Front. Phys.

, 2012, 7(4): 380385

DOI 10.1007/s11467-012-0266-8

PERSPECTIVE
Multiferroic tunnel junctions
Yue-Wei Yin1,2 , Muralikrishna Raju1 , Wei-Jin Hu1,3 , Xiao-Jun Weng4 , Ke Zou1 , Jun Zhu1 ,
Xiao-Guang Li2 , Zhi-Dong Zhang3 , Qi Li1,
1 Department
2 Hefei

of Physics, Pennsylvania State University, University Park, PA 16802, USA

National Laboratory for Physical Sciences at Microscale, Department of Physics, University of Science and
Technology of China, Hefei 230026, China

3 Shenyang

National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences,
Shenyang 110016, China

4 Department

of Materials Science and Engineering, Materials Research Institute, Pennsylvania State University,
University Park, PA 16802, USA
E-mail: qil1@psu.edu
Received July 10, 2012; accepted July 24, 2012

Magnetic tunnel junctions with ferroelectric barriers, often referred to as multiferroic tunnel junctions, have been proposed recently to display new functionalities and new device concepts. One of
the notable predictions is that the combination of two charge polarizing states and the parallel and
antiparallel magnetic states could make it a four resistance state device. We have recently studied
the ferroelectric tunneling using a scanning probe technique and multiferroic tunnel junctions using
ferromagnetic La0.7 Ca0.3 MnO3 and La0.7 Sr0.3 MnO3 as the electrodes and ferroelectric (Ba, Sr)TiO3
as the barrier in trilayer planner junctions. We show that very thin (Ba, Sr)TiO3 lms can sustain
ferroelectricity up till room temperature. The multiferroic tunnel junctions show four resistance
states as predicted and can operate at room temperatures.
Keywords multiferroic tunnel junction, ferroelectric lm, tunneling magnetoresistance eect, tunneling electroresisitance eect, magnetoelectric coupling
PACS numbers 75.85.+t, 77.55.fe, 75.70.Cn, 75.60.Ej, 77.80.Fm

1 Introduction
The demands for faster, smaller, and non-volatile electronics have pushed the limit of semiconductor devices to
ever smaller dimensions. However, the challenge of power
dissipation places a limit on the future device scaling. In
addition, size eects may also post constraint on device
miniaturization. These have led to an emergent need and
development of new concepts for information processing
and storage [1, 2]. For the next generation devices, multifunctional structures have been envisioned, which can
perform new functionality, can be manipulated by several
external independent controls, and can operate with low
power [3, 4]. One of the approaches to multi-functional
devices is to combine ferromagnetic (FM) based spintronics with ferroelectric (FE) based functionality [3, 4].
It can be used as memory cells with multiple resistance
states or to combine logic and memory operations. It

may also be able to achieve cross control of the spin and

charge degrees of freedom. This oers signicant opportunities for new device concepts.
Magnetic tunnel junctions (MTJs) is the most widely
used spintronic device in computer read heads, sensors,
and memories [5]. The parallel and antiparallel magnetization alignments of the two electrodes represent two
logic states with dierent resistances (tunneling magnetoresistance, TMR). Ferroelectric tunneling refers to a
tunnel junction using a ferroelectric as the barrier. The
basic idea of an FTJ was raised by Esaki et al. [6] decades
ago. However, it only aroused considerable research interest recently, largely because only in recent years experiments [79] have shown that ferroelectricity can persist
down to the nanometer scale. This makes it possible to
use ferroelectrics as tunneling barriers. The key property
of an FTJ is the switching of junction resistance with the
reversal of ferroelectric polarization, namely, tunneling
electroresistance (TER) eect. As reviewed by Tsymbal

c Higher Education Press and Springer-Verlag Berlin Heidelberg 2012



Yue-Wei Yin, et al., Front. Phys., 2012, 7(4)

