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Essential factors for the critical current density in superconducting MgB2: connectivity and flux
pinning by grain boundaries
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Abstract
Electrical connectivity and flux pinning strength of grain boundaries are essential factors in
determining the critical current density in superconducting polycrystalline MgB2 . The effect of
these factors is quantitatively investigated for a series of MgB2 bulk samples prepared by
various methods. The electrical connectivity is evaluated using the percolation model and the
obtained electrical connectivity is used for the estimation of the residual resistivity of
superconducting MgB2 grains. The elementary pinning force of grain boundaries is evaluated
using the theoretical result of Yetter et al based on the electron scattering mechanism with the
residual resistivity. It is found that the critical current density is approximately proportional to
the product of the electrical connectivity, the elementary pinning force of grain boundaries and
the reciprocal grain size. This confirms that the critical current density is dominantly determined
by the electrical connectivity and the flux pinning strength of grain boundaries. The flux pinning
property in MgB2 under the condition of full electrical connectivity is compared with that in
Nb3 Sn. The obtained result shows that the flux pinning ability of pure MgB2 is comparable to
or even higher than that of Nb3 Sn, indicating a much higher potential in carbon-doped MgB2 .
This proves that the MgB2 is a promising superconductor for practical applications.
1. Introduction samples fabricated by the usual in situ method was about 1.6
and 0.5 GN m−3 , respectively, for the reciprocal grain size
The superconducting transport property in polycrystalline of 4.3 μm−1 at 20 K. These values are much lower than the
MgB2 is free from the weak link problem which seriously maximum pinning force density of Nb3 Sn at 4.2 K [2], even
influences high temperature superconductors, and it is if the temperature-dependent factor is taken into account. The
empirically known that grain boundaries are dominant pinning small pinning force in MgB2 seems to be partly attributed to
centers in this superconductor. In addition, the product of deteriorated electrical connectivity by porosities and insulating
the condensation energy density and the coherence length, oxide layers.
to which the elementary pinning force is in proportion, is
The correlation between such a small critical current
comparable to that of commercial Nb3 Sn [1]. However, the
density and the electrical connectivity in MgB2 was discussed
pinning force by grain boundaries is significantly lower than
by Rowell [4]. Rowell defined the connectivity as
that in Nb3 Sn [2]. Recently Katsura et al [3] showed that the
maximum pinning force density of B4 C doped and nondoped ρg
K = , (1)
3 Author to whom any correspondence should be addressed.
ρ
2. Experimental details The critical current density of the samples at 20 K, which was
represented in [6], is shown in figure 2 again for convenience.
The polycrystalline MgB2 samples were made from the same The critical current density, Jc , increases monotonically
starting magnesium and amorphous boron powders and the with increasing packing factor, P . Figure 3 represents the
packing factor, P , was systematically changed in the range of relationship between the connectivity, K , and Jc in a self-field.
0.44–0.87 using different methods of synthesis. The details It is found that these are strongly correlated with each other
of the samples are described in the previous paper [6]. These but not in a proportional relationship. This indicates that other
samples have almost the same critical temperature, Tc , as factors which influence Jc may exist.
2
Supercond. Sci. Technol. 21 (2008) 015008 T Matsushita et al
8 10
8
6
7
4 5
3
2
2
0 0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
K
Figure 2. Magnetic field dependences of critical current density Jc at Figure 3. Relationship between the critical current density Jc in the
20 K for the polycrystalline MgB2 bulks with different packing self-field and the connectivity K .
factors.
and ωpl = 5.02 eV is the plasma frequency [10]. The In figure 4 various formulae are compared with experimental
reason for the above choice is that this provides suitable results on Nb. It can be seen that the present formula fits well
values of l and a good correlation between Ginzburg–Landau with experiments for αi < 3. Such a relationship has been
(GL) coherence length, ξ(T ), estimated from l and that from investigated only for Nb. However, the same relationship is
the upper critical field, Bc2 , with a suitable value of the also assumed for MgB2 and this formula is used in the analysis.
BCS coherence length, ξ0 , as will be shown later. The The GL coherence length ξ ∗ estimated from Bc2 at 20 K
obtained values are given in table 2. For the evaluation is given in table 2. The BCS coherence length ξ0 is adjusted
of ξ0 the superconducting energy gap seems to be useful. so that the GL coherence length ξ obtained from equation (4)
However, MgB2 has two energy gaps and it is not clear if with the estimated value of l coincides with ξ ∗ . Figure 5 shows
3
Supercond. Sci. Technol. 21 (2008) 015008 T Matsushita et al
0.8
6 6
0.7 6
2
5 3 5
3 2
4
0.6 4
1
ξ(0) / ξ0
0.5
5 1
0.4
0.3
4
0.2
10-2 10-1 100 101
αi
4
Supercond. Sci. Technol. 21 (2008) 015008 T Matsushita et al
4 0.5
5
5
0.4 5
3
4
0.3
3
1 2
2 0.2
2
3 3
1
1 0.1
2
1
0 0 0
0 0.2 0.4
K
Figure 6. Reciprocal grain size dependence of the maximum pinning Figure 7. Relationship between the electrical connectivity and the
force density of Nb3 Sn at 4.2 K (open square; left) and the normalized critical current density in the same flux pinning condition
compensated critical current density of MgB2 at b = 0.1 and 20 K at b = 0.1 at 20 K.
