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

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Summary

INTRODUCTION

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

TECHNICAL DETAILS
SINGLE-ION PHYSICS
FITS TO THERMODYNAMIC DATA
PARTIAL UP-UP-DOWN ORDER
VIII. CONCLUSIONS
Findings
Rln2 Hc

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