, 59, ., .

765 - 769
P A R A M A G N E T I S M

O F

1994 . 10

S U P E R C O N D U C T I N G

S.V.Panyukov,
I . E . Tamm Department

of Theoretical
Moscow

A.D.

C E R A M I C S

Zaikin

Phytic;

P.N. Lehedev Physics

117924,

Institute

Russia

Submitted 26 April, 1994

Interaction between spontaneous current loops (orbital magnetic moments)
induced by weak links with negative coupling energies (-junctions) can cause para
magnetism of granular high-temperature superconductors. We show that at certain
concentration of -junction the system consists of infinite percolating superconduct
ing cluster and normal regions with frocen-in magnetic field and ordered orbital
magnetic moments.
In

was f o u n d e x p e r i m e n t a l l y [1] (see

review)
samples
critical

also

Ref.

[2] f o i f u r t h e r

references

that

magnetization of

certain h i g h - t e m p e r a t u r e superconducting

can

c r u c i a l l y depend

on

temperature T

whether

these

i n zero or nonzero

samples

are

e x t e r n a l magnetic

cooled
field

effect

were f o u n d t o be paramagnetic

Wohlleben

effect

(WE)

[2].

for H

1 Oe.

The

experimental data

susceptibility o f the W E samples x are well described

=+/(#
where x o - b i /
e

~0.1

I t was shown i n Ref.

negative
system

see

(so

called

(e.g.

Ref.

mechanism
current

[1] for

the

this

magnetic

+ ),

(1)

(i>2 ~ 0.01 4 - 0 . 1 ) is a constant magnetic

A n i n t e r p r e t a t i o n o f W E suggested

various microscopic
our

cooled

b y the expression

[1] t h a t the paramagnetic behavior

m o d e l o f a r a n d o m n e t w o r k o f Josephson

field

we w i l l call

(1)

moment.

cannot be

ascribed

o f isolated magnetic i m p u r i t i e s or s m a l l ferromagnetic clusters inside

the sample.
and

the

Whereas

(i>i ~ O.l-j-0.2) is a diamagnetic p a r t o f the sample susceptibility,

Oe a n d M o = i>2/4ir G

t o the effect

Below

below

H.

zero-field cooled samples showed a usual diamagnetic Meissner response,

samples

and

ceramic

tunneling

[2] for
one

loops

T-junctions

mechanisms

can

can

show

occur

the e x t e r n a l magnetic

that

i n the

field

[4]) Josephson

coupling energies.

impurities,

discussion).
[4]

[ 1 , 3, 2] is based on the
There

in

ground

unconventional pairing

Irrespectively t o
the

presence

state

of a

of

particular

-junctions

spontaneous

superconducting

o r b i t a l magnetic m o m e n t s

associated

etc.

physical

system.

with

such

According

contribution to x
Sharing
sufficient

the

to

Refs.

[ 1 , 3, 2] this m a y result i n a

In

loops

become ordered i n the d i r e c t i o n o f this field a n d the sample acquires nonzero

magnetization.

are

w h i c h m i g h t cause the presence o f T - j u n c t i o n s i n

v i a magnetic

further

i n Refs.

j u n c t i o n s w i t h positive (usual j u n c t i o n s )

total

paramagnetic

0)-

basic

idea

of

this

scenario

we

believe

t o u n d e r s t a n d the n a t u r e o f W E . Indeed for

that
H

i t is

< #

by

no

means

~ 10 - r 100

Oe

t h e system is i n the Meissner state a n d therefore o r b i t a l magnetic m o m e n t s inside

a massive
field.

3d superconducting sample cannot be ordered by an e x t e r n a l magnetic

F u r t h e r m o r e , as the c r i t i c a l t e m p e r a t u r e T

for the whole granular a r r a y is

always smaller t h a n t h a t for i n d i v i d u a l grains local spontaneous

appear

already above T

i n d i c a t i o n for t h i s effect

r e s u l t i n g i n some paramagnetic
has been

effect

c u r r e n t loops m a y
for T > T .
c

No

detected i n [1]. A t last, a simple estimate for

765

the l o o p magnetic m o m e n t ~ I a
c

size a a n d I

= 2eEj

(the t y p i c a l l o o p size is o f order o f the g r a i n

is t h e i n t e r g r a i n

Josephson c r i t i c a l

t y p i c a l e x p e r i m e n t a l parameters a ~ l - i - 5
magnetic

m o m e n t s can be ordered

Oe, whereas

c u r r e n t ) shows t h a t

for

a n d Ej ~ 10 a t T ~ 100 o r b i t a l

only by t h e magnetic

W E persists d o w n t o m u c h lower

fields

field

~ 0.03

~ 1 - r 30

;>, /

Oe [1].