et al. [10], the TER eect of an FTJ could at least be

obtained through the following three eects: i) electrostatic eect which will change the depolarization potential through the asymmetrical screening of the two interfaces of the barrier [11]; ii) asymmetrical interface atomic
arrangement that will inuence the transmission probability by the ferroelectric ionic displacement at interfaces
[12]; and iii) strain eect which will aect the barrier
width due to the piezoelectricity eect [13]. Very recently
large TER eect tested using a scanning probe technique
has been reported on BaTiO3 [1416] and PbZrx Ti1x O3
[17, 18] ferroelectric lms.
Combining a magnetic tunnel junction with a ferroelectric barrier, i.e., a multiferroic tunnel junctions
(MFTJs), will add new functionality beyond the single
MTJs or FTJs. The junction resistance will be sensitive to not only the magnetization alignment of the electrodes, but also the polarization direction of the barrier. This makes MFTJ a quaternary-state device which
can be switched by both electric and magnetic elds.
Theoretical calculations on SrRuO3 /BaTiO3 /SrRuO3
structure have predicted [19] about 50% resistance
dierences between the two polarization states, making the MFTJ a practically useful device. Moreover,
due to the mechanical coupling [20], chemical bonding
[21] or spin dependent screening [22] at the ferromagnetic/ferroelectric interfaces, these articial composites
of ferroic materials may enable the magnetoelectric coupling eect (as reviewed by [3, 4, 2326]), making it possible to control magnetization by electric eld or control
electric polarization by magnetic eld.
The rst reported MFTJ is another type of MFTJ
employing a single phase multiferroic La0.1 Bi0.9 MnO3
barrier in a Au/La2/3 Sr1/3 MnO3 junction where the
TMR is due to the spin ltering eect and the TER
is related to the barrier potential change when polarization is reversed [27]. Recently, by using a Fe indentation technique, Garcia et al. have fabricated the
nanoscale Fe (or Co)/BaTiO3/La0.7 Sr0.3 MnO3 ferroelectric/ferromagnetic/ferroelectric MFTJs and reported the
control of carrier spin polarization by electrically reversing the ferroelectric polarization [28, 29]. Moreover, not only the magnitude, but also the signs of
the TMR can be inverted by ferroelectric switching in
Co/PbZr0.2Ti0.8 O3 /La0.7 Sr0.3 MnO3 MFTJs, showing a
new method of spin control in spintronic devices [30].
The four resistance states have also been reported on
all perovskite La0.7 Sr0.3 MnO3 /BiFeO3 /La0.7 Sr0.3 MnO3
MFTJs where BiFeO3 is an intrinsic multiferroic material [31]. However, all of these results showed small magnetoresistance and can work only at low temperatures.
To obtain both TMR and TER eects in a MFTJ, thin
insulating barrier with persistent ferroelectricity and ferromagnetic electrodes with high spin polarization are
critical. Here, we choose (Ba, Sr)TiO3 as ferroelectric

381

barrier which shows ferroelectricity down to one unit

cell under proper strain condition [7] and half metallic
La0.7 Ca0.3 MnO3 (LCMO) and La0.7 Sr0.3 MnO3 (LSMO)
as ferromagnetic electrodes for the proper lattice match
with the barrier [32]. Large TMR and TER eects have
been observed in the LCMO-based MFTJs [33], and in
LSMO-based MFTJs the four resistance states can be
achieved even up to room temperature [34].

2 Experiment
Epitaxial (Ba, Sr)TiO3 /La0.7 Sr0.3 MnO3 bilayers for
piezoresponse force microscopy (PFM) measurements
and La0.7 Ca0.3 MnO3 /(Ba, Sr)TiO3 /La0.7 Ca0.3 MnO3 and
La0.7 Sr0.3 MnO3 /(Ba, Sr)TiO3 /La0.7 Sr0.3 MnO3 trilayers
for MFTJ investigations were grown on SrTiO3 (100)
substrates by pulsed laser deposition. The heterostructures were deposited in situ at 750C in a 300 mTorr
owing oxygen. The laser energy density was about 1.5
J/cm2 . The epitaxial growth of the trilayers on SrTiO3
is revealed by high-resolution transmission electron microscopy (TEM) and the TEM specimens were prepared
using conventional mechanical polishing followed by Ar
ion milling. Cross-sectional scanning TEM (STEM) was
performed in a JEOL-2010F eld-emission TEM/STEM
operated at 200 keV. The ferroelectric property of the
(Ba, Sr) TiO3 ultrathin lms were investigated by PFM
[Asylum Research-MFP-3D atomic probe microscopy
(AFM)].
The micron-scale MFTJ in the cross-strip geometry
was fabricated by using photolithography and Ar ion
milling in a process similar to what we have used before
[35]. Sputtered MgO or SiO2 was used as an insulating
layer to allow making gold contact leads with the top
electrode without shorting to the bottom electrode. The
schematic drawing of the MFTJ structure is illustrated in
Fig. 1(a). A four-probe method was used to do electrical
transport measurement. The positive bias corresponds to
the current ow from top to bottom electrode and the
magnetic eld was applied along the longitudinal direction of the bottom La0.7 Sr0.3 MnO3 lead.

