Thin Solid Films 583 (2015) 9194

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Thin Solid Films

journal homepage: www.elsevier.com/locate/tsf

Strong spintronic magnetoelectric effect in layered

magnetic metamaterial
P.V. Pyshkin a,b,, A.V. Yanovsky a
a
b

B.Verkin Institute for Low Temperature Physics & Engineering, National Academy of Sciences of Ukraine, 47 Lenin Ave, 61103 Kharkov, Ukraine
Department of Theoretical Physics and History of Science, The Basque Country University (EHU/UPV), PO Box 644, 48080 Bilbao, Spain

a r t i c l e

i n f o

Article history:
Received 22 September 2014
Received in revised form 21 March 2015
Accepted 23 March 2015
Available online 30 March 2015
Keywords:
Metamaterial
Multiferroics
Magnetoelectric effect

a b s t r a c t
It is shown that external magnetic eld or magnetization induces electric polarization of microscopic isolated
magnetic/non-magnetic hybrid structures due to the spin-dependent electron redistribution and mutual capacity.
The magnetoelectric effect can be very strong, for instance the change of electric polarization reaches 100 C/m2
at a constant magnetic eld of only 1.5 T in the case of 100 10 nm structures which tightly ll the space,
composing a metamaterial. The effect does not require using exotic compounds. Based on the obtained results
we suggest a number of recommendations for future experimental design.
2015 Elsevier B.V. All rights reserved.

Spin electronics (spintronics) has been already used in data storage

and other devices. Advantages and physical principles of utilizing the
spin of the charge carriers in electronics are widely discussed, see e.g. recent reviews [1,2] and the Nobel lectures of the 2007 [3,4]. In this article
we show that spintronic materials could manifest unique properties due
to proximity between small magnetic/non-magnetic hybrid structures.
The magnetic/non-magnetic hybrid structures [5] are important
subject of study in spintronics. Here the word non-magnetic refers
to non-magnetic metal or semiconductor, such as Cu or GaAs. And the
term magnetic means magnetic conductors, e.g. the ferromagnetic
metals (Fe, Co), or some paramagnetic metals which are close to ferromagnetic instability (Pd), or the diluted magnetic semiconductors
(Ga1 xMnxAs, Zn1 xBexSe) etc. It is well known [6] that magnetization
induces the giant Zeeman spin splitting of the conduction band in such
magnetic conductors due to the strong exchange interaction depending
on the electron spin direction versus the magnetization axis. As is the convention, the appropriate spin bands are denoted hereinafter by the indices for spin-up or for spin-down.
The giant Zeeman splitting signicantly changes the spin density of
states (DOS) of the conduction electrons. It affects all the spin components of the physical parameters related to the DOS resulting giant magnetic resistance effect [3,4,7], spin-aligning [8] etc. Lots of magnetically
inhomogeneous spintronic devices [1] are proposed as parts of an
electrical circuit: the spin-valve [9], Datta and Dass transistor [10,11],
and other spin transistors [1215].
Corresponding author at: B.Verkin Institute for Low Temperature Physics & Engineering,
National Academy of Sciences of Ukraine, 47 Lenin Ave, 61103 Kharkov, Ukraine.
E-mail address: pavel.pyshkin@gmail.com (P.V. Pyshkin).

http://dx.doi.org/10.1016/j.tsf.2015.03.056
0040-6090/ 2015 Elsevier B.V. All rights reserved.

