Spin-singlet ground state of the coupled Jeff = 12 alternating chain system Sr2 Co(SeO3)3

Abstract

We report a detailed study of the structural, magnetic, thermodynamic, and electronic properties of a coupled Jeff = 12 alternating chain Sr2Co(SeO3)3 compound using magnetic susceptibility χ(T), magnetic specific heat Cm(T), magnetization, and neutron diffraction measurements along with first-principles calculations. The first-principles calculations based on the density functional theory suggest that Sr2Co(SeO3)3 forms a quasi-one-dimensional chain with bond alternation and interchain interactions. χ(T), Cm(T), and neutron powder diffraction measurements confirm that no long-range magnetic ordering occurs down to 100 mK. Instead, a maximum in χ(T) and Cm(T) and an exponential drop of χ(T) and Cp(T) as T→0 K point to a spin-singlet ground state. The analysis of χ(T) and Cm(T) based on a J1-J2 alternating Heisenberg model shows the bond alternation α=J2/J1≈0.7 and a spin gap of Δ≈3 K. Our work demonstrates that Sr2Co(SeO3)3 is a coupled alternating chain system based on spin-orbit entangled Jeff = 12. © 2022 American Physical Society.