Volume 89A, number 2

PHYSICS LETTERS

26 April 1982

COEXISTENCE OF FERROMAGNETISM AND SUPERCONDUCTIVITY IN ErRh4B 4

AND HoMo6S 8 : EXCHANGE OR ELECTROMAGNETIC MECHANISM?
L.N. BULAEVSKII, A.I. BUZDIN, S.V. PANYUKOV
P.N. Lebedev Physical lnstitute, Moscow, USSR
and
M.L. KULIC
Institute of Physics, 11001 Beograd, Yugoslav~
Received 5 January 1982

It is shown that the coexistence of magnetic order and superconductivity in ErRh4B 4 and HoMo6Ss can not be described if the exchange interaction is neglected and that the Ginzburg-Landau approach is not applicable to these systems.

Recent discoveries of superconducting compounds

that contain a lattice of rare earth ions have raised
questions of the nature of the interaction of superconducting electrons and magnetic moments. The experiments on ErRh4B4 [1] and HoMo6S 8 [2] revealed the possibility of the coexistence of magnetic
order and superconductivity in the temperature interval Tc2 ~< T~< Tm, where Tel = 8.7 K, T m = 1.2 K,
To2 = 0.9 K in ErRh4B 4, and Tel = 1.8 K, Tm = 0.70
K, Tc2 = 0.65 K in HoMo6S 8. The interpretation of
experimental data [ 3 - 6 ] leads one to conclude that
nonuniform magnetic order with wave vectors Q
= 0.06 A -1 and 0.003 A -1 is realized in the superconducting states of these compounds, respectively. Theories [3-6] which treat this problem can be divided
into two categories: (a) theories [3,4] which state
that the exchange interaction between superconducting electrons and localized magnetic moments (ex interaction) dominates in the formation of a nonuniform magnetic structure in superconducting state; (b)
theories [5,6] which state that the electromagnetic
dipolar interaction between electrons and magnetic
moments (em interaction) dominates and that the
formation of a nonuniform magnetic order in the superconducting state may be described without the ex
interaction.
0 031-9163/82/0000-0000/$02.75 1982 North-Holland

Now, two questions arise: (i) What are the contributions from the ex and the em terms to the properties
of the real systems, like ErRh4B 4 and HoMo6S8?
Which type of interaction dominates in the determination of the wave vector Q and of the critical temperatures Tin, Tc2 and so on. (ii) Is it correct to study the
systems like ErRh4B 4 (and HoMo6S8) in the framework of the Ginzburg-Landau (GL) approach?
In one of the frequently cited papers [5], which
treats ferromagnetic superconductors phenomenologically, the GL approach was suggested. Moreover, in
this paper the ex interaction between the superconducting and the magnetic subsystems was neglected.
On the basis of these assumptions the helical (spiral)
magnetic structure in the superconducting state was
predicted.
Later, in ref. [6] Greenside, Blount and Varma
(GBV) gave the following criterion for when the inhomogeneous magnetic state in a superconductor (ms
state) may be described by the Ginzburg-Landau (GL)
expansion without the ex terms:
Tmag/Tc ,~ 47r.

(1)

Here Tma8 ~ J 2/E F is the magnetic transition temperaturedue to the ex interaction between the superconducting and the magnetic subsystems, J is the ex93

Volume 89A, number 2

PHYSICS LETTERS

change energy of the conduction electrons with magnetic moments, and Tc is the superconducting transition temperature Tel.
In this paper we show that the criterion (1) is not
sufficient to neglect the ex terms in the framework of
the GL theory, and actually that much smaller values
of Tmag/Tc are needed to do this. It seems quite impossible to fulfill this correct condition on Tmag/Tc
in real systems, and certainly this condition is violated
in ErRh4B 4. So we conclude that the theories [5,6]
which ignore the ex interaction are not appropriate
for the description of real compounds like ErRh4B 4
and HoMo6S 8. We also show that the GL approach
is not applicable for the study of real systems, like
ErRh4B 4 (and HoMo6S8).
In refs. [5,6] the following GL functional, which
should describe magnetic superconductors is considered