I n this L e t t e r we propose an e x p l a n a t i o n for W E w h i c h does n o t face w i t h t h e

above problems.

We

first

o f phenomenological
fluctuating

in

i l l u s t r a t e the m a i n idea o f our e x p l a n a t i o n w i t h the a i d

G i n z b u r g - L a n d a u ( G L ) f u n c t i o n a l for a superconductor

space c r i t i c a l

temperature.

Then

we derive t h i s

with

G L f u n c t i o n a l for

a rigorous m o d e l o f a n e t w o r k w h i c h contains b o t h usual Josephson j u n c t i o n s a n d

ir-junctions.
L e t us consider a 3 d s u p e r c o n d u c t i n g system a n d make t w o assumptions.
following

[ 1 , 3,

2] we assume t h a t

i r - j u n c t i o n s induce

spontaneous

( o r b i t a l magnetic m o m e n t s ) i n the g r o u n d state of our system.

First,

c u r r e n t loops

Second, we assume

t h a t the presence o f such o r b i t a l magnetic m o m e n t s leads t o a local suppression

a superconducting

order parameter w h i c h can

space c r i t i c a l t e m p e r a t u r e ST (r)/T
c

transition

one

can

describe

= t(r).

the

system

be

described

T h e n close t o a s u p e r c o n d u c t i n g
by

the

of

by the f l u c t u a t i n g i n

phenomenological

GL

phase

functional

[5, 6]

+-

(r + < ( r ) ) M

where we define r = T/T

critical

^ | ( v

p o t e n t i a l a n d is the f l u x q u a n t u m .

With

field

fluctuations
~

e n

to

we get

small

disorder

lead

a n d g depend

a superconducting
can

1/2

|rj

re,

results

For

T G such

> ,

shown

e n

the

parameter

~ 1.

the

Ginzburg

Ref.

a r o u n d

t r e a t e d i n a s t a n d a r d way.

where

where

of

order

be

to

the

[6]

to

a small renormalization of

Thermodynamic

the

p a r a m e t e r TQ
fluctuations

statistical

critical

) / W

statistical

= (TD/\T\) ,

1/2

f l u c t u a t i o n s are n o t

of

temperature

/(8^c ).

(3)

important and

phase t r a n s i t i o n takes place

a t T = T

a usual second

. I n this case the

en

system shows a usual diamagnetic Meissner response a n d no W E

TJ

on

order s u p e r c o n d u c t i n g

was

field
vector

= T ( 1 + ' T J ) , T ) < 1 a n d t o the dispersion

)

For

parameters 7

is the

later.

<(<5^) ) = / | - | / / ,

provided

According

of

The

the l a t t i c e t y p e , A

are

() / .

1/1 due
TJ

fluctuations

fixed

on

value (i/>) = /\\ / 7 for T < T

the a i d of (2)

is the mean

details o f the m o d e l a n d w i l l be
Thermodynamic

(2)

- 1 a n d ( t ( r ) t ( r ' ) ) = gS(r - r ' ) . Here T

t e m p e r a t u r e , ~ 0.1 4- 1 depending

its mean

- ^ A ^

(b ~ 2.5)

i n Refs.

[5, 6]

the

physical

that

due

to

p i c t u r e becomes
space

fluctuations

occurs.

more

complicated.

of T

already

there appear s u p e r c o n d u c t i n g domains w i t h an average size ~ {/) 1

1

It

above
and

c o n c e n t r a t i o n ()
p(T)*C Sexp(-S),
If

one

become

766

lowers

the

temperature

larger

and

at

p e r c o l a t i n g cluster.

A ~ 37.8.