In contrast, we discuss the equilibrium states of isolated conducting

magnetic/non-magnetic structures after spin relaxation (i) with and
(ii) without external magnetic eld and show that heterogeneity of
spin , bands could be used to design articial materials that display
strong magnetoelectric (ME) effect.
We discuss direct ME effect: the induction of an electric polarization
by a magnetic eld, see e.g. books [16,17] and reviews [1822]. The
inverse effect will be considered elsewhere. At present, ME effects
have attracted great interest for lots of applications: sensors, information storage, anti-radar coating [23] and others [18]. The conventional
ME effect arises from interaction of electric and magnetic subsystems
in time-asymmetric ionic crystals or piezoelectric and magnetic
subsystems in composite multiferroics [24].
From applied point of view, linear ME effect has special importance
[18,23]. But also it requires specic efforts from fundamental point of
view because the magnetic eld is a pseudo vector, and electric polarization is a vector. So the linear effect in conventional multiferroics is
only possible for a special asymmetry, e.g. in multi-sublattice insulators
with rare-earth elements. As it is shown below, the spintronics provides
linear ME effect with high accuracy due to transfer of conduction
electrons, which are absent in dielectric multiferroics.
In most experiments (see e.g. Ref. [25,26]), the value of the ME effect
is 10 100 C/m2 at a magnetic eld of 3 T or more, giant ME effect is
3600 C/m2 at 7 T [27] with the same 10 100 C/m2 at 2 T. Also
giant ME effect is induced by a weak ac magnetic eld oscillating in
the presence of a strong dc bias eld due to an interaction of magnetostrictive and piezoelectric subsystems in the vicinity of electromechanical resonances in composites like for example PZT/Terfenol-D laminate,
see e.g. [28,20,29,30]. As compared with these composite systems and

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P.V. Pyshkin, A.V. Yanovsky / Thin Solid Films 583 (2015) 9194

single-phase multiferroics, advantages of the materials proposed in a

given work are considered below in the discussion of the result.
In this paper, the strong ME effect of quite a different nature is
predicted. It is related to the spin-dependent redistribution of free electrons in inhomogeneous magnetic conductive structures embedded
into dielectric matrix, forming a metamaterial (Fig. 1), i.e. nanostructured composite material, cf. for example Ref. [31,32]. In contrast to conventional metamaterials the purpose of this one is to reach high mutual
capacity of meta-atoms (articial atoms) from their closeness.
In the beginning let us consider one meta-atom of the metamaterial.
Then we will show how ME effect occurs and why it increases while
these meta-atoms decrease.
The said meta-atom is a standard object in spintronicsa microsized conductor consisting of two parts: a non-magnetic N and magnetic M. At achievable stationary magnetic elds, the energy of giant
Zeeman splitting of magnetized M-part (electron volts in ferromagnetic
metals) is much larger than one of N -part Zeeman splitting. Therefore,
we will neglect the latter. The equilibrium of isolated meta-atom is
determined by the constancy of the charge carriers' total number and
equality of the electrochemical potentials of the meta-atom's magnetic
and non-magnetic parts.
In equilibrium, the chemical potential level M in M-part is the same
for electrons with different spins due to the spin relaxation. Since the electron DOS N() depends on the energy, the chemical potential M differs
from the chemical potential 0 of the system without a magnetic eld.
Let us analyze M dependence on the magnetization and magnetic eld.
For simplicity, we assume that the temperature is much lower than
Fermi energy and Zeeman splitting energy in M-part such that the
Fermi distribution is replaced by a step function. Change of M in a magnetic eld is considered in [33] and experimentally-conrmed in [34]:

interaction in M-part. Here the Zeeman splitting is:

2IM B H;

where M is the magnetization. From here, the variations of M in

paramagnetic and ferromagnetic materials differ signicantly because
paramagnetic magnetization is proportional to H, while ferromagnetic
material has its own magnetization.
More specically, in the case of paramagnetic material:
para

2
H;
1 B

where a = 2IN b 1 is the dimensionless parameter of exchange

enhancement of the M-part magnetic susceptibility for the paramagnetic
material. When 1 M-part is ferromagnetic (Stoner criterion [35]), the
expression (3) is not applicable, and
ferro 2IM

does not depend on the external magnetic eld in the main approximation by H.
Using (1)(4) we obtain the following expression for the chemical
potential variation in the case of the ferromagnetic M-part ( N 1):
ferro H

g B H X
;
2 1

where X = (N N)(N + N)1 refers to spin polarization of DOS at

the Fermi level. And for the case of paramagnetic M-part with exchange
enhancement ( b 1), we obtain:
2

1
N1
N

d M
;


dg B H 2 N 1 N1 4I

para H
1

where g is the electronic g-factor, B is the Bohr magneton, H is the

external magnetic eld; N = N( 0 + /2) and N = N( 0 /2) are
the electron DOS of the corresponding spin subbands at the Fermi
level in the rigid band approximation, N() is the electron DOS (per
one spin) in the absence of the Zeeman splitting, and I refers to Stoner
parameter characterizing the magnitude of the electron exchange

Fig. 1. The metamaterial consisting of a two-layer plates magnet/non-magnet (light/dark

in the picture) in a dielectric matrix (not shown in the picture).