5r = f d 3 r [F s + F m + e(1)
ex + e(2)
ex 1
J ,
F s = T1a l f f

12

+ ~l b l f f l 4 + p 0 1 ( 7 - i r o h ) ~ l

PO = h2 /2m ,

ro = 2e/hc ,

1
F m =alMI 2 +/31MI4 +$~,IM[
2 -B.n+n2/87r

e x - ' l~l Ui"~Atl2

' I ffl 2 ,

e(1)_

e(2)
~ / 2=1 7 M I 2 l f f l 2 e x ,

r/1 ~ j 2 / T c E F =Tmag/Tc,

r/2 =~2~71 ,

(2)

where a = N(O) T 2 ( T - Tc)/Te, N(O) is the density

of states at the Fermi level, a = ~0(T - T m ) / T m ,
a 0 ~ 1, {3 = 1/n Tm, n is the concentration of magnetic atoms, ~, is the interatomic distance, ~ is the
superconducting coherence length at T = 0. The
terms e(lx) and e~2x) describe the ex interaction
Let us study the question concerning the applicability of the GL functional itself. First, for the applicability of the GL approach [eq. (2)] to both subsystems, the condition (T c - T m ) / T c " 1 has to b e
fulfilled. Of course this condition is not fulfilled in
ErRh4B 4 (and in HoMo6S8). Secondly, the magnetic field must vary slowly with the superconducting
coherence length ~. It was obtained in refs. [5,6],
from functional (2) without the ex terms, that the
spiral magnetic structure is realized in the superconducting state at temperatures T < T m = Tm(1 + 47r/a0
- x / ~ ~//Xa0). The wavevector of this spiral structure is
'94

Q = (27r) 1/4 [')'~,(T)]-l/2,

26 April 1982

X2(T) = X2Te/2(Tc _ T ) ,

where X is the London penetration depth at T = 0.

The condition ~Q , I therefore leads to the inequality
(Tc - T ) / T c ,~ 72X2/Ir~ 4 which makes the temperature
interval, where the GBV theory [5,6] is applicable,
rather narrow
( Tc - T m ) / T e ~ 72~.2/7r~4 .

(3)

The condition (3), for example, is not fulfilled in

ErRh4B 4 where the lhs of (3) is of the order of unity,
and the rhs is of the order of 1 0 - 2 - 1 0 - 3 (we estimate 3'~ 3 10 - 8 cm, uF ~ 107 cm/s and then
= 10 - 5 cm from the data on N(0), and ~ ~ 2 X 10 -6
cm from the data for the upper critical magnetic field
Hc2(T ) near Tel [7]).
However, if for some reason (e.g. large X/G) the rhs
of (3) is large enough, the account of the ex interaction essentially modifies the GBV results. The ex
terms will change the values MQ, Q and ~ of the spiral
magnetic superconducting state (ms), predicted in
refs. [5,6]. When one determines the value MQ from
(2), the ex terms may be neglected if they are smaller
than the term Fro, i.e. - B M + B2/8n. In this way
the criterion (1) was obtained in ref. [6]. However,
the ex terms modify more significantly the other parameters of the ms phase [5,6], i.e. Q, ~ and the difference in free energies of the ms state and ferromagnetic normal (fn) state. This is because we should
now compare the ex terms with much smaller energy
F s and not with F m .
The wave vector of the spiral state is obtained from
the minimization of q-dependent terms of the functional [72q 2M2/2 + 7rM~/q 2X2(T)] where ~.- 2(T)
= 8~rp2r21t~ [2. If we compare e(2x) = r/2 q 2 M 2 l ~ 12
with these terms, we get the following condition for
the applicability of the GBV theory: 7721@12 ~ 7 2, i.e.
[(Tc - T)/Tc](Tmag/Tc)'~ (7/~) 2

( r < Tm).

(4)

In the situation of experimental interest, i.e., for (Tc

- T ) / T c ~< 1, the criterion (4) is fulfilled for unrealistically small values of the ex interaction. For example,
in ErRh4B 4 the rhs of (4) is of the order 10 - 4 , while
the lhs is of the order 10 -1. For testing (4), we estimated Tmag (for ErRh4B4) from the measurements
of Tel (x) in compounds Erx Y1-x Rh4 B4, and
Erx LUl_ x Rh4B 4 with nonmagnetic atoms Y and Lu
[8,9]. When x ~ 0, one has dTcl (x)/dx ~. 3 K for

