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HAL Id: jpa-00247143

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Submitted on 1 Jan 1995

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Antisuperconductors: Properties of Layered Compounds with Coupling

J.-P. Carton, P. Lammert, Jacques Prost

To cite this version:

J.-P. Carton, P. Lammert, Jacques Prost. Antisuperconductors: Properties of Layered Com- pounds with Coupling. Journal de Physique I, EDP Sciences, 1995, 5 (11), pp.1379-1384.

�10.1051/jp1:1995204�. �jpa-00247143�

(2)

Classification

Physics

Abstracts

74.20-z 74.50+r 74.62Dh

Short Communication

Antisuperconductors: Properties of Layered Compounds with

~r-3unction Coupling

J.-P.

Carton(~),

P. E.

Lammert(~)

and J.

Prost(~)

(~) Groupe

de

Physico-Chimie Théorique, ESPCI,

10 rue

Vauquehn,

75231 Paris Cedex OS, France

(~)

CEA/Service

de

Physique

de L'Etat Condensé,

CE-Saclay,

91191 Gif-sur-Yvette

Cedex,

France

(Receivedll Apri11995,

revisedl

September1995, accepted

19

September1995)

Résumé. Dans cette note, nous considérons les

propriétés

d'un

supraconducteur hypothé-

tique

composé

de couches

microscopiques, couplées

par effet

Josephson,

mais dont

l'énergie

de

couplage

est minimisée pour

une différence de

phase

de m. L'état de base a des

propriétés

fasci- nantes dues à l'effet combiné de l'ordre supraconducteur et des défauts structuraux du cristal.

Dans le cas de cristaux très

désordonnés,

on attend des

propriétés magnétiques exceptionnelles,

qui sont

compatibles

avec les observations dans

quelques supraconducteurs

cuprate haute-Tc d'un effet "Meissner

paramagnétique"

ou "Wohlleben."

Abstract. In this note, we consider

properties

of a

hypothetical superconductor composed

of

Josephson-coupled microscopic layers

witl~

tunnehng

energy minimized at

a

phase

diiference

of m. The non-zero

phase

offset in the

ground

state

engenders

an

intriguing interplay

between

the

superconductive ordenng

and structural lattice defects. Unusual

magnetic

properties are

expected

in the case of l~igl~ly disordered

crystals,

wl~icl~ are consistent with observations of a

'~paramagnetic

Meissner" or "Wol~lleben" effect in

higl~-Tc

cuprate

superconductors.

Layered superconductors composed

of

essentially

two-dimensional

layers coupled

to each other

by Josephson pair tunneling through

normal

layers,

have been known for some

time,

the earliest

examples being

intercalation

compounds

[1]. The

widely

believed

[2,

3] idea that trie

high-Tc cuprate superconductors

also

belong

to this

dass,

of which there is some

expenmental

evidence

[4, 5],

has renewed interest in such materials.

The dassic theoretical framework for

descnbing

these

systems

is the Lawrence-Doniach model

[3, 6].

The free energy contains a

magnetic contribution,

and contributions from intra-

layer ordering

and

inter-layer Josephson couphng.

To a

good approximation, except

very near

Tc

or in the cores of

vortices,

the

magnitude

lbo of the

superconducting

order

parameter

is

@

Les Editions de Physique 1995

(3)

