We report nuclear magnetic resonance (NMR) studies in the antiferromagnetic state of the quasi-two-dimensional (CuBr)LaNb2O7. The NMR spectra at zero magnetic field and 4.2 K indicate a unique Cu and Br sites with an internal field of 5.7 T (at Cu) and 16.4 T (at Br), confirming a magnetic order. For the large internal field at the Br sites to be compatible with the collinear antiferromagnetic order observed by neutron diffraction experiments (N. Oba et al., J. Phys. Soc. Jpn. 75, (2006) 113601), the Br atoms must move significantly off the center of the square of the Cu sublattice so that the Br nuclei couple predominantly to two parallel Cu moments. While invalidating the frustrated J1-J2 model defined on a C4-symmetric square lattice, our results are compatible with the structural model proposed for (CuCl)LaNb2O7 by Yoshida et al. (J. Phys. Soc. Jpn. 76 (2007) 104703).
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