Volume 89A, number 2

PHYSICS LETTERS

26 April 1982

ErRh 4 B4. Since dTcl (x)/dx ~ rr2 Tmag/2, it follows

that Tmag is of the order of 1 K. So, in ErRh4B 4 the
opposite inequality is fulf'dled. If the condition (4) is
violated, then the ex interaction is essential, and the
wavevector of the spiral structure would be quite different from the value found in refs. [5,6].
The term e ex,
(1) as well as F s, determines the value
of ~k at a given M, and it may be neglected if it is
much smaller than the term F s, i.e. r/1M2 .~a[2. This
criterion says that if conditions (3) and (4) are fulf'dled, then the GBV results are valid in a very narrow
temperature interval Tin(1 - r) < T < T m with r
.~ TmTc/EFTmag. At T < Tm(1 - r) the phase found
by GBV does not exist. So the prediction [5] of the
first order transition temperature To2 from the ms to
the fn state, i.e. Te2 = Tm(1 - r l ) with r 1 ~ (Tc/
EF) 1/2 , is correct only in the case Tmag < Tm(Te/

tion 0 m to the energy of the ferromagnetic state (per

one localized moment) at T = 0, where 0 m = 21rit2n;
It is the magnetic moment, n is the concentration of
localized moments. The value of 0 m is 1.4 K in
ErRh4B 4 (/.t = 5.6itB, n = 1022 c m - 3 ) , and 0 m ~ 3 K
in HoMo6S 8 ~ = 9 g B , n ~ . 4 X 1021 c m - 3 ) . The em
interaction determines also the direction of Q so that
the nonuniform magnetic order in the ms phase is
transverse [I0]. To describe real systems it is necessary
to take into account the magnetic anisotropy. The
theory of the ms phase for magnetic superconductors
with T m ,~ Tel which takes into account both the ex
and em interaction as well as the magnetic anisotropy,
is presented in ref. [4].

EF)I/2.

[1] D.E. Moncton et al., Phys. Rev. Lett. 45 (1980) 2060.

[2] J.W. Lynn, G. Shirane, W. Thomlinson and K.N. Shelton,
Phys. Rev. Lett. 46 (1981) 368;
J.W. Lynn, A. Raggazoni, R. lynn and J. Joffrin, J. de
Phys. Lett. 42 (1981) L-45.
[3] L.N. Bulaevski, A.I. Rusinov and M. Kulid, Solid State
Commun. 30 (1979) 59; J. Low Temp. Phys. 39 (1980)
256.
[4] L.N. Bulaevski, A.I. Buzdin, S.V. Panyukov and M. Kuli6,
submitted to Solid State Commun.
[5 ] E.I. Blount and C.M. Varma, Phys. Rev. Lett. 42 (1979)
1070,
[6] H.S. Greenside, E.I. Blount and C.M. Varma, Phys. Rev.
Lett. 46 (1981) 49, and references therein.
[7] H.R. Ott, W.A. Fertig, D.C. Johnston, M.B. Maple and
B.T. Matthias, J. Low Temp. Phys. 33 (1978) 159;
H. Cantor, E.D. Dahlberg, A.M. Goldman, LE. Toth and
G.L. Christner, Solid State Commun. 34 (1980) 485.
[8] H. Cantor, E.D. Dahlberg, A.M. Goldman, L.E. Toth and
G.L. Christner, Solid State Commun. 34 (1980) 485.
[9] K. Okuda, Y. Nakamura and K. Kadowald, Solid State
Commun. 32 (1979) 185.
[10] A.I. Buzdin and L.N. Bulaevskii, Zh. Eksp. Teor. Fiz. 79
(1980) 1954;
M. Kuli6, Phys. Lett. 81A (1981) 359;
L.N. Bulaevskii, A.I. Buzdin, S.V. Panyukov and A.I.
Rusinov, Solid State Commun., to be published.

We conclude therefore that the account of the ex

interaction is very important to determine the param.
eters of the ms phase in real compounds, and the experimental data on ErRh4B 4 (and HoMo6S8) could
not be described by the theories of refs. [5,6]. Actually, Tmag is of the order of Tm, and Tm is essentially
smaller than Tel in ErRh4B 4 (and HoMo6Ss). So we
cannot use the GL theory for the investigation of the
ms phase in these compounds. It was shown in ref.
[10] that in this case the ex interaction plays the
main role in determining the values of the wave vector
Q and that of the superconducting order parameter in
the ms phase. This does not mean that the em interaction can be fully neglected in the description o f the
ms phase. Its contribution to the value of T m and to
the absolute value of the free energy of the ms phase
and fn state is of the order of the ex interaction in
real crystals. Certainly, the dipolar em interaction significantly contributes to the energy of the magnetically ordered states in ErRh4B 4 and HoMo6S 8. The
long range part of this interaction gives the contribu-

References

95