J. Appl. Cryst. (2015). 48, doi:10.1107/S1600576715002113
Supporting information
Volume 48 (2015)
Supporting information for article:
Antisite defects elimination through Mg-doping in SLT powder
synthesized via a wet-chemical spray-drying method
Dehui Sun, Xueliang Kang, Qian Yu, Kun Cui, Xiaoyong Qin, Xuxia Shi,
Huaqiang Cai, Tadashi Ohachi, Yuanhua Sang and Hong Liu
Supplementary Information
Antisite defect elimination through Mg-doping in SLT powder
synthesized via a wet-chemical spray-drying method
Dehui Sun,a,e Xueliang Kang,a† Qian Yu,b Kun Cui,c Xiaoyong Qin,c Xuxia Shi,c Huaqiang
Cai,b Tadashi Ohachi,d Yuanhua Sanga,e* and Hong Liua,e*
a
State key Laboratory of Crystal Materials, Shandong University, Jinan 250100, P. R. China, b Institute of
Chemical Materials, China Academy of Engineering Physics, Mianyang 621900, P. R. China, c CETC Deqing
Huaying Electronics Co., Ltd., Deqing 313200, P.R. China, d IRE Laboratory, D-egg, Doshisha University, Kyoto
610-0332 Japan, e Innowit Co., Ltd., Jinan 250101,P.R. China.
Correspondence emails: [email protected], [email protected] ; † Co-first authors
Supplement 1 thermal property of the MgO:SLT precursor
Figure S1 TG and DSC curves of the MgO:SLT precursor obtained from a
wet-chemical–spray drying method at heating process.
Fig. S1 shows the thermal analysis of the MgO:SLT precursor obtained from a
wet-chemical–spray drying method. The TG curve in Fig. S1 indicates two distinct
weight loss steps around 490 K and 790 K, respectively. The DSC curve shows two
endothermic peaks at 464 K and 524 K, corresponding to the first significant weight
loss. The endothermic peak at 464 K corresponds to the separation of crystal water
from citric acid, while the one at 524 K is related to the decomposition of NH4Cl and
CA1. A large exothermic peak at 759 K lies in the temperature range of that the
second sharp weight loss, which can be attributed to the ignition of CA2. The small
one at 879 K in the DSC curve is attributed to the formation of a LT phase.
Supplement 2 Lattice constants of MgO:LT crystal powder prepared
by different method
XRD patterns of S-Mg:CLT1200 powder (a), S-Mg:SLT1200 (b) and
W-Mg:SLT720 (c) are shown in Fig. S2. The crystal lattice constants are calculated as
a=b=0.51600 nm, c=1.38083 nm, a=b=0.51597 nm, c=1.37935 nm and a=b=0.51586
nm, c=1.37803 nm for samples S-Mg:CLT1200, S-Mg:SLT1200 and W-Mg:SLT720,
respectively3. Based on that Mg2+ occupies the position of Ta-Li anti-site in the
LiTaO3 lattice, as well as the larger size of Mg2+ than that of Ta4+, the larger lattice
constants of these MgO:LT samples compared with that of the pure LT implies that
Mg2+ entering into lattices, too. It is consistent with the result of the study by T.
Katsumata et al4.
Fig. S2 XRD patterns of S-Mg:CLT1200 (a), S-Mg:SLT1200 (b) and W-Mg:SLT1200
(c).
Supplement 3 the quantity of Mg element doped in the LT lattice
Table S1 The proportion of free Mg2+ in a HCl solution to the total MgO.
Sample
Mg2+/MgO（mol%）
W-Mg:SLT720
0.81
S-Mg:SLT720
40.2
S-Mg:CLT720
39.3
S-Mg:SLT1200
5.12
S-Mg:CLT1200
4.17
When the certain amount of samples were immersed in a HCl solution (5 ml, 6
mol/L), the MgO particles and Mg-rich areas were dissolved quickly. The
concentration of free Mg2+ in the upper solutions was measured by ICP-AES. The
quantity of Mg ions which did not enter into LiTaO3 lattices is calculated on the basis
of the Mg2+ concentration in the solution. The proportions of free Mg2+ in a HCl
solution to the total Mg element which was contained in the sample immersed in the
HCl solution were displayed in Table S1. Around 40 % Mg ions did not enter into the
LT lattice of the S-Mg:SLT720 powder. And around 5% Mg ions still exist out of LT
lattice when the calcination temperature rose to 1473 K. No more than 1% of the Mg
ions can be dissolved for W-Mg:SLT720, which should be from the doped ions on the
surface of the particles instead of the MgO aggregations in the solid reaction method.
Therefore, it is concluded that all Mg2+ has entered into the LiTaO3 lattice for the wet
chemical-spraying synthesis approach.
Supplement 4 the TEM-EDS spectrum
Figure S3 TEM-EDS spectrum of S-Mg:SLT1200 sample
Supplement 5 the optical homogeneity of MgO:SLT crystal
Fig. S4 Optical homogeneity of MgO:SLT crystal measured by ZYGO laser
interferometer.
1
2
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M.N. Liu, D.F. Xue, Solid State Ionics 2006, 177, 275-280.
R. L. Barns and J. R. Carruthers, J. Appl. Cryst. 1970, 3, 395-399.
T. Katsumata, K. Shibata, Mater. Res. Bull. 1994, 29, 559-566.