S{ )=A{T/T yi ^>\,

= w

both
c

concentration

0.15

(see

e.g.

of
[7])

domains
they

and
form

T h i s c o n d i t i o n is r o u g h l y equivalent t o S(r )
p

(4)
their
an

ss 3 a n d

size

infinite
yields

Tp as (3/A) TD

~ 10

at

T = T

below

= 77

Tp the

normal

_ 5

9 / .
2

T h u s for

( l + ) due

e n

to

superconducting

regions

surrounded

state

by

> g l o b a l s u p e r c o n d u c t i v i t y

percolation

is essentially

infinite

applies a s m a l l magnetic

field

becomes trapped

superconducting
inside N-regions
s l i g h t l y below
a

diamagnetic

N-regions

inhomogeneous:

appears
slightly

i t consists

cluster.

The

of

volume

of

t e m p e r a t u r e a n d eventually n o r m a l

above T

below

a n d t h e n cools the

due

t o the

For

s m a l l enough

are disordered

due

to thermal fluctuations.

Meissner
magnetic

< /

Therefore

system

effect

in

moments
at T

just

no p a r a m a g n e t i s m occurs a n d t h e s u p e r c o n d u c t i n g sample shows

response.

until

Below

T* < Tp.

field

i n N-regions

surroundings.

shrinks a n d

grows

H(T)

At

disappear.

I f one
this

transition.

superconducting

s u p e r c o n d u c t i n g phase increases w i t h decreasing

regions

phase

However

due

the

to

value

magnetic

T*

as

the

t h e t e m p e r a t u r e is lowered

magnetic

fiH(T")

flux

is reached

~ T*

moments

conservation

are ordered,

at

the

volume

t h e frozen-in

of
field

certain temperature

the magnetization M

of t h e

sample is s a t u r a t e d (M = M o ) a n d i t s response becomes p a r a m a g n e t i c for n o t very

large H

(1).

rough estimate for Mo ~ /

yields Mo ~ 0.01/4 G .

s h r i n k i n g of t h e N-regions v o l u m e w i t h decreasing
magnetic energy ()
susceptibility

same behavior
lower

T)

0)

exceeds the s u p e r c o n d u c t i n g condensation

remains

(diamagnetic

t e m p e r a t u r e independent
response very close t o T

has been detected

superconducting

domains

already

rigorous analysis based on

transparent

i n Ref.

[1].

at

estimate () ~ -

and

WE

developed

At

at

energy)

Exactly

T*.

fields

does

i n Ref.

the

not

> H

at

destroy

take place.

[5] yields a physically

for t h e parameters

e s t i m a t e { ) t o be of order several / a n d get H

(the

and the

t u r n i n g to paramagnetic

Large magnetic

T > T

the m e t h o d

Further

T is energetically f o r b i d d e n

of Ref.[l]

we

~ 10 Oe i n a good

agreement

N o w let us derive the G L f u n c t i o n a l (2) for a g r a n u l a r superconductor

described

w i t h e x p e r i m e n t a l results [1].
by the

Hamiltonian
H = -

*<

Y,

(5)

r') c o s M r ) - *>(!')),

<r,r')
where

the s u m is t a k e n over

Josephson j u n c t i o n s between

c o n d u c t i n g grains w i t h coordinates
We shall consider

<p(r').

variables

Ej

< 0 w i t h the p r o b a b i l i t y p.

equal

the Josephson c o u p l i n g energies

stochastic
E

to

all neighboring

r and r ' and superconducting

= Eo > 0

Ej

with

For E

the

r ' ) as

Ej(r,

super

phases (p(r)

probability

and

independent

1 p

= 0 this m o d e l has been

and

to

considered

i n details i n Ref.[10] w i t h the a i d o f the replica m e t h o d , the generalization for the

case E

> 0 is s t r a i g h t f o r w a r d . Near the c r i t i c a l t e m p e r a t u r e T

a,f3 = l , ducting

i t is sufficient t o

i n t r o d u c e o n l y t w o order
-,m

order

are

replica indices.

parameter

Edwards-Anderson

parameters
for

The

= (exp(i<p)) a n d Q p
ip-Held represents

g r a n u l a r superconductor

order parameter Q p
a

ular a r r a y w i t h frozen-in spontaneous

= (exp i(<p <P^)),

a

a standard

(see

e.g.

c u r r e n t s . Proceeding
free energy

m = 0

exp(-F /T) m

and

the

i n m u c h t h e same way

o f the system

represented i n terms o f the p a t h i n t e g r a l over replica fields -

[8])

[9] describes t h e . g r o u n d state o f a g r a n

as i n Ref. [10] t h e c o n f i g u r a t i o n a l l y averaged

F = -TdF /dm

supercon

f D4>(T)DQ(T)

exp [ - (

and

can

be

(6)

