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Article history:
Received 14 September 2008
Received in revised form 1 January 2009
Accepted 18 January 2009
Available online 29 January 2009
PACS:
74.70.b
74.72.Jt
74.62.Bf
74.25.Qt
a b s t r a c t
The dielectric properties of Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d (y = 0, 0.5, 1.0, 1.5) superconductor samples were studied at 79 and 290 K by means of capacitance (C) and conductance (G) measurements with
the test frequency (f) in the range of 10 KHz to 10 MHz. A negative capacitance (NC) phenomenon has
been observed, which is most likely arising due to higher Fermi level of ceramic superconductor samples
than metal electrodes. Also the NC may be due to the space charge located at the multiple insulator
superconductor interfaces (grain boundaries) in the materials. The negative dielectric constant (e0 ) and
loss factor (tan d) show strong dispersion at low frequencies. The lower thermal agitation at 79 K may
enhance the polarizability and hence the dielectric constants (e0 and e00 ).
2009 Elsevier B.V. All rights reserved.
Keywords:
Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d
superconductors
Dielectric constant
Polarization
Capacitance
Conductance
1. Introduction
Although the cuprate superconductors have extensively been
characterized but there is a very little work done on their dielectric
properties. In the homologous series of Cu0.5Tl0.5Ba2Can1Cun
O2n+4d superconductors, the most attractive candidate is Cu0.5Tl0.5
Ba2Ca2Cu3O10d (CuTl-1223) due its lower anisotropy, higher critical temperature (Tc) and higher critical current density (Jc) [1,2].
This compound has Cu0.5Tl0.5Ba2O4d charge reservoir layer and
three conducting CuO2 planes. The normal pressure synthesis of
bulk (CuTl-1223) superconductor is very simple and economical
for large-scale production of this material for device fabrication.
Bulk as well as thin lms of (CuTl-1223) superconductor have been
prepared and extensively characterized [15]. The Ca atoms separate the conducting CuO2 planes and consequently the wave function of the Ca atoms develops a correlation among the carriers in
various CuO2 planes. Also the coupling between the CuO2 planes
in oxide superconductors plays very important role in enhancing
the superconducting volume fraction. The coupling strength of mo* Corresponding author. Tel.: +92 52 90642122/51 90642091 (Lab); fax: +92 51
9210256.
E-mail address: mmumtaz75@yahoo.com (M. Mumtaz).
0921-4534/$ - see front matter 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.physc.2009.01.010
2. Experimental
The Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d samples are prepared
by solid-state reaction method accomplished in two stages. At the
rst stage Cu0.5Ba2Ca2yMgyCu0.5Zn2.5O10d (y = 0, 0.5, 1.0, 1.5) precursor material is synthesized by using Ba(NO3)2 (99%, Merck),
Ca(NO3)2 (99%, Merck), MgO (99%, BDH Chemical Ltd. Poole England), Cu2(CN)2 (99%, BDH Chemical Ltd. Poole England) and ZnO
(99.7%, BDH Chemical Ltd. Poole England) as starting compounds.
These compounds are mixed in appropriate ratios and grinded in a
quartz mortar and pestle for about an hour. After grinding, the
material is loaded in a quartz boat for ring in a furnace at
860 C. The material is red twice following one hour intermediate
grinding. The precursor material is then mixed with Tl2O3 (99%,
Merck) to give Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d (y = 0, 0.5,
183
1.0, 1.5) as nal reactant composition. Thallium oxide mixed precursor material is pelletized under 3.8 tons/cm2 pressure. The pellets are wrapped in a thin gold foil and sintered at 860 C for
10 min, followed by quenching to room temperature. The rectangular bar shaped samples of dimensions 2 mm 2.5 mm 10 mm
are used for dc-resistivity and ac-susceptibility measurements. The
resistivity of the samples is measured by four-probe technique and
ac-susceptibility measurements by mutual inductance method
using SR530 Lock-in Amplier at a frequency of 270 Hz with HAC =
0.7 Oe of primary coil. The structure of material is determined by
using X-ray diffraction scan (D/Max IIIC Rigaku with a Cu Ka
source of wavelength 1.54056 ) and cell parameters by using a
computer program. The frequency dependent dielectric measurements are performed with HewlettPackard 4275A Multi-Frequency LCR Meter from 10 KHz to 10 MHz. The conventional
