Determination of the Distributions of the Spin-Hamiltonian Parameters in Spin Triangles: A Combined Magnetic Susceptometry and Electron Paramagnetic Resonance Spectroscopic Study of the Highly Symmetric [Cr3O(PhCOO)6(py)3](ClO4)·0.5py

Magnetic susceptibility and X-band electron paramagnetic resonance (EPR) studies have been carried out on the highly symmetric [Cr 3 O(PhCOO) 6 (py) 3 ](ClO 4 )·0.5py (1; py = pyridine), whose cation exhibits a D 3 h crystallographically imposed molecular symmetry. While magnetic susceptibility data can be interpreted with an equilateral magnetic model described by the effective multispin Hamiltonian Ĥ = -2 J(Ŝ 1 ·Ŝ 2 + Ŝ 2 ·Ŝ 3 + Ŝ 3 ·Ŝ 1 ), EPR data require an isosceles model described by the multispin Hamiltonian Ĥ = -2 J( Ŝ 1 · Ŝ 2 + Ŝ 2 · Ŝ 3 ) - 2 J' Ŝ 3 · Ŝ 1 , where Δ J = J - J' ≠ 0. Moreover, EPR data reveal the interplay of antisymmetric exchange (or Dzyaloshinskii-Moriya) interactions, described by a 2G(Ŝ 1 × Ŝ 2 + Ŝ 2 × Ŝ 3 + Ŝ 3 × Ŝ 1 ) term, which induce significant anisotropy to the S T = 1 / 2 ground state of 1, as well as an important broadening of the g ⊥ resonance ( g strain). Through careful analysis of these data and in conjunction with neutron scattering data, this g strain can be deconvoluted into distributions of the individual spin-Hamiltonian parameters Δ J and |G|. This method of analysis provides simultaneous estimates of the central values and distribution profiles of the spin-Hamiltonian parameters, which are shown not to be described by monodisperse values.