(solid circle; right). The line represents equation (9).
5
−3
with C = 0.451 × 10 N m for Fpmax in Nb3 Sn [2]. To
4
5
discuss the reciprocal grain size dependence of Jc of MgB2 , it 4
is necessary to compensate the effect of the degradation due
to the poor electrical connectivity and to normalize the flux
pinning strength of the samples. Jc of MgB2 normalized by 3
K f pn at b = 0.1 and at 20 K is plotted as a function of Dg−1
in figure 6 for comparison, where the solid line in figure 6
represents equation (9) with C = 0.330 × 104 A m−2 for 2
Jc /K f pn in MgB2 . It can be found that the proportionality 3
approximately holds between Jc and Dg−1 . 2
Since the effect of flux pinning is known for the pinning 1 1
force of grain boundaries and their effective number density,
the dependence of Jc only on the electrical connectivity, K , can
0
be discussed. If the simple pinning model that Jc is determined
only by the grain boundary flux pinning and the electrical
connectivity is assumed, equation (7) is predicted to lead to
Figure 8. Critical current density at b = 0.1 and 20 K versus the
K C f pn product of the essential factors for the critical current density.
Jc (b = 0.1) = (10)
Dg
with C f pn = ( fˆp /Baf )b=0.1 . Hence, this simply leads to current flows through thick insulating oxide layers. That is, if
Jc /K f pn = f (Dg ) as figure 6 shows. Now the normalized the pinning property is the same, Jc is expected to be simply
critical current density is defined as follows: proportional to K .
The above discussion clarifies that the electrical connec-
Jc tivity and the number density and the elementary pinning force
Jcn = . (11)
f pn f (Dg ) of pinning centers are important factors for the critical current
density. Figure 8 shows that the product of these factors can
This gives the Jc value normalized by the factors of grain reproduce the observed critical current density correctly,
boundary flux pinning, i.e. the pinning force and the effective demonstrating that equation (10) holds correct.
number density of pinning centers. If the simple flux pinning Firstly it is necessary to enhance the electrical connectivity
model described by equation (10) holds for the present series for the improvement of the critical current density in MgB2 .
of samples, Jcn is expected to be equal to K . The relationship The packing factor in in situ samples measured by Katsura
between Jcn and K is shown in figure 7. It is found that Jcn et al [3] is about 50% and hence the connectivity in these
is approximately proportional to K , indicating that Jc also samples is estimated to be as small as 10%. This shows that
reduces to zero when K reduces to zero. This result seems to be the critical current density in the non-doped superconductors
natural, since it is not realistic that superconducting tunneling would be comparable to that in Nb3 Sn, if the full connectivity is
5
Supercond. Sci. Technol. 21 (2008) 015008 T Matsushita et al
achieved. This shows that MgB2 is a promising superconductor connectivity and by a factor of 4 by reducing the temperature,
for applications. resulting in 96 GN m−3 at 4.2 K, which dramatically exceeds
In addition the flux pinning by grain boundaries is also a the maximum pinning force density in Nb3 Sn.
key factor for the achievement of high critical current density. Here the reason why the flux pinning in MgB2 is stronger
For this purpose it is desirable to reduce the grain size to a than that in Nb3 Sn is discussed. This can be partly attributed to
sufficient level and to enhance the flux pinning strength of grain larger values of Bc and ξ0 which affect the flux pinning force in
boundaries by making the superconductor dirty. equation (12). That is, a linear extrapolation of Bc (T ) to 4.2 K
Here, it seems to be important to discuss the flux pinning leads to 0.60 T [1] and ξ0 is 6.45 nm, which are larger than
strength of grain boundaries in MgB2 in more detail. It is Bc = 0.50 T [1] and ξ0 = 5.0 nm [8] in Nb3 Sn. The difference
not easy to generally apply the theoretical result of Yetter in these values contributes to the higher pinning ability in
et al for the elementary pinning force of grain boundaries MgB2 by a factor of 1.86. The remaining difference may be
in Nb to that in MgB2 , since it is fairly difficult to assume brought about by a larger numerical factor in equation (12),
typical superconducting parameters for Nb. For example, the probably due to the larger impurity parameter in MgB2 . A
Ginzburg–Landau parameter, κ , changes widely from sample proof of such superior pinning properties in MgB2 can be found
to sample. Hence, this theoretical result is not suitable for in very high Jc values in thin films [13].
