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We report Cu-NMR/NQR and F-NMR studies on the multilayered high-T_c copperoxides Ba_2Ca_{n-1}Cu_nO_{2n}F_2 with n=2,3,4, where n is the number of CuO_2planes. It is revealed that bi-layered Ba_2CaCu_2O_4F_2 is an underdopedsuperconductor with hole carriers, which are introduced into CuO_2 planes by anunexpected deviation from the nominal content of apical fluorines. In aprevious paper, we proposed a self-doping mechanism as the origin of carrierdoping in n=3 and n=4; in the mechanism, electrons are transferred from theinner CuO_2 plane (IP) to the outer one (OP). However, since it has been foundthat the bi-layered compound is hole doped, we have reexamined thesuperconducting and magnetic properties in n=3 and n=4 by Cu-NMR/NQR and F-NMR.The extensive NMR studies have confirmed that the apical-fluorine compounds arenot self-doped but hole-doped, and that antiferromagnetism (AFM) andsuperconductivity (SC) coexist in a single CuO_2 plane. In n=4, the AFMordering occurs at T_N = 80 K, well above T_c=55 K, where the respective AFMmoments are M_AFM=0.11 mu_B and 0.18 mu_B at the OP and the IP. In n=3, on theother hand, the underdoped single IP exhibits a spontaneous moment M_AFM=0.12mu_B at low temperatures and a peak in the nuclear-spin-lattice relaxation rate1/T_1 of F at T_N=23 K, much lower than T_c = 76 K. We note that the increasein the number of IPs from one to two leads to an increase in T_N due tostrengthening the interlayer coupling, although the doping levels for bothcompounds are almost comparable. The present results strongly suggest that theuniform mixing of AFM and SC is a general property inherent to a single CuO_2plane in the underdoped regime for hole-doping.

physical review. b, condensed matter and materials physics

Uniform mixing of antiferromagnetism and high-T_c superconductivity in  multilayered copper oxides Ba_2Ca_{n-1}Cu_nO_{2n}F_2 with apical fluorines  (n=2,3,4): Cu-NMR/NQR and F-NMR