Magnetic neutron spectroscopy of a spin-transitionMn3+molecular complex

Abstract

We have investigated by inelastic neutron scattering (INS), neutron diffraction, andmagnetometry the magnetic properties of the mononuclear complex [Mn3+(pyrol)3(tren)] in both high-spin (5E, HS, S = 2) and low-spin (3T1, LS, S = 1) states. The system presents a spin transition (ST) around 47 K with a small hysteresis width (TST,↑ = 47.5 K and TST,↓ = 46 K) characteristic of an efficient collective transition process. In the HS state, the INS spectrum at 56 K and zero magnetic field is accounted for by a zero-field splitting with D = −5.73(3) cm−1 and |E| = +0.47(2) cm−1 which may be the result of a dynamic Jahn-Teller effect reported in the literature.In the LS state, a single magnetic peak at 4.87 meV is observed, still at zero field. Despite the existence of an unquenched orbital moment (L = 1) in the ground 3T1 state, we argue that it may be described by a genuine S = 1 spin Hamiltonian owing to the existence of a strong trigonal distortion of the Mn3+ coordination octahedron. The observed peak corresponds to a transition M = +1 within the S = 1 ground state split by a large single-ion anisotropy term D = +39.3 cm−1. A full spin-Hamiltonian model is proposed based on these first INS results obtained in a thermal ST molecular magnetic system.