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The magnitude of this shift is termed the exchange bias field HE and in almost all cases, the magnetic hys-teresis loop is shifted in the negative field if one defines the direction of t

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p s s

applications and materials science

status solidi www.pss-a.com

Anomalous training effect

in exchange-biased MnPd/Co bilayers

1 International Training Institute for Materials Science, Hanoi University of Technology, Hanoi, Vietnam

2 Department of Physics, Faculty of Science, National University of Singapore, 117542 Singapore

3 Department of MEMS and Micro-systems Technology, Faculty of Electronics and Communications, College of Technology,

Vietnam National University, Hanoi, Vietnam

Received 27 May 2008, revised 8 September 2008, accepted 25 September 2008

Published online 13 November 2008

PACS 75.25.+z, 75.30.Gw, 75.70.Cn, 81.15.Cd

* Corresponding author: e-mail nnguyenphuoc@yahoo.com , Phone: + 65-6516-2816, Fax: + 65-6777-6126

© 2009 WILEY-VCH Verlag GmbH & Co KGaA, Weinheim

between an antiferromagnet (AF) and a ferromagnet (FM),

discovered in 1956 [1], results in a shift of the hysteresis

loop along the magnetic field axis called exchange bias

(EB) This phenomenon has been studied extensively due

to its widespread application in spin valves and magnetic

tunnel junctions as well as its intriguing physical origin [2]

Normally, exchange bias is described as an additional

uni-directional anisotropy induced by the AF into the FM via

exchange coupling at the interface, causing a single

mag-netic hysteresis loop shifted along the magmag-netic-field axis

after the field-cooling procedure through the Néel point of

the AF The magnitude of this shift is termed the exchange

bias field (HE) and in almost all cases, the magnetic

hys-teresis loop is shifted in the negative field if one defines

the direction of the cooling field (HFC) as the positive

direction This case is referred to as negative EB The

phenomenon of positive EB was first observed in 1996 by

Nogués et al [3] when studying the systems of Fe/FeF2

and Fe/MnF2 They found that the sign of the EB field

changes from negative to positive as the cooling field

in-creases Very recently, it was found that the state of

coex-istence of positive and negative EB could be achieved in

some specific systems [4 – 7] This state manifests itself as

a double hysteresis loop

In this paper, we report on the observation of double-shifted loops in MnPd/Co when the MnPd thickness is less than 18 nm, which can be ascribed to the superposition of positive and negative EB Moreover, we present additional evidences to firmly support this assumption, namely the experimental results of temperature dependence and the observed abnormal training effect

the present work with the structure of Si(100)/MnPd (x nm)/

Co (10 nm) (x = 1.2, 3.6, 6, 12, 18, 36 nm) were fabricated

at room temperature by an RF sputter-deposition system The MnPd layers were sputtered from a composite target constituting a Pd target with Mn chips placed on it The base pressure was about 10–6 mbar, whereas the working argon pressure during deposition was 10–3 mbar The com-position of the MnPd films, identified by energy-dispersive X-ray spectroscopy (EDS), is Mn30Pd70 The samples were then annealed in a high-vacuum oven (10–5 mbar) at the temperature of 570 K for 1 h The purpose of annealing the samples at such a high temperature is to enhance the crys-tallinity of MnPd layers to obtain the antiferromagnetic phase Subsequently, they were cooled in a magnetic field

of 5 kOe to room temperature to induce the exchange bias effect The magnetic properties of the annealed bilayers

Exchange bias has been studied for a series of MnPd/Co

bilayers sputtered onto Si(100) by an RF sputter-deposition

system The double-shifted loops with an anomalous training

effect have been observed The manifestation of

double-shifted loops is interpreted as the coexistence of positive ex-change bias and negative exex-change bias, which is in agree-ment with the temperature dependence and the observed anomalous training effect

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were characterized by a vibrating sample magnetometer

(VSM) in the temperature range from 10 K to 300 K It is

known that Co may be spontaneously oxidized, forming a

thin CoO layer on the top of the samples In order to check

this possibility, we made a similar sample with the Mo

layer on the top and found that the magnetic behavior of

that sample is identical with the sample without a Mo layer

Hence, the effect of oxidation of the Co layer, if any, may

be neglected in our investigation

3 Results and discussion Figure 1a and b show the

magnetic hysteresis loops measured at T = 120 K of

MnPd (6 nm)/Co (10 nm) and MnPd (36 nm)/Co (10 nm)