correct evaluation of the pinning ability of superconducting For confirmation of the present conclusion and a more
MgB2 , although it seems to be useful for relative comparison of exact understanding of the flux pinning properties in MgB2
the same superconductor as used in this paper. For this reason it is required to carry out a systematic research on a series
the theoretical result of Zerweck [8] is used here. In the theory of samples with different grain sizes but with the same
the elementary pinning force of grain boundary per unit length connectivity.
of a parallel flux line for a superconductor with αi 0.34, One of the important results in this paper is that the
which is comparable to sample Bulk1, is predicted as pinning force of grain boundaries can be further improved
by making the superconductor dirty, and this is supported by
B ξ0 2
fˆp = 0.115 c , (12) the theoretical prediction of the electron scattering pinning
μ0 mechanism. Since pure MgB2 samples are fairy clean, a
which amounts to 0.43 × 10−4 N m−1 at 20 K. In the above remarkable enhancement of the pinning force can be expected.
Bc = 0.27 T [1] and ξ0 = 6.45 nm are used. The pinning force This speculation is consistent with the significant improvement
density takes a maximum at about B = 1 T (af = 48.9 nm) of the maximum pinning force density by C-addition [3]. In
in Bulk1. Substitution of fˆp , af and Dg into equation (7) addition, the C-addition also contributes indirectly to the flux
leads to 5.75 GN m−3 . Hence, the expected maximum pinning pinning through the enhancement of the irreversibility field
force density in Bulk1 is 0.28 GN m−3 , taking account of the which is assisted by the enhancement of the upper critical
connectivity K = 0.05. This value is about a quarter of the field [14]. This is helpful for the improvement of the critical
observed result, 1.2 GN m−3 . This disagreement seems to be current density at high fields. Since the condition of C-doping
caused by the underestimation of the elementary pinning force is not yet optimized from both aspects, there is a large room
in Zerweck’s theory. for further improvement of the flux pinning property in MgB2 .
Here the flux pinning characteristics in MgB2 is compared Thus, it can be concluded that MgB2 is a superconducting
with that of Nb3 Sn. In figure 6 the critical current density of material with very high potential for applications.
MgB2 at b = 0.1 at 20 K in the ideal case of K = 1 is directly
compared with the maximum pinning force density of Nb3 Sn 4. Conclusions
at 4.2 K. The enhancement factor of the maximum pinning
force density in MgB2 is evaluated when the temperature is Based on the analysis using the percolation model proposed
decreased from 20 to 4.2 K. The condensation energy density in our previous paper, the electrical connectivity of porous
and the irreversibility field are expected to approximately MgB2 bulk superconductor can be successfully estimated. This
increase by factors of 2.9 and 2.0, respectively. The pinning makes it possible to clarify the relationship between the critical
force density depends approximately on the magnetic field current density and the electrical connectivity. It was found
as B 1/2 up to the magnetic field at which the pinning force that the critical current density increased monotonically with
density takes the maximum value, and this magnetic field increasing electrical connectivity. However, the critical current
is proportional to the irreversibility field due to the scaling density was not proportional to the connectivity, but seemed to
property. Hence, the maximum pinning force density is have a finite value even in the limit of zero connectivity. This
expected to increase by a factor of 2.9 × 21/2 = 4.0. Thus, might suggest a superconducting tunneling current through
the maximum pinning force density in MgB2 at 4.2 K can insulating oxide layers. In order to clarify the reason for the
be expressed by equation (9) with C = 1.32 × 104 N m−3 . deviation from the proportional relationship the effect of flux
This value is 2.9 times as large as that in Nb3 Sn at the pinning on the critical current density was investigated.
same temperature. Therefore, it can be said that the flux The obtained electrical connectivity was also effective for
pinning strength in MgB2 is superior to that in Nb3 Sn. In estimation of the correct residual resistivity in superconducting
fact, the maximum pinning force density of sample Bulk1 is grains from the observed resistivity at 40 K. This information
about 1.2 GN m−3 at 20 K. Hence, this value is expected enabled us to estimate the electron mean free path, an
to be increased by a factor of 20 by achievement of the full important parameter in determination of the elementary
6
Supercond. Sci. Technol. 21 (2008) 015008 T Matsushita et al
pinning force of grain boundaries by the electron scattering force by making the superconductor dirty. One method is the
mechanism. With the aid of a new formula which relates the doping of C atoms, which has been proved to be effective
electron mean free path to the Ginzburg–Landau coherence in improving the critical current density. Thus, MgB2 is a
length, the BCS coherence length was estimated so that a good promising superconducting material, and the densification to
agreement is obtained between the GL coherence length led increase the connectivity and the optimization of the impurity
from the electron mean free path and that led from the upper parameter with C-addition is needed.
critical field.
The impurity parameter was determined using the new Acknowledgment
formula and the elementary pinning force of grain boundaries
was estimated with the aid of theoretical calculations by Yetter The authors would like to thank S Ohtsuka (University of
et al for each sample. It was found that the elementary pinning Tokyo) for the technical support in FE-SEM analysis.
force was not the same but was likely to have a larger value for
the sample with the lower electrical connectivity.
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