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In this material, a converse magnetoelectric effect and especially, an electric field-induced magnetic anisotropy and magnetization switching process have been observed at the changing s

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Electrical Field-Induced Magnetization Switching

in CoFe/NiFe/PZT Multiferroics

Nguyen Thi Minh Hong1, Pham Thai Ha1, Le Viet Cuong1, P T Long2, and Pham Duc Thang1,3,4

1Faculty of Engineering Physics and Nanotechnology and Laboratory for Micro and Nanotechnology,

University of Engineering and Technology, Vietnam National University, Hanoi 10000, Vietnam

2Department of Physics, Chungbuk National University, Cheongju 361-763, Korea

3UNESCO UNISA Africa Chair in Nanosciences and Nanotechnology, College of Graduate Studies, University of South Africa, Pretoria 0002, South Africa

4Nanosciences African Network, iThemba LABS-National Research Foundation of South Africa,

Pretoria 0001, South Africa

In this paper, we have investigated the change in magnetization of multiferroic material, based on magnetic nanostructured CoFe/NiFe film grown on the piezoelectric lead zirconate titanate (PZT), under the effect of the strain originated from PZT layer.

In this material, a converse magnetoelectric effect and especially, an electric field-induced magnetic anisotropy and magnetization switching process have been observed at the changing stages of applied electric voltage In addition, a significant relative change in magnetization, above 100%, is obtained, which facilitates practical applications of the materials This opens possibilities in achieving new types of memory devices, the low energy consumption devices, as well as other functionalities, such as voltage-tunable field sensing A simple theory based on strain-mediated magnetic-electric coupling is also presented to understand the origin of the change in magnetic properties of the materials.

Index Terms— Ferroelectrics, ferromagnetics, magnetization switching, multiferroics.

I INTRODUCTION

MULTIFERROIC materials in which magnetic and

ferroelectric orders coexist have emerged as one of

the promising materials for multifunctional applications in

data storage, field sensors, and next generation spintronic

devices, owing to the advantageous possibility of controlling

the magnetic state via the electric fields and vice versa

[1]–[3] Recently, the research interests have been focused

on the converse magnetoelectric (CME) effect and

magnetiza-tion (M) switching by electric field (E) in multiferroics thanks

to its potential application for new types of memory devices

and low energy consumption devices [4], [5] The physical

nature of electric-magnetic couplings is also of great interest

but has not been thoroughly explored

There are various ways to change magnetic anisotropy

of magnetic films One of the conventional methods is by

changing deposition conditions, e.g., substrate temperature,

gas pressure, and so on A new approach recently applied

for multilayered films is to use a multiferroic structure, in

which the magnetic properties can be tuned by an applied

electric voltage In the previous works, we reported the

finding of the CME effect and the electric-voltage-controlled

magnetic anisotropy in new CoFe/NiFe/piezoelectric lead

zir-conate titanate (PZT) heterostructured nanocomposites [6]–[8]

Interestingly, we observed the switching of the magnetization

at a suitably applied electric voltage

Manuscript received November 22, 2013; revised January 20, 2014;

accepted January 28, 2014 Date of current version June 6, 2014

Corre-sponding author: N T M Hong (e-mail: hongntm@vnu.edu.vn).

Color versions of one or more of the figures in this paper are available

online at http://ieeexplore.ieee.org.

Digital Object Identifier 10.1109/TMAG.2014.2304518

This paper aims to investigate the change in magnetization

of nanostructured CoFe/NiFe/PZT multiferroics, induced by the presence of a stress originated from transverse polarized PZT piezoelectric layer In addition, we present a theoretical study on the CME effect and electric field-induced magnetiza-tion switching, the role of ferromagnetic layer thickness, and bias magnetic field on the magnetization switching process in this material

II EXPERIMENT NiFe and CoFe magnetic layers were magnetron sputtered

in sequence on commercial 500-μm-thick PZT piezoelectric

substrate having transverse polarization (APC-855, American Piezoceramics Inc.) A base pressure of 2× 10−7 torr was achieved prior to the deposition The deposition process was performed at room temperature in an argon gas environment

with a pressure ( pAr) of 2.2 mtorr and at a power of 50 W.