bilayers, respectively A double-shifted loop is observed

in the MnPd (6 nm)/Co (10 nm) bilayer, while the

MnPd (36 nm)/Co (10 nm) bilayer shows a single-shifted

loop, i.e normal EB In the series of MnPd(x nm)/

Co (10 nm) samples, double-shifted loops are seen in

sam-ples with the thickness of MnPd layers smaller than 18 nm

These double-shifted loops have also been observed in

FeF2/Ni [4, 5], and CrMn/Co [6] systems and have been

at-tributed to the coexistence of positive and negative EB In

these systems, an antiferromagnetic coupling at the

inter-face of AF/FM is favored, causing a competition between

the Zeeman and the AF/FM exchange energy, which

re-sults in the crossover from negative to positive EB as the

cooling field is increased When the sample is cooled in an

intermediate applied field, the state of coexistence of

posi-tive and negaposi-tive EB is realized, in which a fraction of AF

spins is aligned in the cooling field due to Zeeman energy, while the rest is aligned in the opposite direction due to AF exchange coupling In our case, if the cooling field is small (less than 4 kOe), only negative EB is observed and as the cooling field is beyond 4 kOe, double hysteresis loops are seen However, due to the limit of the field-cooling system (maximum 5 kOe), we cannot observe the state of complete positive EB One should note that the present state of superposition of positive and negative EB differs from other studies [8, 9] where a double loop can be found after demagnetizing the FM, since in our case the cooling field is strong enough to saturate the magnetization of

Co layer For the sake of convenience, HE1 and HE2 are denoted as the positive and negative exchange bias fields and MS1 and MS2 as the spontaneous positive-biased and negative-biased magnetizations, respectively as seen in Fig 1a Figure 1c and d show the dependences of the EB field, unidirectional anisotropy, and coercivity on the MnPd thicknesses It is noted that for the samples with double loops, the EB field of the whole sample is defined

as the average value of HE1, HE2 and HC is estimated as the average value of the coercivities of each subloop The ob-tained unidirectional anisotropy constant JK is rather large (up to 1.1 erg/cm2) compared to other exchange bias sys-tems [2]

Shown in Fig 2 are the magnetization curves for the MnPd (6 nm)/Co (10 nm) bilayer measured at T = 120 K with the applied magnetic field rotated in the plane of the film It is seen that as the angle θ between the applied field

Figure 1 Magnetic hysteresis loops of MnPd (6 nm)/Co (10 nm) and MnPd (36 nm)/Co (10 nm) bilayers measured at 120 K (Fig 1a

and b) The dependence of exchange bias ( H E ), unidirectional anisotropy constant ( J K ) and coercivity ( H C ) on MnPd thickness (Fig 1c and d) The definitions of H E1 , H E2 , M S1 and M S2 are shown in Fig 1a (See the text for more detail.)

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Figure 2 M–H loops of MnPd (6 nm)/Co (10 nm) at T = 120 K

measured at θ = 0°, 45° and 90° with respect to the field-cooling

direction as shown in the inset

and the cooling field is 45°, we still observe the

double-shifted loops, although the subloops are slanted, indicating

that the applied field is now deviated from the easy axis

As θ = 90°, i.e the applied magnetic field is now along the

hard axis, both subloops become hard-axis curves,

result-ing in a total sresult-ingle hard-axis loop as observed in Fig 2

The present result suggests that double-shift loops

ob-served in our system are quite different from that reported

earlier in the Refs [10 – 12], where double hysteresis loops

are found when the external magnetic field is applied along

the hard axis of the AF, attributed to an additional

biquad-ratic AF – FM interaction

For more evidences to support the idea of two

oppo-sitely oriented AF domains, we have carried out a study of

the temperature dependence of this effect Shown in

Fig 3a are some representative magnetic hysteresis loops

of the MnPd (12 nm)/Co (10 nm) bilayer measured at

various temperatures It is seen that the double-shifted

loops disappear as the temperature is beyond 220 K,

which is the same as the blocking temperature of the

MnPd (36 nm)/Co (10 nm) sample that exhibits a

single-shifted loop The blocking temperature of about 220 K is

very close to the Néel point of Mn30Pd70 bulk materials

[13] The temperature dependence of positive EB field

(de-noted as HE1) and negative EB field (denoted as HE2) is

shown in Fig 3b It is clearly seen that the value of

posi-tive and negaposi-tive EB fields, though different, are varied in

a similar manner This fact can be considered as additional

evidence that the double-shifted loop originates from the

coexistence of positive and negative EB It should be

men-tioned that this explanation is valid only in the case of an

atomically flat interface with uncompensated spins In

real-ity, the natural interface roughness may play a vital role in

the mechanism of exchange bias as argued by some

au-thors [16, 17] Hence, the AF layer may be split into

multi-domain structure, which causes the applied field of 5 kOe

to be subcritical and supercritical, corresponding to the

crossover from negative EB to positive EB

More interestingly, we have observed an abnormal

training effect in the samples that exhibit double-shifted

Figure 3 (a) M–H loops of MnPd (6 nm)/Co (10 nm) bilayer measured at different temperatures (b) Temperature dependence

of positive ( H E1 ) and negative ( H E2 ) exchange bias fields in MnPd (6 nm)/Co (10 nm) bilayer H E1 and H E2 are defined in Fig 1a

loops Figure 4a and b present some representative mag-netic hysteresis loops of a MnPd (12 nm)/Co (10 nm) film after some cycles of measurement and the corresponding values of positive (HE1) and negative (HE2) EB fields as a function of the number of measurements, respectively Since the magnitudes of MS1 and MS2 correspond to the ar-eas that make positive and negative EB respectively, we can denote the normalized values of mS1 and mS2, where

mS1 = MS1/(MS1 + MS2) and mS2 = MS2/(MS1 + MS2), as the fractions of positive- and negative-biased areas The de-pendence of these positive- and negative-biased area frac-tions on the cycle measurement is shown in Fig 4c At first, the negative EB decreases very rapidly from 840 Oe to