1380 JOURNAL DE PHYSIQUE I N°11

constant,

and in that case, one can write the latter two

pieces

of the free energy

simply

m

terms of the order

parameter phase

as

F =

j~~ £ /d~x(

Vjj@n

~~Ajj

8x À~b

n

'o

~

Îd2 ~°~~~~~~ °~~

~

lx / ~~~~~~~'

~~~

where @n is the order

parameter phase

in

superconducting layer

n, and

~~ ~n+1)d

@]+~ =

@n+i

@n

/

A

dl

(2)

4io nd

is the

gauge-invariant phase

difference across

junction layer

n. The

penetration lengths

asso-

ciated with currents in the a-b

planes

and between them

(Josephson current)

are denoted Àab and

Àj respectively,

and ~ %

Àj /Àab

is the

anisotropy

ratio.

The form of this

expression

is dictated

by

gauge invariance

plus

translations in the a-b

plane

and rotations about the axis

perpendicular

to the

planes (z

or

c). Imposing

also time-reversal invariance

requires

F to be

unchanged

under @n -

-@n,

A -

-A,

and

parity

under n - -n,

Az

-

-Az.

In either case, @o is then constrained to be

0,

the usual

value,

or x. The

Josephson

term has its

origm

in a form

cxlb(~~lbn

+ c-c-, is

quadratic

in the

Ginzburg-Landau

order

parameter

field ~b. If the coefficient cx is

small, (which requires

some

explanation iii) higher

order terms can shift the minimum of F to

arbitrary

(@n+i @n(, even in the presence of the discrete

symmetries. However,

@o and

-@o

would be

degenerate.

Mechanisms which could

produce

@o

#

0 in the

ground

state have been descnbed in dis- cussions of

single Josephson junctions, originating

in

strong

Hubbard interactions [8] or local

paramagnetic

moments [9] in the

junction,

or Andreev reflection in a normal metal

junction iii.

Although

discussed in the context of

single macroscopic junctions

or grain boundaries

[10, iii,

the

possibility

of

x-coupling

as an intrinsic feature of bulk

systems

appears not to have been considered. In this note, we discuss

implications

of @o

= x, which we propose to call "antisu-

perconductor."

For a

perfect crystal,

most

properties

are

completely

insensitive to the value of @o.

Unique

features which occur for an

imperfect crystal having

@o = x are the

subject

of this letter. In the

case of a

perfect crystal,

a

simple

redefinition of the

phase

elimmates @o

" x: @n - @n + nx,

without

altering

the vector

potential

A. An alternative method is to

replace

A

by

A + a in the

inter-layer coupling

term of

equation il),

where a is an additional fictitious gauge

potential

such that

~~ <n+i)d

4lo

Id

~ ~~ ~' ~~~

For instance, one may take

~~

ÎÎ~'

~~~

where iî is a unit vector

along

the local normal to the

layers. Gauge

transformations with a

taking

the

place

of A are then

possible.

This latter

approach

is more convenient in the presence of dislocations.

Dislocations

Suppose

that our

antisuperconductor

contains a dislocation of the

layered

structure with

Burg-

ers vector b

parallel

to the average

layer

normal 1

[12],

b =

(bd)à,

b E

Z, (5)

(4)

and with

arbitrary

line director.

The definition of a introduced in the

previous

section is now

generalized by imposing

Î /~

a dl = nC2r

16)

where ne is the number of

insulating layers through

which

path

C passes in the

positive

sense minus the number

passed through

in the

negative

sense. In that case, we have

ia.dl=-)b Ii)

for a dosed contour

encircling

the dislocation line. This gauge formulation is

analogous

to that introduced

by

de Gennes

[13]

for dislocations in smectics-A.

Generally,

even when

Jz

is small

compared

to the critical current

Jo

"

4xàc(cx(~b(/4lo

"

(c4lo/8x)(1/à]d),

1e. the system is

only slightly

disturbed from the local energy

minimum,

neither a non the

gradient

V@ of a smooth

interpolation

of

through

a

junction layer

is small within the

junction. However,

the combination

Vi

e V@

Îa (8)

lbo

is

small,

if we

appropriately

resolve the 2x

ambiguity

m the

change

of across

junction layers.

Although Vi

is then

always well-defined, #

is not a

single-valued

function in the presence of dismclinations.

In regions where the current

density j

is

small,

it can be

expressed

as

~~

A~ j

=

~° Vi

A.

(9)

where A is the tensor of

penetration lengths:

A~

=

À(iîé

+ À(~

jr éil). (10)

Quantization

of the total

magnetic

flux 4l borne

by

a dislocation reads in

gel~eral

u%)=)jÎV#.dl=~+n,

nez.

iii)

o X 2

The

coarse-grail~ed magl~etic

field

obeys

h + V x

(A~

V x

h)

= u

4lo162(x), i12)

where 62 is a delta-ful~ctiol~ distribution with

support alol~g

the dislocation

inormalized by arc-length).