In this CoFe/NiFe/PZT multiferroic structure, the thickness

of CoFe layer is fixed at 190 nm The total thickness of NiFe/CoFe layers was changed from 200 to 280 nm These

samples are noted as S1, S2, S3, and S4, respectively Finally,

a Ta thin layer was sputtered on the top of the samples to prevent oxidization for ferromagnetic layers

Magnetic hysteresis loops, M (H ), were measured using

a vibrating sample magnetometer (VSM) 7400 (Lakeshore)

with the magnetic field (H ) applied in the film plane and

normal to the film plane For the CME effect measurement, the electrodes, having the size of 5× 0.5 mm2, are placed on two sides of transverse polarized PZT substrates by using silver adhesive glue (Fig 1) The CME measurement was performed using the VSM on 5× 5 mm2 sample, placed in a varied 0018-9464 © 2014 IEEE Personal use is permitted, but republication/redistribution requires IEEE permission.

See http://www.ieee.org/publications_standards/publications/rights/index.html for more information.

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Fig 1 Experimental setup of CoFe/NiFe/PZT multiferroics for CME

measurement.

external bias magnetic field (Hbias) and an applied electric

voltage (V ) ranged from −400 to 400 V

III RESULTS ANDDISCUSSION

For the samples S1, S2, S3, and S4, magnetic hysteresis

loops have been measured at room temperature and at

various anglesα = 0° and 90° in which α is the angle between

the film plane direction and the external bias magnetic field

direction The results, not shown here, indicate that in-plane

magnetic anisotropy dominates for all multiferroic samples

due to the magnetic anisotropic contribution of NiFe and

CoFe ferromagnetic layers The magnetization change as a

function of voltage applied along the PZT substrates, M (V ),

measured at various bias magnetic field Hbias= 0, ±50, ±100,

±1000 Oe aligned parallel to sample plane (α = 0°), are

shown in Fig 2

The results point out an almost linear dependence of

mag-netization M on voltage V for all samples Under applied

electric voltage, PZT substrate is elongated in the film plane

and the strain in PZT substrate leads to a strain in NiFe/CoFe

layers Consequently, this alters the magnetic anisotropy of

the magnetic layers via magnetoelastic coupling It indicates

that the elastic stress transfers from PZT piezoelectric phase to

NiFe/CoFe magnetic phase In this effect, the magnetoelastic

energy associated with coupling between the stress and the

magnetization and stress anisotropy field H σ can be formed

in the NiFe/CoFe In this case, the elastic stress associates

with magnetization of magnetostrictive materials and thus, the

stress anisotropy can be induced [9] The change in

magne-tization, M/M, measured at α = 0° and Hbias = −50 Oe

under a voltage ranged from 0 to 400 V is larger than 100%

We observe a maximum valueM/M of 138% for the sample

S2 (corresponding to M = 550 μemu).

The strength of the stress anisotropy is dependent on the

product of the saturation magnetostriction of ferromagnetic

materials λ S and the applied stress σ, namely λ S σ [10].

In the theoretical model, the orientations of magnetization

are defined by the competition between the stress anisotropy

field H σ and magnetocrystalline anisotropy field HK We

con-sider first the magnetoelastic energy which is given by

Eme = K σsin2θ where the stress anisotropy constant Kme

is expressed as K σ = (3/2)λ S σ Apparently, K σ > 0 favors

θ = 0° where the magnetization is parallel to the stress

axis Contrary, K σ < 0 favors perpendicular alignment of the

magnetization (θ = 90°) This means that when the absolute

values of the stress anisotropy constant K σ are larger than the

magnetocrystalline anisotropy constant K1, the magnetization will be aligned along the easy direction determined by the stress anisotropy For the studied samples, PZT substrate has transverse polarization and NiFe/CoFe layers have in-plane magnetic anisotropy, which means the parallel alignment of

magnetization is relative to the stress axis, thus K σ > 0

Mean-while NiFe/CoFe layers have the magnetostriction coefficient

λ S > 0, therefore σ > 0 indicates that the stress in those

layers is tensile This is in accordance with the above results

of increasing M with changing V

On further investigation on the dependence of M on var-ied V , one can observe the electric field-induced switching of

magnetization which occurs at certain applied voltage, called

the magnetization reversed voltage Vrev (as shown in Fig 3)