740 Oe and levels off after 6 cycles, while the positive EB decreases slower After 11 cycles, there is no change in mS1 and mS2 At cycle 12, there is a drastic jump of HE1 and HE2

as well as mS1 and mS2 The drastic change of mS1 and mS2, namely the increase of mS2 and the decrease of mS1, implies that there is an enlargement of the negative-biased area at the cost of reducing the positive-biased area A similar ab-normal training effect has also been observed in the system

of CrMn/Co bilayers [6] and has been explained as the movement of the AF domain wall toward the positive-

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Figure 4 (a) Representative of training-effect hysteresis loops of

MnPd (12 nm)/Co (10 nm) film M–H loops for the cycles 1, 6,

12, 24 and 48 are shown (b) Positive ( H E1 ) and negative ( H E2 )

ex-change bias fields as a function of cycles of measurement (c)

Fractions of positive ( m S1 ) and negative ( m S2 ) exchange bias areas

as a function of cycles of measurement

biased domain Of great interest is the reverse training

effect for negative EB as seen in Fig 4b HE2, which is

de-creased to 740 Oe after 11 cycles of measurement, regains

the previous value of 840 Oe at cycle 12 This surprising

effect implies that the movement of the AF domain wall,

causing the enlargement of the negative-biased area,

rein-duces the untrained state Recently, Brems et al [14]

re-ported on the reverse training effect in CoO/Co bilayers, in

which the EB field regained its untrained value after

carry-ing out a M–H loop measurement along the hard axis and

this effect can be interpreted as a change in the

magnetic-domain structure in the AF layer It should be noted that

recently the physical origin of exchange bias was described

as due to a fraction of uncompensated interfacial spins

(about 4%) that are locked to the AF lattice and do not

ro-tate in an external magnetic field, while most of the other interfacial spins are affected by the external field [15] The training effect can therefore be understood as the loss of the pinned uncompensated spins Taking into account this argument, we can state that after the movement of the AF domain wall causing the enlargement of the negative-biased area, the fraction of uncompensated interfacial spins increases to its original value that results in the reverse training effect observed in our system However, for the decrease of the positive-biased area, the positive exchange bias decreases from 400 Oe to 250 Oe after the movement

of the AF domain wall, i.e the reverse training effect has not been observed in the positive subloop It is well known that positive exchange bias is in a high-energy state so it is less stable than the negative exchange bias Therefore, we may expect that after the AF domain-wall movement, the fraction of pinned uncompensated spins will be reduced It

is also very interesting to see that as we carried out more measurement, namely cycle 12 upward, the positive EB is not changed while the change of negative EB from cycle

12 to cycle 17 is very similar to the change from cycle 1 to cycle 6 This implies that after the movement of the AF domain wall, the negative-biased area is reinduced to the untreated state It is noticed that previously, Nowak et al [17, 18] explained the training effect in terms of the rear-rangement of AF domain by using their domain state model Hauet et al [19] studied the mechanism of the training effect in hard/soft Tb12Fe88/Gd40/Fe60 bilayers with positive exchange bias and found that a partial magnetiza-tion reversal of soft layers generates new domain of the hard layers, which has been subjected to a training effect

It is evidenced from their experiments that the training ef-fect is due to an irreversible reorientation of the hard-layer magnetization Hence, the present explanation employing the idea of the movement of AF domain seems to be rea-sonable for the interpretation of the abnormal training ef-fect However, one should not rule out other possibilities, e.g the granular model for the AF with thermal activation [20, 21], as a potential explanation for this behavior Re-cently, Binek [22] considered the training effect in the framework of nonequilibrium thermodynamics and found that training of the exchange bias effect originates from spin configurational relaxation, which is activated through consecutive-cycled hysteresis loops Based on this idea, one can explain the breakdown of the power-law behavior when n = 1, which is quite similar to the nonmonotonic behavior in this work Further investigation may thus need

to be performed to get a better understanding of this in-triguing effect

4 Summary and conclusion To summarize, we

pre-sent an EB system exhibiting a double-shifted loop, which results from the overlap of the two oppositely biased loops The angular and temperature dependences are consistent with this argument An abnormal training effect is qualita-tively explained using this assumption We believe that the present results will be useful for understanding the

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mecha-nism of some peculiar effects associated with exchange

bias

AcknowledgementsWe thank Dr Givord and Dr

Demp-sey from the Laboratory Louis Néel for their kind experimental

supports and stimulating discussions This work is supported by

the State Programs on Fundamental Research of Vietnam under

the Grants 4.049.06 and 4.105.06

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