The

corresponding electromagnetic

energy is

proportional

to

u~.

For

screw dis-

locations,

an additional

n-dependent

condensation

penalty

associated with a normal cote may

occur.

Two cases are now to be

distinguished:

ii

b odd. The minimum energy is obtained for u

=

+1/2.

A

magnetic

flux hue carrying flux

4lo/2

is bound to the dislocation. The

sign

of the flux is

arbitrary, reflecting

time-reversal

invariance of the Hamiltonian.

(see

also Ref.

[14])

ii)

b even. The

system

is not frustrated and the

ground

state has v

= 0.

The formalism admits excited state solutions with additional

integer multiples

of

4lo along

the dislocation. Just as in

ordinary superconductors, however,

such

configurations

should be

(5)

1382 JOURNAL DE

PHYSIQUE

I N°11

ul~stable to

splittil~g

into

multiple

vortices of minimum allowed flux. In

conclusion,

a dislocation will

produce

a

spontaneous

local

magnetization

if the

Burgers

vector is of odd

strength.

The

magnetization

is

parallel

to the direction of the dislocation line:

parallel

to the

layers

for

edge

dislocations and

perpendicular

for screw dislocations.

The

binding

energy between the

4lo/2

vortex and an odd

Burgers

vector dislocation is in- finite in the sense that the relative energy of the

superconducting

state

containing

the naked dislocation is

divergent

in the

system

radius. Under the action of a

Magnus

force

resulting

from an electrical current, the vortex could be

pulled

off the

defect;

a new

ihalf)

vortex would be created

spontaneously

to

replace

it. These are

essentially linear,

rather than

point like, pins,

so a

single

defect can

compete

with the Lorentz force.

Unfortunately,

it appears

quite

diilicult to calculate the

pinning

force.

The

foregoing applies

to vortices associated to either an

edge

or screw dislocation. Their

shapes

and core structures are

quite different, however,

and

consequently,

so too are their

energies.

We consider them

separately.

i) Edge dislocation,

b

= 1.

The

large-scale

structure of currents and

magnetic

field for this vortex is very similar to that

of a vortex oriented

parallel

to the

layers

of an

ordinary superconductor [15,16],

aside from

rescaling by

a factor of u

i= 1/2). Again

as in that case, smce

(c $ d,

no normal core is

required.

The vortex is

elhptical

in

cross-section,

with

major-to-minor

axis ratio ~. The core

of the vortex

iwhich

is not in the normal

phase)

has width d in the c-direction and

~d along

the

planes.

This is the

region

m which the

nonlinearity

of the governmg

equations

comes into

play.

The energy pet unit

length

is evaluated as m references

[15]

and

[16]:

~~~g~ ~

jij~ 40~

~ ~~ Cil(

~Î)~ ~ÎÎ)

~

a~Àj

~~

~Î~'

~~~~

The

prefactor

of

1/4

reflects the

magnitude

of the flux.

ii)

Screw

dislocation,

b

= 1.

The distortion of the lattice which occurs here leads to additional

coupling

between the

in-plane

and

Josephson

currents since

they

are no

longer purely perpendicular

or

along1, particularly

close to the dislocation.

However,

this turns out to be a minor

perturbation [17]

on the limit

d/Àab

" 0 with

Jo

fixed. In this latter

situation,

it is dear that one has a vortex with

purely in-plane

currents. It possesses a normal core of radius

(ab,

and is unremarkable

except

for the value of

magnetic

flux which it carries. The vortex has

inearly) cylindrical

symmetry and a radius

Àab.

