Magnetoelectric susceptibility tensor of multiferroic TbMnO3 with cycloidal antiferromagnetic

structure in external field

Igor V. Bychkov*, Dmitry A. Kuzmin and Sergey J. Lamekhov

Chelyabinsk State University, 454001, Chelyabinsk, Br. Kashirinyh Street, 129, Russia

Vladimir G. Shavrov

The Institute of Radioengineering and Electronics of RAS, 125009, Moscow, Mokhovaya Street, 11-7,

Russia

Magnetoelectric, dielectric and magnetic susceptibility tensors of multiferroic TbMnO3 with cycloidal

antiferromagnetic structure in external electric and magnetic fields have been investigated with taking

into account dynamics of spin, electro-dipole and acoustic subsystems. All components of tensors depend

on values of external electric and magnetic fields. The possibility of control of electrodynamic properties

of multiferroic TbMnO3 with cycloidal antiferromagnetic structure by external electric and magnetic

fields has been shown. The resonant interaction of spin, electro-dipole, electromagnetic and acoustic

waves in such material is observed.

*E-mail address: [email protected]

1
 Nowadays multiferroics, materials with magnetic and electric ordering, attracts researchers attention

for their unusual physical properties1-3: existing of electromagnons and possibility to control it by an

external electric field. Often multiferroics have a modulated magnetic structure, which contribute a

number of features in the spectrum and dynamics of spin, acoustic and electromagnetic excitations in

material4-6: band structure is observed, the nonreciprocity effect is manifested, i.e., difference between the

velocity of wave transmission along and against the modulation axis. Orthorhombic multiferroic TbMnO3

(Pbnm), for example, has a cycloidal antiferromagnetic structure at temperatures T < 28 K 7. The coupled

spin, electro-dipole and electromagnetic waves in TbMnO3 with cycloidal antiferromagnetic structure had

been theoretically investigated earlier8,9, however the influence of external electric and magnetic fields on

dynamic properties of such material are not studied enough. The present work is devoted to studying of

electrodynamical properties of orthorhombic multiferroics placed in an external electric and magnetic

fields of different directions. Derivations of dynamcis of the coupled excitations in the modulated

magnetic structures are carried out in regime L a , where L = 2 k is the period of modulated

structure, a is the lattice constant, k is the wave number of modulated structure, when the

phenomenological method is applicable.

Method of Lagrange has been used for investigating of dynamics of TbMnO3 with cycloidal

antiferromagnetic structure. The Lagrangians expression is L = E F , where E - the kinetic energy, F

- the Ginzburg-Landau function. In case of orthorhombic multiferroic TbMnO3:

1 1 1 2
( ) ( ) ( )
a w u 2 2
E=
V 2 A 2 + M + P 2 + u 2 dr; F = { A 2 + Az 2 + A 4 + y A
V 2 2 4 2
+
2
yA
2 1 2 2 2 b 2
MH + M + ( AM ) +
2 2
2

2 2
( )
A M + P PE + Pz Az y Ay Ay y Az + (1)
+ cijlmuij ulm + bijlm Ai A j ulm + dijlm Pi Pj ulm }dr.

Where M = M1 + M 2 + M 3 + M 4 is the magnetization of the crystal; A = M1 M 2 M 3 + M 4 is the

(
vector of antiferromagnetism; P is the vector of polarization; uij = ui x j + u j xi ) 2 is the tensor of

deformations; u is the displacement vector; w is the constants of anisotropy; a, u , , 1 , 2 is the

2
constants of homogeneous exchange; , is the constants of heterogeneous exchange; b, is the

constants of electric and magnetoelectric interactions; cijlk , bijlk , dijlk is the tensors of elasticity,

magnetostriction and electrostriction; = mvc z 2 , where z and m is the charge and the reduced mass of

the elementary cell with the volume vc ; = 8g 2 M 0 2 , where is the static transversal magnetic

susceptibility, g is the gyromagnetic ratio, M 0 is the magnetization of sub lattices.

