Chemical tuning of a honeycomb magnet through a critical point

Abstract

BaCo2(AsO4)2 (BCAO) has seen extensive study since its initial identification as a proximate Kitaev quantum spin liquid candidate. Thought to be described by the highly anisotropic XXZ-J_1-J_3 model, the ease with which magnetic order is suppressed in the system indicates proximity to a spin liquid phase. Upon chemical tuning via partial arsenic substitution with vanadium, we show an initial suppression of long-range incommensurate order in the BCAO system to T = 3.0 K, followed by increased spin freezing at higher substitution levels. Between these two regions, at around 10% substitution, the system is shown to pass through a critical point where the competing J_1/J_3 exchange interactions become more balanced, producing a more complex magnetic ground state, likely stabilized by quantum fluctuations. This state shows how slight compositional change in magnetically-frustrated systems may be leveraged to tune ground state degeneracies and potentially realize a quantum spin liquid state.

Main text (43 pages, 9 figures, 1 table); Supplementary information (32 pages, 18 figures, 14 tables)

References in corpus (12)

• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Weak-field induced nonmagnetic state in a Co-based honeycomb
• Geometrical frustration versus Kitaev interactions in BaCo${}_2$(AsO${}_4$)${}_2$
• Tunable Magnetic Transition to a Singlet Ground State in a 2D Van der Waals Layered Trimerized Kagomé Magnet
• A magnetic continuum observed by terahertz spectroscopy in a quantum spin liquid candidate BaCo${}_2$(AsO${}_4$)${}_2$
• XY magnetism, Kitaev exchange, and long-range frustration in the $J_{\mathrm{eff}}=1/2$ honeycomb cobaltates
• Polarized-neutron investigation of magnetic ordering and spin dynamics in BaCo${}_2$(AsO${}_4$)${}_2$ frustrated honeycomb-lattice magnet
• Evidence of discrete energy states and cluster-glass behavior in Sr${}_{2-x}$La${}_x$CoNbO${}_6$
• Spin-glass state and reversed magnetic anisotropy induced by Cr doping in the Kitaev magnet $\alpha$-RuCl${}_3$
• Structural properties and Raman spectra of columbite-type NiNb${}_{2-x}$V${}_x$O${}_6$ synthesized under high pressure
• Ferromagnetic cluster-glass phase in Ca(Co,Ir)2As2 crystals
• Evolution of Magnetism in the $N{a}_{3-d}N{a}_{1-x}M{g}_{x}I{r}_2{O}_6$ Series of Honeycomb Iridates

Cited by in corpus (2)

• Continuum of spin excitations in an ordered magnet
• Spin-orbit entangled moments and magnetic exchange interactions in cobalt-based honeycomb magnets BaCo${}_2$($X$O${}_4$)${}_2$ ($X$ = P, As, Sb)