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Spin-spin correlations and microscopic origin of net magnetization in thespin-1 trimer chain compound CaNi3P4O14 have been investigated by powderneutron diffraction. The present study reveals a 3D long-range magneticordering below 16 K where the magnetic structure consists of ferromagnetictrimers that are coupled ferromagnetically along the spin-chain. The momentcomponents along the a and c axes arrange antiferromagnetically. Our studyestablishes that the uncompensated moment components along the b axis result ina net magnetization per unit cell. The magnetic structure, determined in thepresent study, is in agreement with the results of recent first principlescalculation; however, it is in contrast to a fascinating experimentalprediction of ferrimagnetic ordering based on the periodicity of the exchangeinteractions in CaNi3P4O14. Our study also confirms the presence of broaddiffuse magnetic scattering, due to 1D short-range spin-spin correlations, overa 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 dominatingspin-spin correlation above Tc is ferromagnetic and along the b axis. Thenearest neighbour spin-spin correlations along the a and c axes are found to beweakly antiferromagnetic. The nature of the trimer spin structure of theshort-range state is similar to that of the 3D long-range ordered state. Thepresent investigation of microscopic nature of the magnetic ground state alsoexplains the condition required for the 1/3 magnetization plateau to beobserved 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 magnetbelow the Tc=16 K with full ordered moment values of ~2 mu_B/Ni2+ (1.98 and1.96 mu_B/Ni2+ for two Ni sites, respectively) at 1.5 K.

Long-range and short-range magnetic correlations, and microscopic origin of net magnetization in the spin-1 trimer chain compound CaNi3P4O14