The planar triangular $S=3/2$ magnet AgCrSe${}_2$: magnetic frustration, short range correlations, and field tuned anisotropic cycloidal magnetic order

Abstract

Our studies evidence an anisotropic magnetic order below $T_N=32$~K. Susceptibility data in small fields of about 1~T reveal an antiferromagnetic (AFM) order for $H\perp c$, whereas for $H\parallel c$ the data are reminiscent of a field-induced ferromagnetic (FM) structure. At low temperatures and for $H\perp c$, the field-dependent magnetization and AC susceptibility data evidence a metamagnetic transition at $H^{+}=5$~T, which is absent for $H\parallel c$. We assign this to a transition from a planar cycloidal spin structure at low fields to a planar fan-like arrangement above $H^{+}$. A fully FM polarized state is obtained above the saturation field of $H_{\perp S}=23.7$~T at 2~K with a magnetization of $M_s=2.8$~${\mu }_{\mathrm{B}}/Cr$. For $H\parallel c$, $M(H)$ monotonously increases and saturates at the same $M_s$ value at $H_{\parallel S}=25.1$~T at 4.2~K. Above $T_N$, the magnetic susceptibility and specific heat indicate signatures of two dimensional (2D) frustration related to the presence of planar ferromagnetic and antiferromagnetic exchange interactions. We found a pronounced nearly isotropic maximum in both properties at about $T^{\ast }=45$~K, which is a clear fingerprint of short-range correlations and emergent spin fluctuations. Calculations based on a planar 2D Heisenberg model support our experimental findings and suggest a predominant FM exchange among nearest and AFM exchange among third-nearest neighbors. Only a minor contribution might be assigned to the antisymmetric Dzyaloshinskii-Moriya interaction possible related to the non-centrosymmetric polar space group $R3m$. Due to these competing interactions, the magnetism in AgCrSe${}_2$, in contrast to the oxygen based delafossites, can be tuned by relatively small, experimentally accessible, magnetic fields, allowing us to establish the complete anisotropic magnetic $H-T$ phase diagram in detail.

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• Magnetodielectric Properties in Two Dimensional Magnetic Insulators
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