We report on the observation of multiple third-harmonic conical waves generated in an annular periodically poled nonlinear photonic crystal. We show that the conical beams are formed as a result of the cascading effect involving two parametric processes that satisfy either the transverse and/or longitudinal phase-patching conditions. This is the first experimental observation of third-harmonic generation based on nonlinear Raman-Nath diffraction. © 2011 Optical Society of America OCIS codes: 190.2620, 190.4410, 220.4000, 050.1940 Third-harmonic generation (THG, also called frequency tripling) is important in many applications as an effective way to achieve coherent light source at shorter wavelengths. To get efficient THG one often employs a two-step cascaded process that involves successive second-harmonic generation (SHG, ω þ ω ¼ 2ω) and sum-. In a nonlinear photonic crystal (NPC) [2][3][4], this process can be realized by using the quasi-phase-matching (QPM) technique [5][6][7][8] that involves a periodic variation to the sign of the second-order nonlinearity χ ð2Þ [9]. The resulting modulation enables one to phase-match the constituent processes via a set of reciprocal lattice vectors (RLV), i.e. k 2 − 2k 1 ¼ G 1 for SHG and k 3 − k 1 − k 2 ¼ G 2 for SFM, with k l ðl ¼ 1; 2; 3Þ being the wave vector of the interacting waves and G 1;2 being RLV [10][11][12]. While these two vectorial relations have been widely used in realization of efficient cascaded THG, it is interesting to see the emission of a third-harmonic (TH) via the socalled Čerenkov-type interaction [13]. The Čerenkov THG represents the type of noncollinear frequency tripling that satisfies only the longitudinal phase-matching conditions: k 2 cos θ 1 ¼ 2k 1 for SHG and k 3 cos θ 2 ¼ k 2 cos θ 1 þ k 1 for SFM, with θ 1;2 being the Čerenkov angles for the secondharmonic (SH) and TH waves, respectively.One question is raised whether it is possible to realize cascaded frequency tripling via transverse phasematching only. It was shown recently that the propagation of a light beam in periodic NPC leads to multiorder diffraction of the SH when the transverse phase-matching condition k 2 sin α ¼ mG (m is integer) is satisfied [14][15][16], in an analogy to linear Raman-Nath diffraction [17]. Thus, one may expect the nonlinear Raman-Nath diffraction of the TH wave via transverse phase-matched SHG and SFM. However, up until now, only the purely longitudinal (Čerenkov) phase-matched THG was observed [13]. In this Letter we report for the first time on experimental observation of THG which relies on cascaded transverse (Raman-Nath) phase-matching. Moreover, we observe for the first time the THG nonlinear diffraction based on cascading of transverse and longitudinal phase-matched processes. The different phase-matching possibilities provide a set of TH rings at different angles.The annular NPC was fabricated using electric poling of a Z-cut MgO:doped stoichiometric lithium tantalate (SLT) crystal (thickness 490 μm). The period is 7:5 μm and the duty factor var...