two-probe technique is used for the measurements. Silver paint
is applied to both the surfaces of the sample and the copper leads
were xed to the silver electrode surfaces. The sample is mounted
on the sample holder. The experimental set up for dielectric measurement is shown in Fig. 1. For the room temperature (290 K)
measurements the holder is kept out side the liquid nitrogen
dewer and for the measurements at liquid nitrogen temperature
(79 K) the holder is lowered in the liquid nitrogen dewer. By measuring the capacitance (C) and conductance (G) of the samples, the
dielectric constants (e0 and e00 ), dielectric loss (tan d) and ac-conductivity (rac) of the samples were determined using following
expressions [17]:
Cd
Ae0
Gd
xAe0
e0
e00
e
e0
rac xe0 e0 tan d
1
2
00
tan d
3
4
0.36
(cm)
0.45
y=0
y = 0.5
y = 1.0
y = 1.5
0.27
0.18
ac(emu/gm)
184
0.09
0.00
100
6
0
-6
-12
-18
-24
-30
-36
y=0
y = 0.5
y = 1.0
y = 1.5
80
150
200
250
Temperature (K)
300
0.0 a
79K
y=0
y = 0.5
y = 1.0
y = 1.5
-2.0x10
-4.0x10
-6.0x10
-8.0x10
0.00 b
290K
-1.40x10
-2.80x10
-4.20x10
-5.60x10
10
10
f (Hz)
10
10
185
developed at the outer surface of the device because the free carriers are swept by the metal electrodes. Also the NC may be due to
the space charge located at the multiple insulatorsuperconductor
interfaces (grain boundaries) in the materials. Our frequency
dependent dielectric measurements are consistent with the previous measurements [17]. These ceramic materials with higher
dielectric constant are very useful in microelectronic devices as
capacitors and memory devices. Their use about the memory devices would help to sustain the remnant spins due to their higher
capacitance. The imaginary part of the dielectric constant (e00 ) represents absorption and attenuation of energy across the interfaces,
when the sample is exposed to the external electric eld. The interfaces include the grain boundaries, localized defects and localized
charge densities at the defects sites. The imaginary part of the
dielectric arises due to lag in polarization with the applied ac-eld
and is observed to decrease with the increase in frequency. The value of e00 at the low frequency of 10 KHz decreases from 5.4 107 to
2.7 107 with the increase of Mg doping in Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d superconductor at 79 K and its value is further
decreased from 2.4 107 to 1.1 107 with the increase of Mg
doping at room temperature (290 K), Fig. 5.
The dielectric loss factor (tan d) is the ratio of the energy dissipated per radian in the material to the energy stored at the peak
of the polarization and it determines the mechanism of the ac-conduction and dielectric relaxation. The value of tan d increases as the
frequency decreases and attains the maximum value at the low frequency of 10 KHz. At 10 KHz, the value of tan d decreases from
745 to 362 with the increase of Mg concentration at room temperature (290 K), which is further decreased from 222 to 71 closer to liquid nitrogen temperature (79 K), Fig. 6. A low frequency of
10 KHz, the value of tan d decreases with the increase of Mg doping,
both at 79 and 290 K.
The ac-conductivity (rac) of the Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d (y = 0, 0.5, 1.0, 1.5) at temperatures of 79 and 290 K is
shown in Fig. 7. The value of rac increases with the increase of
0 a
6x10
79K
5x10
4x10
-120
-160
2x10
-200
-240
2.5x10
tan
//
290K
2.0x10
-300
-450
-600
1.0x10
5.0x10
290K
-750
b
10
-150
1.5x10
0.0
y=0
y = 0.5
y = 1.0
y = 1.5
-80
3x10
1x10
79K
-40
y=0
y = 0.5
y = 1.0
y = 1.5
10
f (Hz)
10
10
10
10
f ( Hz )
10
10
75
60
30
ac(1/ cm)
79K
y=0
y = 0.5
y = 1.0
y = 1.5
45
15
0
50
40
30
290K
20
10
0
10
10
f (H z)
10
10
-4.9x10
79K
290K
-5.6x10
-4.2x10
-4.5x10
Fig. 7. Plot of ac-conductivity (rac) versus frequency of Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d (y = 0, 0.5, 1.0, 1.5) superconductors at temperatures (a) 79 K
and (b) 290 K.
-6.3x10
-4.8x10
-7.0x10
-5.1x10
-7.7x10
-5.4x10
7
2.4x10
5.4x10
2.1x10
//
4.5x10
//
1.8x10
7
3.6x10
1.5x10
7
2.7x10
tan
1.2x10
-80
-400
-120
-500
-600
-160
-700
-200
-800
ac
tan
90
80
45
75
40
70
35
65
60
ac
186
30
0.0
0.5
1.0
1.5
Mg content
Fig. 8. The summary of e0 , e00 , tan d, and rac measurements versus Mg content in
Cu0.5Tl0.5Ba2Ca2yMgyCu0.5Zn2.5O10d superconductors.
187
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