Its

energy/length

is

simply

~~~~~~'

~

~

~

Îb

~~

Il 4)

One

might

think that the

system

would

prefer

to

replace

the normal core with one m which the

Josephson coupling

is

completely

frustrated. In

fact,

such a deviation of the

inter-plane phase

difference from

x can

only

heal over a distance

mJ

Àj

and this would cost an energy or order

(4lo/4x)~il/d~)

A similar remark

applies

to the

proposal

of

having

a

phase

difference

of zero across the extra

half-plane insulating layer

of the

edge

dislocation. This would result

m zero current

everywhere,

but would also have an energy which

diverges linearly

with the

system size.

The choice of sign for 4l

=

+4lo/2

for an isolated dislocation m the absence of extemal field entails

spontaneous breaking

of the time-reversal

symmetry;

the two

signs

are

equally probable.

(6)

However,

the vortices associated with two dioEerent dislocations interact. The range of the

pair

interaction is as usual the

penetration depths

of the associated field. For a screw

dislocation,

this is

Àab,

and for an

edge dislocation,

it is

àab

in the z-direction and

àj parallel

to the

layers.

Two

roughly parallel

dislocation lines within interaction range of each

other,

but distant

enough

that the cores are distinct will carry

anti-parallel

flux. Dislocations fines which are

separated

by

much less that the interaction range should behave as a

single

dislocation of even

Burgers

vector and therefore not carry any

magnetic

flux at all. A dislocation fine which spans the entire

sample

can

provide

return flux for another

such,

and since the

magnetic

field is not screened outside the

sample,

the

corresponding

interaction is

long-ranged.

Under zero-field

conditions,

a

sample containing

defects will therefore

display randomly

oriented frozen

magnetic

moments what one may call an

Ising

hne

glass.

These lines could be observed

by

standard decoration

techniques

since

they

are insensitive to the direction of the

magnetization.

An external field will be able to orient the flux lines

only

if it exceeds

Hc,

in

strength.

Full vortices with the favorable

sign

will then

penetrate

the

sample

and annihilate

"misaligned" 4lo/2 vortices, leaving

a net

alignment.

This behavior does not lead to observations

strikingly

dioEerent from conventional

superconductors. However,

under field-cooled conditions a

paramagnetic

response of the moments associated with

sample-spanning

dislocations should be observable. Such a

"paramagnetic

Meissner effect"

[10,11,18,19] (PME)

is

expected

for any field direction in a

single crystal having

all

types

of dislocations. To overcome the

interaction,

the external field must still exceed some coercive threshold which will

depend

on its direction as well as the distribution of defects. For

example,

screw dislocations will become

aligned

for

Hz

>

Hj°~~,

where we can estimate

jfcoer ~

~0

XÀab ~~~

~-D

/À~j,

(~ ~)

~

4xà(~

2D '

where D is the average distance between defects. This estimate is

simply

the field of a

4lo/2

vortex at a distance D. Note that it is

vanishingly

small close to the

normal-antisuperconductor

transition.

Discussion

Symmetry

considerations have led us to

postulate

the existence of

"antisuperconductors"

which differ from conventional

superconductors

m a subtle but

significant respect.

We now consider the likelihood of

finding

a matenal with such a

phase,

or whether

they

have

perhaps already

been observed.

i)

The existence of

spontaneous

currents due to the presence of

x-Josephson junctions

has been invoked

by

several authors to

explain

the

paramagnetic

Meissner effect observed in some CUO based

high-Tc superconductors.

These

x-junctions

were assumed to dwell in

intergranular

links

[10,11,18,19].

We stress that such an effect may also arise from more intrinsic features such

as

topological

defects of the

layered

structure common to all these

cuprate compounds.

If so, the

microscopic tunneling

mechanism between CUO

planes

as trie ongm of trie

x-coupling

would prove to be fundamental. In view of trie

complexity

of the

interlayer regions,

the

possibility

of x

couphng

cannot be ruled out at

present.

Dislocation-bound vortices could reconcile the

contradictory

