Abstract
Frustrated quasidoublets without time-reversal symmetry can host highly unconventional magnetic structures with continuously distributed order parameters even in a single-phase crystal. Here, we report the comprehensive thermodynamic and neutron diffraction investigation on the single crystal of TmMgGaO$_4$, which entails non-Kramers Tm$^{3+}$ ions arranged on a geometrically perfect triangular lattice. The crystal electric field (CEF) randomness caused by the site-mixing disorder of the nonmagnetic Mg$^{2+}$ and Ga$^{3+}$ ions, merges two lowest-lying CEF singlets of Tm$^{3+}$ into a ground-state (GS) quasidoublet. Well below $T_c$ $\sim$ 0.7 K, a small fraction of the antiferromagnetically coupled Tm$^{3+}$ Ising quasidoublets with small inner gaps condense into two-dimensional (2D) up-up-down magnetic structures with continuously distributed order parameters, and give rise to the \emph{columnar} magnetic neutron reflections below $\mu_0H_c$ $\sim$ 2.6 T, with highly anisotropic correlation lengths, $\xi_{ab}$ $\geq$ 250$a$ in the triangular plane and $\xi_c$ $<$ $c$/12 between the planes. The remaining fraction of the Tm$^{3+}$ ions remain nonmagnetic at 0 T and become uniformly polarized by the applied longitudinal field at low temperatures. We argue that the similar model can be generally applied to other compounds of non-Kramers rare-earth ions with correlated GS quasidoublets.
Highlights
Geometrical frustration can render the ground state(s) (GS) of the correlated spin system macroscopically degenerate and completely disordered in the classical Ising case [1,2,3,4,5,6] or trigger strong quantum fluctuations that prevent the conventional symmetry breaking even down to ∼0 K in the quantum case [7,8,9,10,11,12,13,14,15]
We show that frustrated quasidoublets without time-reversal symmetry can host highly unconventional magnetic structures with continuously distributed order parameters even in a single-phase crystal
The many-body correlated physics may be significantly changed when Yb3þ is replaced by the non-Kramers Tm3þ (4f12) ion on the triangular lattice, as the time-reversal symmetry is no longer preserved, and the previously symmetry-protected degeneracy of the GS crystal electric field (CEF) doublet may get “lifted.” And exotic quantum phases may emerge in the new frustrated magnet, TmMgGaO4
Summary
Geometrical frustration can render the ground state(s) (GS) of the correlated spin system macroscopically degenerate and completely disordered in the classical Ising case [1,2,3,4,5,6] or trigger strong quantum fluctuations that prevent the conventional symmetry breaking even down to ∼0 K in the quantum case [7,8,9,10,11,12,13,14,15]. The many-body correlated physics may be significantly changed when Yb3þ is replaced by the non-Kramers Tm3þ (4f12) ion on the triangular lattice, as the time-reversal symmetry is no longer preserved, and the previously symmetry-protected degeneracy of the GS CEF doublet may get “lifted.” And exotic quantum phases may emerge in the new frustrated magnet, TmMgGaO4. At low temperatures and in small longitudinal fields, a fraction of the Tm3þ ions—those characterized by a small gap between the two CEF singlets—give rise to the novel 2D Ising up-up-down (uud) phase with the continuously distributed order parameter, under the frustrated intersite couplings on the triangular lattice. A similar model can be generally applied to other non-Kramers rare-earth magnets with correlated GS quasidoublets
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