Applied Svprrconduclivity Printed in Great Britain.
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Vol.1, Nos l-9. pp. 925 - 933. 1993 All rights reserved
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SUPERCONDUCTING
CERAMICS
T. Grenet
Laboratoire
and M. Cyrot
Louis NCel, CNRS, BP 166,38042
ABSTRACT:
Grenoble Cedex 9, France
Unusual forms of resistive superconducting
transition
have been observed in some n-type cuprate ceramics. Their shape are strongly magnetic field dependent.
In some cases, the transition shows
a double peak behavior : the resistivity presenting reaching
zero. This behavior
two maxima before
and its change with magnetic
been explained by an interplay between the superconducting of the grains and the Josephson temperature
field has transition
of the intergranular region.
We present a model based on a self consistent medium approach which describes the various behaviors one can observe in these ceramics. Superconductivity interest
has been
superconductors studied2
in granular systems has always attracted a lot of attentionl. further
enhanced
since
the discovery
of high
This
temperature
because of the intrinsic granular structures of the ceramics. We have
the
superconducting
properties
of the
electron-doped
compounds
Ln2_xMxCu04_y (Ln = Pr, Nd, Sm, Eu ; M = Ce and Th). The granular structure of the sample influences
strongly the superconducting
behavior.
resistive transition have been observed, sometimes In this paper
,after reviewing
the different
Some unusual forms of the
causing a “double peak” transition.
behaviors
we have observed
in these
ceramics, we develop a model to interpret it. The sample is described as a colIection of superconducting concentration
grains with a distribution
of Tc due to the strong dependence
of oxygen and Ce or Th. The intergrain
ability to permit
a Josephson
described
via a distribution
materials
is the resistivity
current
between
of Josephson
region is described through the
the superconducting
temperature.
of Tc on
grains. This is
The third characteristic
of the grains and of the intergrain
of the
regions. We develop a
theory based on a self consistent medium. The different behaviors that we observed are due to the interplay temperatures.
between
the Josephson
The behavior under a magnetic
change of the Josephson temperature
with field. 925
and the superconducting field is mainly explained
critical
by the rapid
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The behavior of the r~istivity versus tempcratur~ strongly depends on the sample. Moreover for a given sample it strongly changes with magnetic field. The different behaviors are so anomalous that they seen unreasonable at first sight.
T (K)
3.0
,
,
,
,
[
,
,
,
,
,
,
-
2.5 b- 1 kOe 2.0-
d- 30 kOe e- 59.6 kOe
1.5-
.50
’ 0
lo
’ ’ 10
’ ’ 15
kg ’ 20
’
I 25
’
30
00
1: resistivity versus temperate fields for a Nd-Ce-Cu-0
’
T (KI
T (K) XI
cc> &me
’ 5
curves measured at different magnetic
sample (a), a Pr-Th-Cu-0
sample (b), a
Sm-Ce-Cu-0 sample (c) and a Eu-Ce-Cu-0 sample.(d). Some are well behaved in the sense that the resistivity in zero field strongly decrease at Tc and under magnetic field Tc (H) justdecreases (fig. la). In figure lb, we show one sample which is reasonably well behaved under zero field but in intermediate field has a
World Congress on Superconductivity
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knee below Tc. In figure lc, we observe that below Tc the resistivity decreases to a minimum, then increases before decreasing to zero with temperature. This maximum of resistivity increases with magnetic field. In figure ld, after the minimum below Tc the resistivity increases up to the lowest temperatures used in our experiment. We also note in this case that the resistivity just below Tcg is larger in very low field than in high field. Figure 2 shows the behavior of a sample of Sm&eo.1$u03,97 which presents this so strange double peak behavior. Below the critical temperatu~ of the grains there are two maxima in the resistivity versus temperature.
1.8 r
1RfRf30K)
Tonset
1.2
0.60
0.0
f;,irrure2: resistivity versus temperature curves measured under different fields for a Sm-Ce-Cu-0 sample We first give the qualitative explanation for the following three unusual behaviors a) b)
increase of resistivity below Tcg minimum of resistivity at Tmin and further increase of resistivity below Ttin
behavior at very low temperature c> increase to the lowest temperature used.