The ground state of TbMnO3 with cycloidal antiferromagnetic structure is described by vectors of

antiferromagnetism and polarization with following components: P0 x = P0 y = 0; P0 z = P0 ; A0 x = 0;

A0 y = A 1 sin ky; A0 z = A2 cos ky . The coordinate axiss direction defined by x||a, y||b, z||c. So, y-axis is the

modulation axis, z-axis is the direction of the spontaneous polarization in TbMnO3.

Expressions for determining the parameters of the ground state can be obtained from the minimum of

energy. In case of external electric field E is collinear to a spontaneous polarization P0z and external

magnetic field have all non-zero components:

2 2 2
2
(
)
M 0x 2 A12 + A22 + = H 0x ; M 0y , z 1 A1,2
2
+
2
A1 + A22 + = H 0y , z ;

( )

3
( 2 2
) 2 2
(
k A1 + A2 + k A1 + A2 A1 A2 P0 = 0;
2
)
( )
p3 P03 + P0 p1a1 A12 + p1a 2 A22 + b kA1 A2 = E0 z ; (2)
a13 A13 + (
A1 a11 p P02 + a11a 2 A22 + a11my (
M 02x + M 02y + M 02z ) + 4 ( k + k + a )) 8kP A = 0;
4 2
0 2

a23 A23 + A (a
2 21 p P0
2
+ a21a1 A12 + a21my (M 2
0x + M 02y + M 02z ) + 4 ( k + k + a + w)) 8kP A = 0;
4 2
0 1

Here, the following notation has been introduced: = det cij , p3 = 8 1 ( D3 D3 ) ,

p1a1 = 4 1 ( B 2 D3 ) , p1a 2 = 4 1 ( B 3 D3 ) , a13 = 3u 24 1 ( B 2 B2 ) , a11 p = 32 1 ( D3B2 ) ,

a11my = 4 ( 1 + 2 ) , c44 8 1 ( B 3B2 ) ,

2 1
a11a 2 = a21a1 = u B44 a23 = 3u 24 1 ( B 3 B3 ) , a21my = 4 2 ,

( )
a21 p = 32 1 ( D3 B3 ) , i = 1i , 2 i , 3i , i = ( i1 , i 2 , i 3 ) , = B, D, i = 1, 2,3, ji can be

obtained from expression for by changing of j column to vector i .

The equilibrium deformations are heterogeneous:

3
 0
u xx (
= 2 1 1B 2 A12 cos 2 ky + 1B 3 A 2 2 sin 2 ky + 1D 3 P02 ; )
u 0yy = 2 1
( 2 2 2 2 2 2 2
B 2 A1 cos ky + B 3 A 2 sin ky + D 3 P0
2
); (3)
u zz0 = 2 1 ( 3 2 2 3 2 2 3
B 2 A1 cos ky + B 3 A 2 sin ky + D 3 P0
2
);
1
0
u xy 0
= u xz = 0; ( )
u 0yz = B44 2c44 A1 A2 sin ky cos ky.

For investigation of dynamic characteristics one have to take into account the system of Lagrange

equations for A , M , P and u . Solving the system of equations by method of low oscillations,

linearizing and using the form of harmonic series for variables, in approach of first harmonics for the

waves, propagating along y-axis, the oscillating amplitudes of polarization p and antiferromagnetism a

vectors can be expressed as pi = ij e j + ijem h j , mi = ij h j + ijme e j , where, ij , ij is the tensors of

( )
*
dielectric and magnetic susceptibility, consequently, ijme = ijem is the magnetoelectric susceptibility

tensor (operation * means the complex conjugation).