At this voltage, large strains produced in PZT can transfer

to NiFe/CoFe and induce a change in the orientations of the magnetization, i.e., in the magnetic anisotropy This allows us

to control magnetization switching by using an electric field instead of a traditional magnetic field At the same magnetic

field Hbias, Vrev decreases with increasing the thickness of NiFe

In this paper, the thickness of ferromagnetic layer CoFe has been reduced to 190 nm in comparison to that in the previous works [7] Consequently, the results show a decrease

of Vrev from −500 to −75 V at the same bias magnetic field of 5 Oe This finding is interesting since it reduces the consumption energy in the applications Hence, these multifer-roic structures CoFe/NiFe/PZT have a promising application

for future spintronic devices For sample S3 especially, the electric field-induced magnetization switching can be achieved

at Vrev = −70 V without Hbias The magnetization state can

be controlled by an external voltage, even without the use of a bias magnetic field This opens a possibility for application of CME devices with size reduction and exclusion of interference effect from electromagnet or permanent magnet [11]

In order to provide more explanations to the field-induced magnetization switching phenomenon, the voltage-induced magnetic susceptibilityχ was derived from M(V ) data, taken

at various magnetic field Hbias = −50, −100, −200, −500, and−2000 Oe and shown in Fig 3 for one typical sample S1

As can be seen from Fig 4, first, χ has a negative value

at high applied voltage When decreasing applied voltage,

χ decreases to a minimum, increases then cancels at fixed voltage (Vrev) and finally changes in sign One observes that the higher Hbiasis, the higher Vrevrequires At high magnetic field, the magnetization rotates progressively from easy axis

to the field direction In this state, a much higher energy is

necessary to switch magnetization and therefore, Vrevincreases

with increasing Hbias Once magnetization is aligned along the direction of the magnetic field, magnetization switching process no longer occurs andχ approaches to zero In general,

magnetization switching can be decided by the competition between the magnetic field energy and applied electric field energy

In addition to considering the magnetization changes of samples as a function of applied voltages at various magnetic

fields, we also observed the difference of M value measured

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Fig 2. Magnetization M as a function of applied voltage V measured at various magnetic fields at angle α = 0°.

Fig 3. Magnetization reversed voltage value (Vrev ) for samples measured

at various magnetic fields.

at various angles α (Table I) The results show that the

dependence M (V ) still has a virtually linear increase as we

increase the applied voltage on PZT substrate However, the

change in magnetization decreases gradually when magnetic

field direction deviates from the film plane direction Notably,

this change is very small atα = 90° and even Vrevcan achieve

a voltage as small as 0.5 V for sample S3 at magnetic field

Fig 4 Voltage dependence of magnetic susceptibilityχ for sample S1

These obtained results can be explained based on the magnetization process which is described by the model for different orientations of applied magnetic fields Atα = 0°,

magnetization and magnetic field direction are parallel together (having in-plane magnetic anisotropy) Thus, mag-netization switching process requires much more electric field energy to rotate magnetization in the reverse direction On the other hand, when α = 90°, smaller voltage is needed to

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TABLE I

V ALUE OFVrev FOR S AMPLES M EASURED AT V ARIOUS

A NGLEαAND ATHbias = −100 Oe

reverse magnetization from the initial state to the orientation

of applied magnetic field Thus, the rotation of magnetization

toward applied magnetic field direction leads to a vantage of

energy, causing the decrease of Vrev value

IV CONCLUSION The magnetic properties, including CME effect and electric

field-induced magnetization, of nanostructured multiferroic

CoFe/NiFe/PZT films have been studied Under the strain

originated from PZT piezoelectric layer in the presence of the

external electric voltage, induced switching of magnetization

and magnetic anisotropy have been observed This opens

possibilities in achieving new types of memory devices, low

energy consumption devices, as well as other functionalities,

such as voltage-tunable field sensing

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