Spin-spin correlations and microscopic origin of net magnetization in the
spin-1 trimer chain compound CaNi3P4O14 have been investigated by powder
neutron diffraction. The present study reveals a 3D long-range magnetic
ordering below 16 K where the magnetic structure consists of ferromagnetic
trimers that are coupled ferromagnetically along the spin-chain. The moment
components along the a and c axes arrange antiferromagnetically. Our study
establishes that the uncompensated moment components along the b axis result in
a net magnetization per unit cell. The magnetic structure, determined in the
present study, is in agreement with the results of recent first principles
calculation; however, it is in contrast to a fascinating experimental
prediction of ferrimagnetic ordering based on the periodicity of the exchange
interactions in CaNi3P4O14. Our study also confirms the presence of broad
diffuse magnetic scattering, due to 1D short-range spin-spin correlations, over
a wide temperature range below ~50 K down to a temperature well below the Tc.
Total neutron scattering analysis by the RMC method reveals that the dominating
spin-spin correlation above Tc is ferromagnetic and along the b axis. The
nearest neighbour spin-spin correlations along the a and c axes are found to be
weakly antiferromagnetic. The nature of the trimer spin structure of the
short-range state is similar to that of the 3D long-range ordered state. The
present investigation of microscopic nature of the magnetic ground state also
explains the condition required for the 1/3 magnetization plateau to be
observed in the trimer spin-chains. In spite of the S=1 trimer chain system,
the present compound CaNi3P4O14 is found to be a good realization of 3D magnet
below the Tc=16 K with full ordered moment values of ~2 mu_B/Ni2+ (1.98 and
1.96 mu_B/Ni2+ for two Ni sites, respectively) at 1.5 K.Comment: 10 pages, 8 figure
