ISSN 1063-7834, Physics of the Solid State, 2011, Vol. 53, No. 3, pp. 510–517. © Pleiades Publishing, Ltd., 2011.
Original Russian Text © E.A. Mikhaleva, I.N. Flerov, V.S. Bondarev, M.V. Gorev, A.D. Vasiliev, T.N. Davydova, 2011, published in Fizika Tverdogo Tela, 2011, Vol. 53, No. 3,
pp. 478–484.
510
1. INTRODUCTION
In recent years, the electrocaloric, magnetocaloric,
and barocaloric effects have attracted increased atten-
tion of researchers due to the fundamental and applied
aspects of these phenomena. As regards the applied
aspects, the case in point is the possibility of using
materials having caloric effects in solid-state cooling
devices [1, 2]. The cooling technique based on any
caloric effect lies in a reversible change in the temper-
ature or entropy of a thermodynamic system (ferro-
electric, ferromagnetic, and ferroelastic) in response
to external fields (electric, magnetic, and mechanical
stresses) under adiabatic or isothermal conditions,
respectively, which makes it possible to organize a
classical inverse Carnot cycle. For a long time, the
magnetocaloric and electrocaloric effects have not
attracted special attention, because their magnitudes
in materials known by that time were too small in
order to provide a high efficiency of refrigeration
cycles. However, gradual progress in theoretical and
experimental methods of investigation of magneto-
thermal and electrothermal properties of materials
and discovery of new compounds (ferroics), which
undergo phase transitions accompanied by significant
changes in the entropy, favored the renewal of scien-
tific and practical interest in the study of the magneto-
caloric and electrocaloric effects. At present, there
exist a wide range of magnets and a rather limited
number of ferroelectrics that can be recommended for
the use as solid refrigerants [1–3]. Among magnetic
materials, large magnitudes of the intensive (ΔT
ad
) and
extensive (ΔS
ce
) effects are characteristic of perovs-
kite-like manganites, alloys, intermetallic com-
pounds, etc. In the family of ferroelectrics, order–dis-
order phase transitions, i.e., transitions associated
with the large change in the entropy ΔS/R > ln2, occur
more rarely. The largest electrocaloric effect was
observed in lead zirconate titanate thin films, and,
only in this form, the material appeared to be compet-
itive in the caloric efficiency with the most promising
magnetic solid-state refrigerants [1, 4].
Experimental investigations of the barocaloric
effect (BCE), which has long been used in vapor–gas
refrigeration cycles, have been started rather recently,
and, correspondingly, this effect has been studied to a
considerably lesser extent as compared to the magne-
tocaloric and electrocaloric effects. The technique of
adiabatic cooling in the vicinity of the structural phase
transition induced by the external pressure in com-
pounds containing rare-earth ions was proposed in
1998 [5]. More recently, investigations of the baroca-
loric effect in ferroelastics revealed that, at relatively
low hydrostatic pressures, fluoroxygen compounds
that undergo phase transitions associated with the
ordering of cations and anions can be characterized by
values of ΔS
ce
and ΔT
ad
comparable to the best param-
eters of the magnetocaloric effect in magnets [6, 7]. It
was demonstrated that one of the factors responsible
FERROELECTRICITY
Phase Transitions and Caloric Effects in Ferroelectric Solid
Solutions of Ammonium and Rubidium Hydrosulfates
E. A. Mikhaleva
a, b,
*, I. N. Flerov
a, b,
**, V. S. Bondarev
a, b
, M. V. Gorev
a, b
,
A. D. Vasiliev
a, b
, and T. N. Davydova
b
a
Institute of Engineering Physics and Radioelectronics, Siberian Federal University,
pr. Svobodny 79, Krasnoyarsk, 660041 Russia
* e-mail: katerina@iph.krasn.ru
** e-mail: flerov@iph.krasn.ru
b
Kirensky Institute of Physics, Siberian Branch, Russian Academy of Sciences,
Akademgorodok 50, Krasnoyarsk, 660036 Russia
Received June 24, 2010
Abstract—Structural, calorimetric, dielectric, and electrocaloric investigations of Rb
x
(NH
4
)
1– x
HSO
4
ferro-
electric solid solutions have been performed. It has been found that rubidium atoms inhomogeneously
occupy nonequivalent crystallographic positions in the structure P2
1
/c. The influence of the rubidium con-
centration on the sequence of phase transitions in the NH
4
HSO
4
compound has been established. It has been
revealed that the consequences of the Landau theory can be applied to the description of the temperature
dependences of the anomalous heat capacity and the electrocaloric effect over a wide range of temperatures.
Comparative evaluations of the electrocaloric and barocaloric effects in hydrosulfate and triglycine sulfate
crystals have been carried out.
DOI: 10.1134/S1063783411030188