We perform angular non-critical phase-matching third-harmonic generation (T
HG) experiments in KTiOPO4 (KTP). From these experiments, we determine the
magnitude and sign of the two phase-matched nonlinear coefficients of KTiOP
O4 by a complete analysis of phase-matching properties of the cascaded quad
ratic and pure cubic processes. the resolution of the coupled propagation e
quations and by the calculation of the quadratic and cubic dielectric susce
ptibility tensor by an extended bond charge model; we find: chi(24)((3))(53
9 nm) = 14.6 x 10(-22) m(2) V-2 and chi(16)((3)) (491 nm) = 8.0 x 10(-22) m
(2) V-2. We also demonstrate that the two studied THG are mainly governed b
y the cubic interaction.