Eur. Phys. J. Appl. Phys. 92, 20401 (2020) DOI: 10.

1051/epjap/2020200075

Comparison of random field strengths in (1-x)SrTiO3-xBiFeO3

and (1-x)SrTiO3-xBaTiO3 relaxor ferroelectrics by means
of acoustic emission
Evgeniy Dul’kin, and Michael Roth

sciences
Eur. Phys. J. Appl. Phys. 92, 20401 (2020)
© EDP Sciences, 2020
THE EUROPEAN
https://doi.org/10.1051/epjap/2020200075 PHYSICAL JOURNAL
APPLIED PHYSICS
Regular Article

Comparison of random field strengths in (1-x)SrTiO3-xBiFeO3

and (1-x)SrTiO3-xBaTiO3 relaxor ferroelectrics by means
of acoustic emission
Evgeniy Dul’kin*, and Michael Roth
Department of Applied Physics, The Hebrew University of Jerusalem, Jerusalem 91904, Israel

Received: 21 March 2020 / Received in final form: 2 September 2020 / Accepted: 2 October 2020

Abstract. In relaxor (1-x)SrTiO3-xBiFeO3 ferroelectrics ceramics (x = 0.2, 0.3 and 0.4) both intermediate
temperatures and Burns temperatures were successfully detected and their behavior were investigated in
dependence on an external bias field using an acoustic emission. All these temperatures exhibit a non-trivial
behavior, i.e. attain the minima at some threshold fields as a bias field enhances. It is established that
the threshold fields decrease as x increases in (1-x)SrTiO3-xBiFeO3, as it previously observed in
(1-x)SrTiO3-xBaTiO3 (E. Dul’kin, J. Zhai, M. Roth, Phys. Status Solidi B 252, 2079 (2015)). Based on the
data of the threshold fields the mechanisms of arising of random electric fields are discussed and their strengths
are compared in both these relaxor ferroelectrics.

1 Introduction During a last time the (1-x)SrTiO3-xBiFeO3 compound

After being discovered in 1954 by Smolenskii with
co-workers the relaxor ferroelectrics (RFEs) are the objects
of scrupulous study due to their fundamental intrinsic
chemical disorder on both their A- and B-sites in contrast
to ordered ferroelectrics (FEs) [1]. Such a chemical disorder
is known to be a reason to arise the quenched random
electric fields (RFs) [2], which in turn is known to be a
reason to nuclei the polar nanoregions (PNRs) [3]. It is well
documented that the PNRs nucleate below high-lying
Burns temperature, TB [4], start to grow below intermedi-
ate temperature, T* [4–6], provide a huge, smeared and
frequency dependent maximum of permittivity, e, at
temperature Tm [7], and freeze below freezing temperature,
Tf [8], as the temperature decreases.
When applying a weak electric bias field, E, a non-
trivial behavior of Tm is well proven to appear in
dependence on E, which is called the V-shape effect,
manifesting in initial decrease of Tm and its subsequent
increase after attaining a minimum at some threshold field,
Eth, as E enhances. The V-shape effect is observed in some
well-known RFEs [9–18], and is concluded to be a
competition between both the RFs and E when affecting
the PNRs [10–13]. Moreover, along with Tm both T* and
TB also exhibit the V-shape at the same Eth [4,14], because
they are a consequence of PNRs, too, and, so, are
characteristic for RFEs. And, so, the V-shape is the same
intrinsic feature of relaxor state as well as the frequency
dispersion of e.
* e-mail: evgeniy.dulkin@mail.huji.ac.il
attract an attention as being a complicated one with
contradictory properties. SrTiO3 (STO) refers to the
incipient ferroelectrics, in which the ferroelectric phase is
suppressed by quantum fluctuations (zero-point motions)
down to the lowest temperatures [19–22], and possesses a
nonpolar antiferrodistorsive tetragonal phase below
168 °C, which is assumed to suppress the ferroelectric
transition in addition to the quantum fluctuations [23],
whereas the BiFeO3 (BFO) is a rhombohedral ferroelectric
marked by high Curie temperature, Tc ≈ 820–840 °C
[24,25]. (1-x)STO-xBFO compounds with 0.05 < x < 0.2
exhibit a visible frequency dispersion up to room
temperature [26–28], and the TB is estimated by a
deviation of the 1/e dependence from a straight line [26].
Meanwhile an estimation of TB by dielectric data is
known to be non-correct [1], in comparison with acoustic
emission (AE) data [29]. Indeed, neither the T* nor the TB
is detected in 0.9STO-0.1BFO, but successfully detected in
both 0.8STO-0.2BFO and 0.7STO-0.3BFO ones using the
ultrasound technique, and based on these data it is
concluded that the relaxor state occurs in (1-x)STO-xBFO
compound when x > 0.1 [30].
Because the V-shape is recognized to be an intrinsic
feature of RFEs, a goal of the present work is to detect both
T* and TB as well as to study their behavior in dependence
on bias electric field in (1-x)STO-xBFO compound with
x = 0.2, 0.3 and 0.4 by means of AE.
2 Samples and experimental
The solid solution samples (1-x)STO-xBFO (x = 0.2, 0.3
and 0.4) were prepared using the conventional ceramic
technique. The oxides TiO2, Fe2O3, Bi2O3, and a strontium

