The photoelasticity of the
C
a
3
T
a
G
a
3
S
i
2
O
14
(CTGS) crystal was studied by an interferometric method based on a single-pass Mach-Zehnder interferometer. The maximum number of sample orientations for the piezo-optic experiments was applied to prove accuracy in the determination of the piezo-optic coefficients. Based on the matrices of the piezo-optic coefficients and the elastic stiffness coefficients, all the coefficients
p
ik
of the elastic-optic matrix are calculated. For the highest
p
ik
coefficient, the acousto-optic efficiency is evaluated. The results obtained for CTGS are compared with the corresponding results for
L
a
3
G
a
5
S
i
O
14
(langasite) crystals. The highest acousto-optic figure of merit of CTGS
M
2
=
1.66
⋅
10
−
15
s
3
/
k
g
is two and three times higher, compared with langasite and strontium borate, respectively, which are often used for acousto-optic modulation of light in the ultraviolet spectral range.
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