Abstract

The singlet ground state magnetism in pyrochlore osmates Y2_2Os2_2O7_7 and Ho2_2Os2_2O7_7 is studied by DC and AC susceptibility, specific heat, and neutron powder diffraction measurements. Despite the expected non-magnetic singlet in the strong spin-orbit coupling (SOC) limit for Os4+^{4+} (5d45d^4), Y2_2Os2_2O7_7 exhibits a spin-glass (SG) ground state below 4 K with weak magnetism, suggesting possible proximity to a quantum phase transition between the non-magnetic state in the strong SOC limit and the magnetic state in the strong superexchange limit. Ho2_2Os2_2O7_7 has the same structural distortion as occurs in Y2_2Os2_2O7_7. However, the Os sublattice in Ho2_2Os2_2O7_7 shows long-range magnetic ordering below 36\,K. The sharp difference of the magnetic ground state between Y2_2Os2_2O7_7 and Ho2_2Os2_2O7_7 signals the singlet ground state magnetism in R2R_2Os2_2O7_7 is fragile and can be disturbed by the weak 4f−5d4f-5d interactions.

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