Solid State Ionics 34 (1989) 93-95
North-Holland, Amsterdam
SPECIFIC HEAT OF KDP NEAR THE TETRAGONAL-MONOCLINIC PHASE TRANSITION
R.A. VARGAS, M. CHACON and J.C. TROCHEZ
Departamento de Fisica, Universidad del Valle, Apartado Abreo 25360, Cali, Colombia
Received 14 October 1988: accepted for publication 2 January 1989
Specific heat measurements of KH2PO4 (KDP) have been performed from 340 to 490 K using ac calorimetric methods. A
steplike anomaly in the specific heat is observed with transition temperature 453 K on heating runs of single crystal samples,
which shows the tetragonal~monoclinic phase transition of KDP. The results also show that the high-temperature monoctinic
phase is metastable below 453 K.
1. Introduction 2. Experimental
The phase behavior of potasium dihydrogen phos-
phate (KDP) has been widely reported [ 1-4 ]. Be-
low its ferro-paraelectric phase transition at 122 K
(under normal pressure) is orthorhombic, while a
tetragonal structure is stable at room temperature. A
third crystalline modification - monoclinic - has
been inferred from high-temperature X-ray studies
[1], although some further refinements seem nec-
essary, mainly concerning the atomic distribution
within the unit cell. Other DTA, TGA 2, proton con-
ductivity, dielectric constant [5] and Raman scat-
tering results [4] are in favor of the existence of two
high-temperature phases with different long-range
crystalline order. Nevertheless, it has become ap-
parent that the discrepancies in the previously re-
ported results concerning the tetragonal-monoclinic
phase boundary are due to inherent problems of
sample preparation or its thermal history.
In the present work a new attempt was made to
look carefully at the thermal response of single-crys-
tal and powder samples of KDP in the high-temper-
ature region, seeking new information concerning the
tetragonal-monoclinic phase boundary. The thermal
analysis of the samples was made using the ac ca-
lorimetry technique.
Small single crystals of KDP were grown by the
solution evaporation technique at a controlled tem-
perature near 27°C and in a dry atmosphere. Merck
reagent-grade KH2PO4 powder was used as starting
material. Polycrystalline samples in the form of pel-
lets compacted from a powder or single crystals were
also used.
An ac calorimeter apparatus for high temperature
thermal analysis of solid samples in an inert atmo-
sphere, which has been described elsewhere [ 6 ], was
used to determine the temperature-dependent spe-
cific heat of KDP. The samples were typically of sev-
eral square millimeters in area and about 0.15 mm
thickness. The temperature oscillations were in-
duced in the sample by a square power input of fre-
quency COo=2 Hz, produced by a beam of light
chopped at this frequency. Our measured signal-to-
noise ratio was best at this frequency within the cor-
responding operating range which is determined by
the condition that the amplitude of the temperature
oscillations of the sample, I Tac I, at a fixed ambient
furnace temperature, are inversely proportional to
the frequency of the chopped heat pulse. The cali-
bration constant of the apparatus, K, according to
the basic equation of the ac calorimetry method,
Cp= K/LTa,. I, was not obtained, so the reported data
correspond to 1/ I ~+ I.
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