remarks of Braunisch et ai.

[10]

"The persistence of trie PME after

powdering

mdicates...that these weak links are

intragranular."

The

density

of dislocations

(or B)

can be estimated from the value of the field at which x = 0: H cf 0.5 Oe

[loi yields

an average inter- defect distance of a fe~. microns. The

sample

obtained after

powdenng ito

a size of 2 3

~tm)

would contain about one defect per grain, which

gives

the

strongest

PME. The most condusive evidence for these

spontaneously

created vortices would be

provided by

decoration

experiments

on zero-field cooled

samples.

(7)

1384 JOURNAL DE

PHYSIQUE

I N°11

ii)

Such

antisuperconductors might

be

deliberately engineered,

smce the

technology

now

exists to build up

layered compounds layer-by-layer [20].

In this case, one or several atomic

layers

are intercalated between the

superconducting

sheets.

Josephson coupling

arises

through hopping

on these intermediate sites. While the

sign

of o

is

positive

for direct

tunneling,

it can have either

sign

for indirect

tunneling.

In

particular, tunneling

ma localized

magnetic impurity

sites was studied

long

ago

by

Bulaevskii et ai.

[6,17].

They

showed that the

junction

current is the difference

Jo Js

of two terms, the latter

being

related to the

spin-dependent tunneling amplitude.

The

difference,

hence cx, can be

negative

if the second term is

large enough:

the reader is referred to the

original

papers for a discussion of the

required

conditions. A

transparent

formulation of these

phenomena

was

given by Spivak

and Kivelson

[5]. They

observed that

transfernng

a

pair

via a

singly occupied

site results in

a

sign change

of the

pair

wave

function, giving

a <

0, provided

that the intra-site Coulomb interaction is

strong enough

to enforce

single

occupancy. These observations indicate a direction to follow in

attempting

to fabricate

insulating x-junctions.

The most

interesting

behavior of

staggered superconductors

is the very unusual interaction of the

superconducting

order with lattice defects. This

provides

one

experimental signature, precisely

the

paramagnetic

Meissner effect

IPME)

which has been

reported

for some

high-Tc

materials

[loi. Josephson junctions

between such a material and an

ordinary superconductor behave, perhaps

rather

surprisingly,

in an

entirely

conventional manner, and therefore do not

provide good experimental

tests unless it is

possible

to observe the

complicated

counter-

propagating

current

pattem.

It may be that some

currently

known

layered superconductor belongs

to the dass described here.

Antisuperconductors

could also be

engineered

at the

mesoscopic level,

once a way were found to

produce

x

Josephson junctions.

References

[1] Gamble F-R-, di Salvo F-J-, Klemm R-A- and Geballe T.H., Science 168

(1970)

568.

[2]

Chakravarty

S., Sudb@A., Andersen P-W- and

Strong

S., Science 261

(1993)

337.

[3] For a review, see

Feinberg

D., J.

Phys.

iii France 4

(1994)

16.

[4] Kleiner R.,

Steinmeyer

F., Kunkel G. and Müller P.,

Physica

C185-189

(1991)

2617.

[SI Kleiner R. and Müller P.,

Phys.

Reu. B 49

(1994)

1327.

[6] Lawrence W-E- and Doniach

S.,

Proc. Conf. Low

Temp.

Phys. LT12

(1970)

361.

[7] Altsl~uler B-L-, Kl~meInitskii D.E. and

Spivak B-Z-,

Sohd State Comm. 48

(1983)

841.

[8]

Spivak

B-I- and Kivelson S-A-

,

Phys.

Reu. B 43

(1990)

1tC3740.

[9] Bulaevskii L.N., Kuzii V.V. and

Sobyanin

A.A., Sand State Comm. 25

(1978)

1053.

[10] Braumsch W. et ai.,

Phys.

Reu. Lett. 68

(1992)

1908.

[Il]

Chen D.X. and Hemando A.,

Europhys.

Lett. 26

(1994)

365.

[12]

In-plane

components of tl~e

Burgers

vector bave been

ignored

here

smce

tl~ey

are irrelevant to the present discussion.

[13] de Gennes

P.-G.,

Sand State Comm. 10

(1972)

753.

[14] Villain J., J.

Phys.

C10

(1977)

4793.

[15] Carton J.-P., J. Phys. f

France1(1991)

113.

[16] Clem J-R-,

Coifey

M.W. and Hao Z.,

Phys.

Reu B 44

(1991)

2732.

[17] Carton J.-P., Lammert P. and Prost J., unpublished.

[18] Braumsch W. et

ai., Phys.

Reu. B 48

(1993)

4030.

[19] Heinzel

Ch., Theilig

Th. and Ziemann

P., Phys.

Reu. B 48

(1993)

3445.

[20]

Laguës

M. et ai., Science 262

(1993)

1850.

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