Excitation spectrum of a model antiferromagnetic spin-trimer

Abstract

We present an inelastic neutron scattering (INS) study of the excitation spectrum of a model S = 1/2 equilateral Heisenberg trimer, Cu_3(O_2C_16H_23)_6.1.2C_6H_12. Earlier measurements were interpreted on the basis of a spin ground state consisting of a pair of degenerate S = 1/2 doublets, with an S = 3/2 quartet excited state. Given that the simplest model of magnetism for this compound includes a degenerate ground state, using thermodynamic probes to determine the excitation energy between the ground and excited states is challenging. An estimate of the excitation energy between the ground and excited states based on magnetic susceptibility measurements is roughly ~28 meV. INS measurements of this compound are likewise challenging since inter- and intramolecular vibrational modes associated with the organic ligands are at frequencies similar to the magnetic excitations. However, by measuring a non-magnetic analog, i.e. ligands only, as well as the temperature dependence of the excitations in the magnetic system, we are able to determine the excitation energy as being approximately 36.5 meV at T = 10 K, with a gradual softening to 32 meV with increasing temperature. We emphasize the consideration of ligand/lattice based excitations while interpreting magnetic excitations of such nanomagnetic systems containing organic molecules while underscoring the importance of INS in determining the magnetic excitation spectrum in systems with degenerate ground states.