed in the experiments, and that its                               and P. Gru¨nberg, Phys. Status Solidi A 125, 635  1991 .
strength varies with the square of  J                                            7 U. Ko¨bler, K. Wagner, R. Wichers, A. Fuss, and W. Zinn, J. Magn. Magn.
                                                    1 . Considering that  J1
is a step change in the bilinear coupling arising from the                            Mater. 103, 236  1992 .
                                                                                 8 M. From, L. X. Liao, J. F. Cochran, and B. Heinrich, J. Appl. Phys. 75,
short period oscillation, and that the measured coupling rep-                         6181  1994 .
resents an average of J                                                          9
                                 1 , Eq.  1  predicts for J2 a tempera-               R. J. Hicken, C. Daboo, M. Gester, A. J. R. Ives, S. J. Gray, and J. A. C.
ture dependence following J2                                                          Bland, J. Appl. Phys. 78, 6670  1997 .
                                              1(T)/A(T). In order to verify     10
this prediction, it is necessary to take into account the tem-                        A. J. R. Ives, J. A. C. Bland, R. J. Hicken, and C. Daboo, Phys. Rev. B 55,
                                                                                      12428  1997 .
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determined A T  by measuring the volume mode frequencies                               1996 .
in a 250 Å thick single film of  100  Fe/MgO as a function of                   12 S. O. Demokritov, J. Phys. D 31, 925  1998 .
                                                                                13
temperature using BLS.                                                                Y. Wang, P. M. Levy, and J. L. Fry, Phys. Rev. Lett. 65, 2732  1990 .
                                                                                14 D. M. Edwards, J. Mathon, R. B. Muniz, and M. S. Phan, Phys. Rev. Lett.
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fluctuation mechanism cannot by itself explain the measured                     15 P. Bruno and C. Chappert, Phys. Rev. Lett. 67, 1602  1991 ; Phys. Rev. B
BEC in the whole range of Cr spacer layer thickness. The                              46, 261  1992 .
                                                                                16 A. T. Costa, Jr., J. d'Albuquerque e Castro, and R. B. Muniz, Phys. Rev.
first argument is that Eq.  1  predicts that the amplitude of J2                      B 56, 13697  1997 .
decays with increasing s following J2                                           17
                                                     1. This is in complete           C. J. Gutierrez, J. J. Krebs, M. E. Filipkowski, and G. A. Prinz, J. Magn.
disagreement with the data, which show that while the peak                            Magn. Mater. 116, L305  1992 .
                                                                                18
amplitude of J                                                                        J. Slonczewski, Phys. Rev. Lett. 67, 3172  1991 ; J. Magn. Magn. Mater.
                    1 does decrease with increasing s, the ratio                      150, 13  1995 .
J2 /J1 is  0.1 in the first AF peak and  1 in the second AF                     19 J. Barna´s and P. Gru¨nberg, J. Magn. Magn. Mater. 121, 326  1993 .
peak. The second argument is based on the temperature de-                       20 R. P. Erickson, K. B. Hathaway, and J. R. Cullen, Phys. Rev. B 47, 2626
pendence of the coupling constants. The solid lines in Fig.                            1993 .
                                                                                21
2 b  are the fits of the J                                                            D. M. Edwards, J. M. Ward, and J. Mathon, J. Magn. Magn. Mater. 126,
                                   2(T) data with   f 1(T)  b, obtained               380  1993 .
with the values b 11.8, 6.6, and 1.7 for the samples with Cr                    22 M. Scha¨fer, S. Demokritov, S. Mu¨ller-Pfeiffer, R. Scha¨fer, M. Schneider,
layer thickness s 11, 13, and 15 Å, respectively. This shows                          P. Gru¨nberg, and W. Zinn, J. Appl. Phys. 77, 6432  1995 .
that only for the sample with s 15 Å the temperature varia-                     23 Z. Celinski, B. Heinrich, and J. F. Cochran, J. Magn. Magn. Mater. 145,
tion of J                           2                                                 L1  1995 .
             2 is close to the J1(T) dependence predicted by the                24 A. Azevedo, C. Chesman, S. M. Rezende, F. M. de Aguiar, X. Bian, and
exchange fluctuation mechanism. In order to verify if this                            S. S. P. Parkin, Phys. Rev. Lett. 76, 4837  1996 .
dependence really applies to the s 15 Å sample, one needs                       25 S. M. Rezende, C. Chesman, M. A. Lucena, A. Azevedo, F. M. de Aguiar,
to take into account the temperature variation of the ex-                             and S. S. P. Parkin, J. Appl. Phys. 84, 958  1998 .
                                                                                26
change stiffness. So we fitted the BLS data with A(T)                                 M. D. Stiles, Phys. Rev. B 54, 14679  1996 ; and references therein.
                                                                                27 A. T. Costa, Jr., J. d'Albuquerque e Castro, and R. M. Muniz  unpub-
   f 1(T) a,, with T0 122 K appropriate for this sample.                              lished .