The study shows that in case of H || x , i.e. H = ( H 0 x , 0, 0 ) , the tensors ij and ij are diagonals with

the following components:

( ) ( )( )( )
1 2 1
xx = 1 2px 2 ; zz = 1 mx 2 l2 +ay az + +ayaz mx pz mx pz
pz mx
;

( )( )
2
1 2 tz2 +
ay az + az
+ ay


yy = ;
(
py ay +az + +azay

2
)
iBzy44 2 +azay Dz 44 + Dz 32 By 44 2 Dz 32 ay
+ Dz 44l2 tz2
( z 2 z +
B 44 D 44 az (5)
1
)
1
( ) ( ) ( )
1
xx = 1 zz pz mx 1 2 l2 ; yy = 1 +ax 2 2my +ax + 12xy 2 tx2 ;
2
1
2 1 2 2
(
zz = 1 2 ax
2
2
) 2 2 2
1xz 2 xz mz ax (
)( )
Here the following notation has been introduced: (
+ax = By 66 2 tx2 2 +ax 2 2 tx2 , )( )
+
ay ( )( ) (
= By 22 2 l2 2 +ay 2 2 l2 , az = Bz 32 2 l2 2 az 2 2 l2 , By 66 2 = ( 2c66 ) B66
2 2
A1 , )( ) 1

( +
az , ay )= y 2 2
B 44 tz ( (
2 +az 2 , ay
2
)) ( 2
tz2 , ) + az
ay ( )
= i 2 2 l2 + iBy 22Bz 32 l2 ,

( )
+azay = i 2+ 2 tz2 + iBz 44 By 44tz2 , By 22 2 = 2 ( c22 ) B22
2 2
A1 ,
1
Bz 32 2 = 2 ( c22 ) B32
2 2 1
A2 ,

4
 py = Dz 44 2 tz2 2 2py ( )( 2
)
tz2 , pz = Dz 32 2l2 2 2pz ( )( 2
)
l2 , By 44 2 = ( 2c44 ) B44
2
A12 ,
1

( ) ( )( )
2
mx = 2 l2 42 xy az + 42 xz +ay + i 222 xy 22 xz +ayaz 2 2mx +
ay az + +ayaz ,

mx
pz
= 2 l2 me {(
Ay 2 + az Az 2
ay + me az )( )( 2
2 xy ) (
i22 xz iDz 32l2 Bz 32 +ayaz + By 22 az )( 2
2 xy + i22 xz )} ,
( ) (
2 2 2 Az 2 + az + i Ay 2 + + 2 Ay 2 + az i Az 2
az ) ( )
mx = ( 2
l2 ) z
l 2 xy me ay me ay 2 xz me ay me
,
pz 2 2 y + az z
( + 2 z + az
D 32l 2 xy B 22 ay iB 32 ay 2 xz B 32 ay + iB 22 az
y
) ( )
1 1 1
Bz 44 2 = ( 2c44 ) B44
2
A22 , Bz 66 2 = ( 2c66 ) B66
2
A22 , Bzy44 2 = Bz 44By 44 , Dz 32 2 = 4 ( c22 ) D32
2 2
P0 ,

me( ) 2 = 2 1A(1,2) k
1
Dz 44 2 = ( c44 ) D44 i2 j ( y , z ) = ( )
2 1 2 A y,z
P02 , i M 0 j A(1,2 ) , i = 1, 2, j = x, y, z ,

2 = 1 u B44

2
{ }
( 2c44 )1 A1 A2 2P0 k , tx = stx q, tz = stz q, l = sl q, stx = 2c66 , stz = 2c44 ,

sl = c22 are the velocities of transversal x and y polarized and longitudinal acoustic waves, q is the

wave number of the propagating wave, ( (

2pi = 1 b + 4 Di , u 0p , i = x, y, z , ))
(
u 0p = 2 1 1D 3 , 2D 3 , 3D 3 , 2mx = 1 + 2 A12 + A22
) ( ) 2 , 2my = 1 + 2 A12 + A22
( ) 2 + 1 A12 2 ,

a( x , y , z ) 2 =
a + M

2
1 0( x , y , z ) + 2 M + 4 B (1,2,3 ) , u
1
0P
+ k 2 + k 4 + ( )
,
({ ( ) } (
+ u A12 + A22 + 4 B 1,2,3 , u 0A1 + u 0A2 2 u A12 A22 + 4 B 1,2,3 , u 0A1 u 0A2
( ) )) ({ } ( )) 4

2mz = 1 + 2 A12 + A22

( ) 2 + 1 A22 2 .