:
either decrease to zero resistivity or,
For behavior “a” suppose that we have a range of grain critical temperatures in between Tcmax and Tcmin which is likely to occur as Tc is strongly dependent on all concentrations3. Some grains below Tc map become superconducting. In between two superconducting grains conduction is due to tunnelling and the intergrain resistivity increases with decreasing temperature. This can cancel the decrease of resistivity due to the transition of the superconducting grains. The distribution of Tc is peaked near a temperature Tonset and below this temperature a large number of grains become superconducting and the resistivity strongly decreases.
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For behavior “b”. When most grains are superconducting at Tmin the resistivity is due to the intergrain region. The behavior of the tunnel junctions makes the resistivity increase when decreasing the temperature, producing the observed minimum. For behavior “c”. If the tunnel junctions have low enough resistivity a Josephson Current can occur and the resistivity if the junctions will decrease to zero giving a zero resistivity to the macroscopic sample. IF the tunnel junctions have large resistivity no Josephson current can occur and the resistivity always increases with decreasing temperature. This qualitative explanation relies on conventional superconductivitfl.
It requires
first that the intergrain resistivity is of the order of the grain resistivity. This requirement was not fulfilled with usual conventional superconductors(l). Secondly it requires that the temperature below which Josephson current occurs is lower than the critical temperature of the grains. In order to build the model, we have use an effective medium approach due to Landaue# for the calculation of the resistivity. In this approach the medium is described using two kind of grains A and B defined by their different conductivity OA and bg. The medium has an effective conductivity on obtained by assuming that on the average, the polarizability created by a grain A or B in this effective medium is zero. This model has been refined by Yoshida(6) and applied to grains which have a core and a shell made of different materials. In the following we will use this particular refinement. We have to describe the following situations -
:
two normal grains with a resistive junction
- two superconducting grains linked by a Josephson current - two superconducting grains linked by a resistive junction when the temperature is larger than the Josephson temperature - one normal grain and one superconducting grain with a resistive junction. Thus we introduce the following type of cells made of a core and a shell
:
a)
a normal core surrounded by a normal shell
b)
a superconducting core surrounded by a superconducting shell
c>
a superconducting core surrounded by a normal shell.
The cores represent the grains which can be either normal or superconducting depending on the temperature and the magnetic field.
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TABLE I cell
Reasons
Ratio x;
Normalcore
T > Tc (0) or H > Hc2 (T)
1 -cs Cs2 Cj
i=3
Superconducting shell
H
Superconducting core
H < Hc2 (T)
fT Cs2 (1-Cj)
i=4
Tunnel junction
and superconducting neighbor andT>Tj fT (1-Cs) cs
i=S
HTj
(l-fT) Cs2 (l-cj)
i=6
or H c Hc2 (T)
(1-f$ cs (l-C@
i=7
Normal shell Superconducting core
i=l i=2
or H < Hc2 (T) and normal neighbor Superconducting core Weak link
and normal neighbor
The shell represents the intergrain region. A normal shell can be either a tunnel junction or a weak link. A superconducting shell is a junction with a Josephson current. In table 1, we describe the different types of cells, the reason of their appearance and the probability of appearance. Cs is the probability that a grain is superconducting, Cj is the probability that the junction i.e. the shell is superconducting which happens for T < Tj where Tj is the Josephson temperature of the junction. fT is the ratio of tunnel functions. Thus l-fT is the ratio of weak links. We have seven types of cells. The main approximation in the model is that we have excluded correlations between the shells of neighbo~g
cores. The self consis#nt equation reads
igl = = Xi Si
0
where Si is the normalized conductive
of the cell i. To calculate it we assume that
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all the cells have the same size
- the normal core has resistivity Oid - the junction has resistivity Gin which does not change when the grains become superconducting
for weak links or which becomes activated in the case of tunnel
junctions. In order to describe the inhomogeneity
of the system, we consider a distribution
function for the critical temperature of the grains, a distribution function of the normal resistance of the junctions, the latter will permit to calculate the critical current and the Josephson temperature of the junction. When we apply a magnetic field, in order to calculate the ratio of the superconducting grains as a function of T and H we introduce two experimental parameters dHc2 Cab) dHc;! 6) T=Tc,and the London penetration depth XL. In order T=Tcand dT dT to describe the effect of the field on a junction, we introduce a third distribution junction which gives the distribution of size of the junctions and, assume that the critical current, hence the Josephson temperature follows
where @ is the flux into the junction. All these data permit to calculate the seven normalized conductivities.