g B N F
2
H ;
41 2 N F

where N(F) is the rst derivative of the DOS with respect to the energy
at Fermi level. Thus, the chemical potential change for paramagnetic M
is H2, while it is linear for ferromagnetic M, both far from the ferromagnetic transition with H. Also it is nonlinear and huge ( IM) at
crossing the transition with H.
Under equilibrium condition, the electrochemical potentials of M
and N parts of the meta-atom are equal, as has been said, for times
longer than electron spin relaxation time. Because of non zero M ,
the electrochemical potentials equilibrate by the transfer of electrons
between the N and M parts (transfer direction is determined by the
sign of M ). Now let's see what happens in a metamaterial which
consists of these meta-atoms.
For simplicity, we consider a chain of identically oriented MN metaatoms (Fig. 2(a)), separated by the insulatorI. The results for such a quasione-dimensional system are extended to three-dimensional systems.
As noted above, the appearance of M induces the redistribution of
charge carriers and subsequently the formation of an electric potential
difference between M and N pieces [36]. This effect can be regarded
as magneto-contact potential difference, i.e. a part of the contact potential difference [37] that depends on magnetic eld. So the electric
charges appear at the interfaces M=N , M/I , and N =I . Thus the chain
can be represented as an equivalent electrical circuit shown in
Fig. 2(c). In this gure, the MN I chain is a series of the two alternating capacities: C MN is the capacity of M=N interface and C N I M is the
capacity of N =I=M interface. The difference in electron chemical potential from change of a magnetic eld is represented as power sources
with the voltage of U = e1 connected to each of MN capacitances.
It can be seen from the Fig. 2(c) that the extra charges are concentrated at the M=N and N =I =M interfaces. They are proportional to
the capacity of the interfaces: qMN UC MN , qN I M C N IM because
of the potential equality for the interconnected plates of C MN and
C N IM . The electric potential as function of coordinate is shown

P.V. Pyshkin, A.V. Yanovsky / Thin Solid Films 583 (2015) 9194

93

Cu/Fe/BaTiO3

Fig. 3. The metamaterial Cu/Fe/BaTiO3 electric polarization dependence on the external

magnetic eld. Dashed line: l + w = 106 cm; solid line: l + w = 3 106 cm; dotted
line: l + w = 105 cm. For comparison, the values of ferroelectric polarization of
known multiferroics were added: Mn0.95Co0.05WO4 from [25] (triangles) and CuBr2 from
[26] (circles).
Fig. 2. (a) Metamaterial is represented by MN I chain, (b) electrical potential for b 0,
and (c) equivalent circuit.

at Fig. 2(b). Using the formula for a at capacitor, we get: C N I M

S=4w, C N M S=4a, where is the permittivity of I , and S is a
cross-section, w is the distance between MN meta-atoms, and a is a
distance of charge separation on M=N interface (of the order of screening length). The process of spatial separation of a charge results in
appearance of the electric polarization [38]:
P

1
V cell

Z
dV j;

dt
V cell

where Vcell is the volume of elementary cell and j is a density of current

in charge redistribution and insulator polarization processes. Thus,
using (7) we obtain that the external magnetic eld induces an electric
polarization:
P H H

1
:
2ew l

So this is the ME effect. Here 0 b b 1 is the dimensionless coefcient

of the packing density of the chains in the dielectric matrix. As can be seen,
the direction of the electric polarization vector depends only on the relative position of M=N structures in it, but not on the direction of the applied magnetic eld. Also, as can be seen from (8) polarization will
increase when dielectric permittivity of I increases, the size of M=N
structures decreases, and when they are located more compactly. Additionally, the expression (8) does not include parameters of material N .
This is due to the fact that the calculation does not take into account
changes of the Fermi level by lling the electron quantum states. This correction is necessary only for extremely small meta-atoms (of the order of
several interatomic distances). Note that it is the permittivity 1 that
makes nonzero electric polarization. Otherwise only net quadrupole will
be created. So, insulator 1 breaks the symmetry in charge redistribution, also it distinctly contributes to the total dipole moment.
The linear ME effect calculated by (8) and (5) is shown in Fig. 3 for
different thicknesses of N =M=I layers and the following parameters:
M-layer is Fe, N -layer is Cu, and insulatorbarium titanate (BaTiO3)
[39] with = 1400; we set 0:5 , single multilayer thickness
l + w = 10 6 cm for dashed line, 3 10 6 cm for solid line, and
10 5 cm for dotted line. As the graphs show, the magnitude of P for
submicron structures comes up to tens of C/m2 that is comparable