The magnetoelectric susceptibility tensor ijme has only one non-zero component:

1
me
xz = zz mx mx
pz
(6)

( )
In case of H || y , i.e. H = 0, H 0 y , 0 , the tensors ij and ij also are diagonals with the components:

( ) ; = ( ) ( + ) ( ) ;
1 + ay 2 mz 1
xx = 1 2px 2 yy
1
mz
2 2
tz

ay
+
az az mz py
py
mz py

my ( ) ( + )
2 2 + + az 2
1
1
; = ( ) + ( )
l ay az ay
+ 1 2 2 + 4 2 2
zz = ; (7)
( )
xx ax mx ax 1 yy tx
my pz pz
my
2 my
pz
yy = zz pz ( ) ; = ( ) .
1
my
1 2 2 1
l zz yy py
1
mz
1 2 2 1
tz

5
 Note, that in (7):

(
py = py ay +az + +azay
2
) z 2 4
D 44 tz
2iBzy44 2 +azay + By 44 2 ay + Bz 44 2 +az , me

Ay 2 Ay 2
= me Bz 32Dz 32

+
pz = pz ay (
az + ay
+ az


2
)+
Ay 2 +
+ Az 2
Ay 2 2
( (
2 z z 2 + az Az 2 2 2
) 2
ime ay me l + B 32 D 32l ay me l B 22D 32 l ,
y z

) ( ( ) )
( (
2 y z 2 Ay 2 2 2 z
)
me az me l B 22D 32 l ay me l + B 32 D 32 l
Az 2 2 + az z 2
) ( ( ) )
(
my = 2 2 l2 12yy + 22 yy )( ) (
az + 42 yz +ay + 2i 12yy + 22 yy 22 yz +ayaz )
2

Az 2
, me Az 2
= me By 22 Dz 32
(
2 2
my )( +
ay
az +
+ az 2
ay
),
( ) ( )( )
2
mz = 21 2 tz2 14yy ay + 14yz +az 2 2mz +
ay az + +ayaz ,

my
pz
= Az 2 2
l (
B 32 D 32 l ay 1 yy )
Ay 2 2 2 + z z 2 + az 2 + 2 i2 + +
me 2 yy 2 yz ay
,
( )
+ az
2 y z 2
( 2 2
)
+ me l B 22 D 32 l az 1 yy + 2 yy i2 yz ay
2
( )
my 2 2
pz = 2 l ( Az 2
2 + 22 yy me
1 yy )(
Ay 2 +
az + 22 yz me Ay 2
ay + i me )
12yy + 22 yy + 22 yz me
Az 2
+ayaz ,
{ ( ) }
mz
py
= 21 Dz 44tz2 i12yz Bz 44 az

+
12yy By 44 ay +ayaz 12yz Bz 44 + i12yy By 44 ,
( )
my z 2 4
y 2 z 2 + y z + az

pz = D 44 tz B 44 az B 44 ay 2iB 44 B 44 ay . The other symbols have been

introduced above.

In this case there are two non-zeros components of magnetoelectric susceptibility tensor:

1 1
me
yz = zz my my ; zy = yy mz mz ;
pz me py
(8)

In case of H || z , i.e. H = ( 0, 0, H 0 z ) , the tensors ij and ij are:

( ) ; = ( ) ( + ) ( )
1 + ay 2 1
xx = 1 2px 2 yy
1
mz
2 2
tz

ay
+
az az my py my py
py my
;

my( ) ( + )
2 2 + + az 2
1
1
; = ( ) ( )( )
l ay az ay
1 2 2 4 2 2 2 2
zz = mx ax ; (9)
( )
xx ax 1zz
mz pz
pz
mz 2 mz
pz
yy = yy
py ( ) ; = ( ) ;
1
mz
1 2 2 1
tz zz zz pz
1
my
1 2 2 1
l

6
 In (9) the following notation has been used:

( ) ( ) ( )( )
2
my = 21 2 tz2 14zy az + 212zy 12zz ay
+ + az
+ i 12zz + 12zy 2zy ay 2 my
2 +
ay az + +ayaz ,