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Fig. 1. The acoustic emission, AE, count rate of all 0.8STO-

0.2BFO, 0.7STO-0.3BFO and 0.6STO-0.4BFO in dependence on
temperature in absence of bias field, E. Fig. 2. The intermediate, T*, and Burns, TB, temperatures of all
0.8STO-0.2BFO, 0.7STO-0.3BFO and 0.6STO-0.4BFO com-
pounds in dependence on bias field, E.
carbonate SrCO3 were used as initial reagents. The
synthesis and sintering of ceramics were carried out in
platinum crucibles at a temperature of 1100 °C for 24 h and
temperatures of 1320–1300 °C for 1 hour, respectively.
Then the samples were polished and silver contacts were
fired at 650 °C for 30 min.
The AE technique is described in great detail elsewhere
[14]. A sample is pasted with a silver epoxy to the polished
side of a fused silica acoustic rod waveguide. A PZT-19 disk
piezoelectric sensor is attached to the rear end of the
waveguide. The sensor is electrically coupled to a 500 kHz
bandpass low noise variable (up to 40 dB) preamplifier
connected to a detector-amplifier (40 dB). A Cr-Al
thermocouple junction is glued to the waveguide near a
sample. A higher part of the acoustic waveguide with the
sample pasted is vertically mounted from below into the
resistance furnace. Both the thermocouple and amplifier
outputs are interfaced with a PC for a coupled readout. The
silver contacts of a sample are connected to a high voltage
power supply. Temperature dependences of the AE count
rate N_ (s 1) are measured at several fixed values of bias
voltage upon heating from 100 to 400 °C with rate of about Fig. 3. The threshold fields, Eths, in dependence on amount of
1–3 °C/min. both BFO and BTO, x.

TB were detected in 0.6STO-0.4BFO previously using the

3 Results and discussion
Figure 1 presents the AE count rate N_ of all 0.8STO-
0.2BFO, 0.7STO-0.3BFO and 0.6STO-0.4BFO com-
pounds in dependence on temperature in absence of bias
field E. AE exhibits three groups of signals in low-
temperature region and three groups in high-temperature
one. The sharp bursts of N_ point out both T* (177.1 and
153 °C) and TB (260.5 and 310 °C), which are found to be in
excellent agreement with those recently detected in
0.8STO-0.2BFO and 0.7STO-0.3BFO compounds using
ultrasound technique [30]. In 0.6STO-0.4BFO, the sharp
bursts of N_ are found to be 163 and 300°C, corresponding to
T* and TB, respectively. Note, that neither the T*, nor the
ultrasound technique [27].
Figure 2 presents both T* and TB, detected by AE, of
all 0.8STO-0.2BFO, 0.7STO-0.3BFO and 0.6STO-0.4BFO
compounds in dependence on bias field E. All the T*(E)
and TB(E) dependences clearly exhibit the V-shape effect
with Eth ≈ 0.8, 0.6 and 0.4 kV/cm for all the 0.8STO-
0.2BFO, 0.7STO-0.3BFO and 0.6STO-0.4BFO, respec-
tively, characteristic for RFEs [9–18]. Unfortunately, N _
of all the compounds exhibits a too large scattering to be
plotted reliably in dependence on E.
Figure 3 presents all the Eths of (1-x)STO-xBFO
compounds in dependence on x. Also Figure 3 presents
all the Eths of (1-x)SrTiO3-xBaTiO3 ((1-x)STO-xBTO))
compounds in dependence on x, previously detected by