3 Results and discussion

To characterize the structural quality, X-ray diraction
2 and scans as well as high resolution cross sectional STEM have been conducted on selected samples.
X-ray diraction shows that all layers are grown epitaxially. Figure 1(b) is a high-resolution cross-sectional
high-angle annular-dark-eld (HAADF) STEM image of an as-grown La0.7 Ca0.3 MnO3 /Ba0.5 Sr0.5 TiO3 /
La0.7 Ca0.3 MnO3 trilayer. Almost atomically smooth
growth of the Ba0.5 Sr0.5 TiO3 barrier was obtained
even for our relatively thick La0.7 Ca0.3 MnO3 bottom

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Yue-Wei Yin, et al., Front. Phys., 2012, 7(4)

Fig. 1 (a) The schematic diagram of the MFTJ (the

MgO or SiO2 insulating layer between the top and bottom lead is not shown). (b) Cross-sectional HAADF STEM
image of a La0.7 Ca0.3 MnO3 (LCMO)/Ba0.5 Sr0.5 TiO3 (BSTO)/
La0.7 Ca0.3 MnO3 trilayer.

lm (30 nm), indicating high quality heterostructure

growth.
To conrm the ferroelectricity of nanoscale (Ba,
Sr)TiO3 lm, PFM and conducting atomic force microscopy (CAFM) have been performed at room temperature on several (Ba, Sr)TiO3 /La0.7 Sr0.3 MnO3 samples.
As illustrated in Fig. 2(a), these investigations were carried out based on a scanning probe microscopy (Asylum
Research-MFP-3D AFM) using a conductive AFM tip
in contact with the (Ba, Sr)TiO3 surface. Figure 2(b)
shows an out-of-plane PFM phase image at room temperature for a 3.5 nm Ba0.95 Sr0.05 TiO3 thin lm on top
of a 30 nm La0.7 Sr0.3 MnO3 bottom electrode. Here, a
word PSU and the background were written by negative (6.0 V) and positive (+6.0 V) voltages respectively.
The observed PSU pattern indicates the occurrence of
ferroelectric switching. Figure 1(b) shows a local voltage dependence of piezoresponse phase which suggests a
180 phase contrast and provides evidence for ferroelectricity of nanoscale (Ba, Sr)TiO3 lm. The current

(I)voltage (V ) characteristic of this sample have also

been tested by CAFM, as shown in Fig. 3. After polarize the ferroelectricity upward and downward, two obvious dierent IV was observed. At 1 V, a large TER
30 000% was obtained.
In trilayer junction structures, due to the large junction area ( 10 m 10 m) in comparison with the
scanning probe contact area (with a diameter of about
several tens of nanometers), large TER has not been reported presumably due to the weak links and multidomain structures when the ferroelectric barrier is poled to
reverse its directions using a large voltage. In addition,
it was proposed that the large TER observed from the
PFM measurement without the top electrode is due to
the surface absorption of elements which acted as an additional dielectric layer on top of the ferroelectric layer
[36]. By increasing the asymmetry of the junction, the
dielectric layer will serve as a switch changing its barrier height dramatically when the electrostatic potential
is changed by polarization reversal, leading to the giant
TER values in PFM test.
Figure 4(a) shows the non-linear IV characteristic
of a La0.7 Sr0.3 MnO3 /Ba0.95 Sr0.05 TiO3 /La0.7 Sr0.3 MnO3
MFTJ ( 10 m 20 m in area) at room temperature.
The corresponding dierential conductance G = dI/dV
shows a parabolic dependence on bias voltage, as can be
seen in the normalized conductance G(V)/G(0) shown
in the inset of Fig. 4(a). As indicated by the solid line in
the inset of Fig. 4(a), the good tting of the conductance
curve with Brinkman model [37] indicates that the electron tunneling dominates the transport process. Figure
4(b) shows potential diagrams drew based on the tting
parameters, the barrier thickness (d), average barrier
height ()
and the asymmetry in the barrier () for the
curves with the barrier polarized downward and upward
(with a poling voltage of Vpulse +1.4 V or 1.4 V). The
dierences between the barrier parameters after poling
the ferroelectricity down or up suggest that the ferroelectricity can aect the electron transport properties of
MFTJ, which will result in the TER eect. Similar to the
theoretical prediction [19], the TER eect may be caused
by the asymmetric Ba0.95 Sr0.05 TiO3 /La0.7 Sr0.3 MnO3
interface which will induce asymmetric ferroelectric
displacements in the barrier and lead to a change in

Fig. 2 (a) A shematic drawing of PFM and CAFM measurement setup. (b) Out of plane PFM phase image and (c) local
PFM phase as a function of bias voltage of a 3.5 nm Ba0.95 Sr0.05 TiO3 lm on 30 nm La0.7 Sr0.3 MnO3 electrode.

Yue-Wei Yin, et al., Front. Phys., 2012, 7(4)

383

blue dots means that the switching was observed between

parallel and antiparallel magnetic states [reached by R
H sweep (see Fig. 6)], respectively. Hence, after applying positive and negative voltages, two parallel and two
antiparallel states i.e. a distinct four-state device was
represented.

Fig. 3 IV characteristics measured by CAFM on a

Ba0.95 Sr0.05 TiO3 /La0.7 Sr0.3 MnO3 sample. Arrows indicate the
orientation of ferroelectricity.