( )
mz = 2 2 l2 24 zy az ( ) ( ) + az
2
+
+ 12zz + 22 zz ay + 2i 12zz + 22 zz 22 zy ay

( +
2 2mz ay)( + az 2
az + ay ,
)
my
py
= 21 Dz 44 tz2 12zz Bz 44 az

+
+ 12zy By 44 ay + az
+ i ay (
12zz Bz 44 + 12zy By 44 ,
)
my 2 2 2 2
( +
) + az
py = D 44 tz 1zy tz 2B 44 az + B 44 ay + i ay
z z y
Bz 44 + 2By 44 ,
( )

mz
pz
= Az 2 2
(l )
Ay 2 2 2 + z z 2 2 + az + i 2 + 2 + +
me B 32 D 32 l 2 zy ay 1zz 2 zz ay ( ,
)
+ az
2
( y z 2
)
+ me l B 22D 32 l 2 zy az i 1zz + 2 zz ay
2 2 2
( )

( )
i Ay 2 2 2 + z z 2 2 + az + i 2 + 2 + +
2 me ay ( )
mz = 2 2
(
l ) l B 32 D 32 l 2 zy ay 1zz 2 zz
+ az
.
pz
+

Az 2
me 2
2
l y
B 22 (z
D 32 l )
2 2

2 zy
az + i 2
1 zz + 2
2 zz ay (
)
Also there are two non-zeros components of tensor ijme :

1 1
me
yy = yy my mz ; zz = zz mz my .
py me pz
(10)

Note, that without an external magnetic field the tensor of magnetoelectric susceptibility has no non-

zeros components. So, an external magnetic field activates some components of the tensor depending on

the direction of field.

FIG. 1. Frequency dependence of some components of the susceptibility tensor.

(10 kOe = 1 T, 100 CGSE 30 kV/cm)

7
 One can see that all components of all tensors have a resonant type. This effect is manifested in cause

of resonant interaction of subsystems of TbMnO3. As well as k , A1 , A2 , P0 and M 0i are the functions

from H and Ez , defined from solving of the system of equations (2), the resonant frequency values

depend on values of both electric and magnetic fields and its direction. Fig. 1 shows this dependence. Let

( ) ( )
1 1
us now estimate some dependences. From (2), A12 A102 u2 2 H 2 , A22 A20
2
u2 ( 1 2 2 ) H 2 ,
1 1
M 0i 1H i P0 k b 1 A1 A2 + b 1Ez , A102 = ( 2u ) ( w 2 L1 ) , 2
A20 = ( 2u ) ( w + 2 L1 ) , k 2 2 ,

L1 = a 2 4 < 0 . For values of constants9-12 1014 cm2, 1028 cm4, a 100 , u 0.1 ,

w 10 , 100 , b 0.4 , 109 , 1,2 104 we have A1,20

2
103 Oe2, k 107 cm-1. So, for example,

( )
12
11 H x A202 ( u2 ) vary in range of 0 12xz ( 12xz )
1
12xz ( ) ( 1 2 2 ) H x2
1 2
with changing
max

of H x , and take a maximum ( 12xz ) 1021 s-2 in field H x 105 Oe. Decreasing of field to H x 104 Oe
max

will decrease this value to 12xz 1019 s-2. The frequency changes with the electric field on value

( )
12
about k 1b 1Ez 1010 s-1 for Ez 100 CGSE (about 30 kV/cm). It shifts the resonant

frequency corresponding to interaction of electromagnetic wave with antiferromagnetic subsystem to

lower frequencies on value about 1xz and to higher frequencies on . The dielectric and magnetic

susceptibility tensors have different expressions for their components in magnetic field of different

directions. As well as reflectance and transmittance of electromagnetic waves depends on the dielectric

and magnetic susceptibility, these characteristics also depend on values of electric and magnetic fields

and its direction. So, it is possible to control the electrodynamic properties of TbMnO3 by external

electric and magnetic fields.

8
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