Recently, 17 O NMR has been performed for the first time on AmO 2 . We have observed a drastic broadening of the NMR spectrum, along with a sudden drop of NMR signal intensity, below T 0 = 8.5 K. These data provide the first microscopic evidence for a phase transition at this temperature as a bulk property of this system. In this paper, we compare NMR results for AmO 2 with those from UO 2 and NpO 2 . In the ordered state we have recorded an 17 O NMR spectrum with a triangular line shape, which resembles neither that of UO 2 nor NpO 2 . This spectrum indicates that the internal local field H int is distributed very nearly randomly from zero to a maximum value, that is, H max int ∼ 7kOe. The temperature dependences of the Knight shift and the nuclear relaxation rate are also compared.KEYWORDS: actinide dioxide, NMR, phase transition, self-radiation effect Actinide dioxides (AnO 2 : An = U, Np, Pu and Am, etc.) are all cubic insulators with rather well-localized 5 f electrons. The actinide ions have the same tetravalent state, so that the number of 5 f electrons per actinide ion varies systematically, with two for U 4+ , three for Np 4+ , four for Pu 4+ and five for Am 4+ in the same cubic fluorite structure. In f -electron systems, the f -electron state is represented in terms of multipole degrees of freedom. Available multipoles on each material are dependent on the character of the crystalline electric field (CEF) ground state determined by the number of f -electrons as well as the symmetry of the crystal. In the cubic symmetry of AnO 2 , even the higher order multipoles are not quenched, and are found to affect the physical properties at low temperatures.UO 2 exhibits an antiferromagnetic (AFM) phase transition at T N = 30.8 K. The magnetic order has the transverse triple-q structure with an ordered moment of 1.74µ B /U atom.1-5) Recently, resonant X-ray scattering measurements have revealed the occurrence of long-range antiferroquadrupolar (AFQ) ordering as a secondary order parameter below T N . 6) NpO 2 is known to exhibit a rather mysterious phase transition at T 0 = 26 K. The compound was thought for many years to be an antiferromagnet; 7-10) however, neither Mössbauer spectroscopy 11,12) nor neutron diffraction [13][14][15] detected any ordered moment below T 0 . It is now recognized that the phase transition originates from an octupole moment of Γ 5 symmetry (or other high-order multipoles with the same symmetry) allowed by the Γ 8 quartet CEF ground state of the Np 5f electrons. [16][17][18][19][20][21][22][23][24][25] The longitudinal triple-q Γ 5 antiferrooctupolar (AFO) order scenario was suggested initially by resonant X-ray scattering 17) and then strongly supported from a microscopic viewpoint by 17 O NMR studies. 20,21,[26][27][28] AmO 2 also exhibits a phase transition at T 0 =8.5 K. However, owing to the limited number of experimental data, the mechanism of this phase transition has remained a mystery for more than 30 years. The phase transition was first reported from magnetic susceptibility ...