In order to
decrease the number of parameters, we take for the distribution of resistance and size of the junctions
:
D(L)
=k
ifL<&
=o
ifL>&,
and D(R)
=&ifRR,,
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TABLE II Lax = 0.5 pm R,=Rco+500A 0,x = 103 (Qm)-l
(3,o = 1.2 105 (Qm)-1 dBc+) = - 0,2T/K dT
dBq(a,b) = dT
- 5
fT = 0.70
T/K
Table II gives in the first column the parameters used in our calculation which are either given in the literature or measured independently. The second column gives the values of the parameters that we have adjusted to fit the experimental curves. On figure 3 we show two sets of curves in order to show the effect of fT the number of tunnel junctions. 7.0
I
1
50 kOe
I
1
I
,30-,
I
H=
I
I
I
I
I
1OkOe
6.0 5.0 4.0 3.0 2.0 1.0
H-O
q.
0.0 0
5
20
10
25
T(I(;S
(a>
I
0.0
0
4 *Vf2
l6
2o
0.9
Figura: calculated resistivity curves using the parameters values listed in Table II and: fT = 0.5 (a) and fT = 0.3 (b). The temperature dependance of the normal state resistivity is omitted.
The height of the maximum is strongly increasing with this number. This permits us to evaluate the ratio of tunnel junctions compared to weak link by fitting this maximum. The position of this maximum with field permits to determine the average value of the size of the junctions. The distance between T,., and Tonset gives indication on the range
932
World Congress on Superconductivity
of T, in our materials. Thus by analyzing the shape of the curves of resistivity versus temperature one can extract a lot of informations on the granularity of the system. In figure 4 we give a particular fitting of a Sm Ce Cu 0 sample.
1
0
mre
5
10
15 T (K)
4: compared experimental
20
25
30
(with experimental
points) and
calculated resistivity curves in the case of a Sm-Ce-Cu-0 sample.
In conclusion, we have shown that the curves resistivity versus temperature as a function of magnetic field can present a lot of unconventional behavior. By fitting this behavior with a simple mean field theory one can extract impo~~t ~owledge
on the
granularity of the system, for instance the range of critical temperature. Note that the highest critical temperatures of the grains correspond to the temperature below which the resistivity deviates from the normal state behavior (restored under high enough magnetic fields) and that the transition of these grains to the superconducting state causes an increase instead of a decrease of the global sample’s resistance. We can also extract the size of the junction, the ratio of tunnel versus weak links and the Josephson temperature of the junctions. By measuring the resistivity after treatments, one can also follow the evolution of the junctions’ characteristics.
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REFERENCES
1. Y. Shapira and G. Deutscher,
Phys. Rev. B 27,4463
(1983).
2. A. Gerber, J. Beille, T. Grenet and M. Cyrot, Europhys.
Lett. 12,5,441
(1990).
A. Gerber, T. Gerber, M. Cyrot and J. Beille, Phys. Rev. Lett. 65,320l
(1990).
3. J.T. Market-t et al, Physica C 158, 178 (1989).
4. See for instance,
M. Cyrot and D. Pavuna, Introduction
high Tc superconductors.
5. R. Landauer,
World Scientitic 1992.
J. Appl. Phys. 23, 779 (1952).
6. K. Yosida, J. Phys. C : Solid State Phys. 15, L 87 (1982). Phil Mag 53,55 (1986).
to superconductivity
and