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 E. Dul’kin and M. Roth: Eur. Phys. J. Appl. Phys. 92, 20401 (2020)
Table 1. Data of threshold fields of (1-x)STO-xBTO and
(1-x)STO-xBFO relaxors ferroelectrics.
Compound Eth (kV/cm) Source
0.4STO-0.6BTO 0.75 Reference [31]
0.3STO-0.7BTO 0.6 Reference [31]
0.2STO-0.8BTO 0.4 Reference [31]
0.8STO-0.2BFO 0.8 Present
0.7STO-0.3BFO 0.6 Present
0.6STO-0.4BFO 0.4 Present
means of AE, too [31] (Tab. 1). One can clearly see that
both the Eth(x) dependences are linear and practically
parallel with the slopes of about 2 and 1.75 kV/cmx for
(1-x)STO-xBFO and (1-x)STO-xBTO, respectively. A
reason of such the decrease of Eth is clear: the larger a
content of FEs, the weaker the RFs, and so, the weaker bias
field E is needed to affect the PNRs.
As it shortly mentioned in Introduction, being initially
pinned by RFs, the PNRs start switching to E, as E
enhances, the Tm decreases until E becomes equal to RFs at
Eth, where the Tm attains minimum, causing the V-shape
effect, and then starts to increase in manner of FEs with
second-order phase transition [10]. So, a measurement of
Eth gives us an occasion to determine a strength of the RFs,
Eth = RFs, in fact.
Let us now consider the mechanisms of creation the RFs
in both (1-x)STO-xBFO and (1-x)STO-xBTO. In (1-x)
STO-xBFO the RFs are created when substituting of Sr2+
(rSr = 1.44Å (C.N. XII)) for Bi3+ (rBi = 1.30Å (C.N. VIII))
on A-site and Ti4+ (rTi = 0.6Å (C.N. VI)) for Fe3+
(rFe = 0.55Å (C.N. VI)) on B-site, due to difference of
their charges, heterovalent substitution [1]. Otherwise, in
(1-x)STO-xBTO the RFs are created when substituting of
Sr2+ for Ba2+ on A-site due to difference in their ion radii
(rBa = 1.61Å (C.N. XII) vs. rSr = 1.44Å (C.N. XII)),
isovalent substitution [1], leading to arising the corre-
sponding electrostrictive strains [32]. It is clear that the
RFs, caused by the former mechanism, is stronger than the
RFs, caused by the latter one, and, so, more than twice
amount of BTO in (1-x)STO-xBTO compound in compar-
ison with amount of BFO in (1-x)STO-xBFO compound is
required to create the same RFs.
4 Conclusion
In summary, we have investigated the (1-x)SrTiO3-xBiFeO3
(x = 0.2, 0.3 and 0.4) relaxor ferroelectrics by means of
acoustic emission and detected both intermediate and Burns
temperatures. We have detected the V-shape effect of these
temperatures in dependence on bias electric field and
established that the threshold fields linear decrease as x
increases. We have compared these threshold fields with
those previously detected in (1-x)SrTiO3-xBaTiO3 com-
pound by means of acoustic emission, too. We have discussed
the mechanisms of creating the random electric fields in
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3
both (1-x)SrTiO3-xBiFeO3 and (1-x)SrTiO3-xBaTiO3
compounds and compared them and concluded the random
fields in the former compound is stronger than in the latter
compound.
Author contribution statement
E. Dul’kin: measuring the crystals using an acoustic
emission method. M. Roth: treatment the data and plot the
Figures. E. Dul’kin and M. Roth: analysis the Figures and
conclusions.
Authors kindly thank to Elena Smirnova for providing
the (1-x)SrTiO3-xBiFeO3 ceramic samples.
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Cite this article as: Evgeniy Dul’kin, Michael Roth, Comparison of random field strengths in (1-x)SrTiO3-xBiFeO3 and (1-x)
SrTiO3-xBaTiO3 relaxor ferroelectrics by means of acoustic emission, Eur. Phys. J. Appl. Phys. 92, 20401 (2020)

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