Fig. 5 In response to (a) the applied voltage pulses, (b)

switching of the junction resistance (measured at 10 A) for
a La0.7 Sr0.3 MnO3 /Ba0.95 Sr0.05 TiO3 /La0.7 Sr0.3 MnO3 MFTJ at
parallel (red) and antiparallel (blue) states.

Fig. 4 (a) IV curve of a La0.7 Sr0.3 MnO3 /Ba0.95 Sr0.05 TiO3 /

La0.7 Sr0.3 MnO3 MFTJ. Inset: Bias dependence of the normalized
dynamics conductance calculated from the IV curve (round dots)
and tting results by Brinkman model (solid line). (b) The barrier potential diagrams of the MFTJ with ferroelectric polarization
upward and downward.

complex band structure in Ba0.95 Sr0.05 TiO3 . Moreover,

although 1.4 V was used as poling voltages, we do
not have direct evidence that the voltage is enough to
completely poling the ferroelectric layer. Therefore, other
switching mechanisms like the interfacial electrochemical
modication by electric eld may also take responsibility
for the results [3840]. More work is being carried on to
understand the underlying mechanism.
Figure 5 shows that, by reversing the barrier polarization repeatedly, the junction resistances measured at
10 A bias between the two polarization states can be
switched between each other directly. Here, the red and

Fig. 6 R vs. H of the La0.7 Sr0.3 MnO3 /Ba0.95 Sr0.05 TiO3 /

La0.7 Sr0.3 MnO3 MFTJ measured at 10 mV and 280 K after poling the ferroelectricity upward (red) and downward (blue). The
horizontal arrows indicate the directions of the electrode magnetization and the vertical arrows indicate the directions of the barrier
polarization.

Figure 6(a) shows the magnetic eld (H) dependence

of the junction resistance (R) at a xed voltage bias

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Yue-Wei Yin, et al., Front. Phys., 2012, 7(4)

of 10 mV after aligning the ferroelectric polarization of

Ba0.95 Sr0.05 TiO3 barrier downward or upward. A sharp
resistance change against the magnetic eld is observed
between two magnetic states (parallel and antiparallel),
suggesting an almost entire ip of the magnetic domains.
After reversing the polarization of barrier, the entire R
H curve shifts so that both parallel and antiparallel resistances switched to dierent values and four resistance
states were observed. Figure 6(b) shows two resistance
memory loops (measured at 10 mV) as a function of
magnetic eld for the two polarization states. A standard
MTJ memory loop with two states (parallel and antiparallel) is obtained for both polarization states and it can
be switched between two states by sweeping magnetic
eld. Similar to the RH loops in Fig. 6(a), the resistance can be switched from one memory loop to aother
by reversing the ferroelectricity of the barrier. It is worth
mentioning that, from Fig. 6(b), the four states can be
observed at zero magnetic and electric eld, which means
that the memory device is non-volatile.
Larger TER and TMR eect (up to 300%) can
be obtained at lower temperatures in the trilayer
junctions [33]. Figure 7 shows the RVp loops of
a
La0.7 Ca0.3 MnO3 /Ba0.5 Sr0.5 TiO3 /La0.7 Ca0.3 MnO3
MFTJ ( 8 m 8 m in area) in parallel magnetization
state at 4.2 K. Here, each data point in the hysteresis
loop is tested at a xed voltage bias [0.1 V for Fig. 7(a),
0.15 V for Fig. 7(b)] after pulsing a voltage. The TER
values decreases from 45 % to 22 % with the increasing
bias from 0.1 V to 0.15 V, and are all higher than
the TER at room temperature shown in Figs. 5 and 6
(2%) which are tested at even lower bias. The junction
resistance changes when the polarization was switched

by external voltage pulses and saturates afterward, indicating the coercive eld for the polarization reversal should be reached. The switching voltage is slightly
asymmetric, possibly due to the imprint of the ferroelectric layer.

4 Conclusions
In conclusion, we have fabricated all-oxide multiferroic
tunnel junctions by pulsed laser deposition technique.
Four distinct resistance states with large resistance differentials have been obtained and the device can operate
at room temperatures. Using scanning probe technique,
much larger TER eect can be obtained than that of
the large size planner trilayer tunnel junctions. Further
study on the origins of the dierences should be conducted so that larger TER eect can also be obtained
in trilayer junctions, which can be used in practical devices. These results pave the way for new multilevel and
nonvolatile devices.
Acknowledgements The work was supported in part by DOE
DE-FG02-08ER4653 (QL), NSF DMR-1207474 (QL), Penn State
MRSEC seed grant (QL), and NBRP-2012CB922003 (XL), and
NSFC-50831006 (ZZ).

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