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Co-existing Singlet and Ordered S=1/2 Moments in the Ground State of the Triclinic Quantum Magnet CuMoO4

CuMoO4 is a triclinic quantum magnet based on S = 1/2 moments at the Cu2+ site. It has recently attracted interest due to the remarkable changes in its chromic and volumetric properties at high temperatures, and in its magnetic properties at low temperatures. This material exhibits a first order structural phase transition at T_C ~ 190 K as well as a magnetic phase transition at T_N ~ 1.75 K. We report low temperature heat capacity measurements as well as extensive elastic and inelastic neutron scattering measurements on powder samples taken above and below T_N. We observe neutron diffraction consistent with a simple (1/2, 0, 0) antiferromagnetic structure indicating a doubling of the a-axis periodicity below T_N. In addition, inelastic neutron scattering above a spin gap of ~ 2.3 meV is consistent with triplet excitations out of paired S = 1/2 moments which form singlet dimers. Low lying spin wave excitations are also observed and these originate from ordered S = 1/2 moments below T_N. Taken together these measurements show the ground state of CuMoO4 to display both non-magnetic singlets, and ferromagnetically-coupled spins coexisting within an antiferromagnetic structure below T_N ~ 1.75 K.