Qp
a

+ H )/T]
INT

767

where
2714

ca~

(7)

90

dr

(8)

5"

As before the parameter is equal to = / 1,

the mean field superconducting c r i t i c a l t e m p e r a t u r e
Due to the presence of -junctions i t t u r n s o u t to
mean field result T = ZEQ [8]. T h e parameter r is

where for our p a r t i c u l a r model

is T = z[( 1 p)Eo pE \ [11].
be smaller t h a n the s t a n d a r d
defined by the expressions

Tq

= (/)

l,

T = - ^

(9)

I n this paper we r e s t r i c t our a t t e n t i o n t o the r e p l i c a - s y m m e t r i c case Q p = Q

described by the unique g r o u n d state for each disorder c o n f i g u r a t i o n . C a l c u l a t i n g
the Gaussian i n t e g r a l over Q i n ( 6 ) - ( 8 ) we get
a

dr

(10)

a= l

I t is easy to see t h a t after an i d e n t i f i c a t i o n ip = ip a n d averaging over the

stochastic variable t(r) the G L f u n c t i o n a l (2) coincides w i t h H {ip} +
Hi {^}
(7), (10).
C o m p a r i n g the expressions obtained by these t w o methods we f i n d
7 = 5 + 1 / 2 . Note t h a t the r e p l i c a - s y m m e t r i c s o l u t i o n o f our p r o b l e m is valid only
for T > T or, e q u i v a l e n t s , for p < p ~ (E - y/E E /2z)/(E
+ *).
For larger
values o f p > p a t T <T
the s y m m e t r y between replicas is broken a n d the phase
d i a g r a m o f t h e system is more c o m p l i c a t e d .
I n this case i t consists o f n o r m a l
and s u p e r c o n d u c t i n g spin-glass-like phases w i t h nonzero average value o f t h e order
parameter Q pT h e physical properties o f these phases w i l l be studied i n details
elsewhere [11].
Let us summarize the results o f our analysis. For TD < bra or, equivalently,
for p < p - e, e ~ 1 0 ~ / c and a sufficiently h i g h t e m p e r a t u r e T > T^
there is
no global phase coherence i n our system and the a r r a y is i n t h e n o r m a l state.
Spontaneous current loops [4] can occur already i n this state provided i n d i v i d u a l
grains are s u p e r c o n d u c t i n g . Due t o the lack o f global s u p e r c o n d u c t i v i t y these loops
- i f present - are confined to the scale of order a a n d are completely uncorrelated
i n different parts o f the sample. For p <p e effect o f disorder is n o t i m p o r t a n t
a n d a t T = T^
the system suffers a usual second order phase t r a n s i t i o n i n t o a
global s u p e r c o n d u c t i n g state w i t h *f 0, correlated spontaneous c u r r e n t loops o f
the t y p i c a l scale ~ A j ; > a a n d s t a n d a r d Meissner properties i n relatively s m a l l
magnetic fields. N o W E occurs i n this state.
a

nt

en

en

For larger values o f p > p e effect o f disorder is s t r o n g and i n t e r a c t i o n

between c u r r e n t loops becomes crucially i m p o r t a n t . I n this case superconducting
domains w i t h an average size a n d c o n c e n t r a t i o n p (4) appear already above
TZ .
At T = T
these domains f o r m an i n f i n i t e p e r c o l a t i n g cluster and t h e
system becomes globally s u p e r c o n d u c t i n g . For T < T the system consists o f a n
i n f i n i t e s u p e r c o n d u c t i n g cluster a n d n o r m a l regions w i t h frozen-in magnetic field
c

en

768

and
all

ordered
main

arguments
samples
We
work
Grant

1.
2.
3.
4.
5.
6.
7.
8.
9.
10.
11.
12.

orbital

features o f
based

on

magnetic
WE
the

moments.

This

in superconducting
GL

free

energy

(1)

physical

ceramics
also

picture

[1].

We

describe

allows

to

explain

believe t h a t

WE

in

single

similar
crystal

[12].
would

was
No.

like

to

supported

thank
by

the

C.Bruder
Russian

and

D . K h o m s k i i for

Foundation

for

useful

Fundamental

discussions.
Research

This
under

93-02-14052.

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769