with results Ref. [25,26], and is obtained in quite a low magnetic eld.
The nanostructures (about 10 nm) are even better and the corresponding
polarization is about hundreds of C/m2 at the same magnetic eld. It is
obvious from (8) that the P can be increased by using the dielectric with
a greater , such as the copolymers, ceramics, etc., or nonstationary
nonintrinsic colossal , see e.g. [40] and references in it. Due to timedependent nature of the non-intrinsic colossal , we have not discussed
the inuence of amplifying effects like spin-electric effect, spin-charge
oscillation and corresponding resonances [41,42] as well as other accompanying effects, such as electric inhomogeneity, large energy dissipation
and leakage currents. We will address this important and complex question elsewhere.
It is also worth noting that the spintronic materials can provide a
record colossal value of ME effect even for 1: one needs M so that
the H would cross the critical magnetic eld point in the selected range
of magnetic eld for the specic method of fabrication and environmental
conditions. The similar transitions are used to gain colossal magnetic resistance induced by applied magnetic eld [4346]. The change of the
electrochemical potential during the transition is of the order of Stoner
parameter, that is of the order of an electron volt depending on the substance. This can lead to enormous electric elds even in the case of conventional dielectrics P ( 1)I/(d + w), that corresponds to the
eld 105 106V/cm and a record ME effect respectively.
If the M-layer is paramagnetic with a strong exchange gain (e.g. Pd),
the dependence of the electric polarization H, according to (6), (8) is
quadratic and can be enhanced using M-s which are close to satisfaction of the Stoner criterion of ferromagnetism and have a strong DOS
dependence on the energy near Fermi level:

dN 
N F
>>
:
d  F
F
In summary, we have substantiated that metamaterial consisting of
oriented isolated inhomogeneous magnetic conductors can exhibit
strong (regarding known range of ME effect) electric polarization response on a magnetic eld. It is interesting that the polarization direction is determined by location and orientation of the N M structures
in the material. This feature allows to separate predicted effect even
from other ME effects that can be imposed, in particular, if the intrinsic
ME coupling is present in insulator I. In such a case we propose changing the sample orientation relative to the external magnetic eld in the
measurements.

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P.V. Pyshkin, A.V. Yanovsky / Thin Solid Films 583 (2015) 9194

It has been shown that linear ME effect occurs when M-part of

meta-atoms is ferromagnetic. As indicated above, the linear ME effect
is interesting in that H is a pseudo vector, and P is a vector. In our effect
P is composed of the true scalar (average energy of the electron magnetic moment in magnetic eld) and true vector (the direction of electron
transfer during the equilibration). The accuracy of the linear behavior is
very high because it's determined by /F 103 104. In view of
this and above, the proposed material could compete with PZT/
Terfenol-D laminate composites being promising in the higher static
magnetic eld providing high degree of linearity of P(H) in much
wider range of H that is important for application [20].
In the case of the paramagnetic M-parts, ME effect is quadratic in H.
In particular, it can be detected by a frequency-doubled response to a
variable magnetic eld. Here we have applied equilibrium approach. It
is valid for quasi-static magnetic eld when the characteristic frequency
is less than the reverse time of the nuclear and electron spin relaxation
(109 1012 sec1). The results of the study in variable electromagnetic
elds of higher frequency will be published later.
Notice one more application of the effect. Since the magnetized state
is preserved after ferromagnetic transition, the electric polarization of
the metamaterials can also retain for a long time. Therefore, these materials may be used as magnetically driven electrets, i.e. substances with
long-lasting electrically polarized state.
Finally, we emphasize that the electric dipole moment of standalone
meta-atom is extremely small, because the charge separation is conned only within a very thin layer in the vicinity of the MN interface
because of absence of neighbors' mutual capacity. Therefore, only the
nanostructured metamaterial exhibits strong ME response.
This work was supported by the grant of the NAS of Ukraine #4/13N. The authors thank Prof. A. I. Kopeliovich for continuing interest in this
work and valuable comments.
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