Spin gap in a quasi-one-dimensional S=12 antiferromagnet: Cu2(1,4diazacycloheptane)2Cl4

Abstract
Cu2(1,4-diazacycloheptane)2Cl4 contains double chains of spin-12 Cu2+ ions. We report ac susceptibility, specific heat, and inelastic neutron-scattering measurements on this material. The magnetic susceptibility χ(T) shows a rounded maximum at T=8 K indicative of a low-dimensional antiferromagnet with no zero-field magnetic phase transition. We compare the χ(T) data with exact diagonalization results for various one-dimensional spin Hamiltonians and find excellent agreement for a spin ladder with intrarung coupling J1=1.143(3) meV and two mutually frustrating interrung interactions J2=0.21(3) meV and J3=0.09(5) meV. The specific heat in zero field is exponentially activated with an activation energy Δ=0.87(1) meV. A spin gap is also found through inelastic neutron scattering on powder samples that identify a band of magnetic excitations for 0.8<ħω<1.5 meV. Using sum rules we derive an expression for the dynamic spin-correlation function associated with noninteracting propagating triplets in a spin ladder. The Van Hove singularities of such a model are not observed in our scattering data, indicating that magnetic excitations in Cu2(1,4-diazacycloheptane)2Cl4 are more complicated. For magnetic fields above Hc17.2 T specific-heat data versus temperature show anomalies indicating a phase transition to an ordered state below T=1 K.
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