Polar magnetism and chemical bond in alpha-RuCl3

Abstract

Ruthenium trichloride is the subject of many recent experimental and theoretical studies. Johnson et al. infer a candidate for the magnetic structure (Cc2/m) from results gathered in an extensive set of experiments on an untwined sample of alpha-RuCl3 [R. D. Johnson et al., Phys. Rev. B 92, 235119 (2015)]. The proposed zigzag antiferromagnetic ground state of Ru ions does not respond to bulk magnetic probes. Properties of the candidate magnetic structure not previously explored include polar magnetism that supports Ru Dirac multipoles, e.g., a ruthenium anapole. In a general case, Dirac dipoles are capable of generating interactions between magnetic ions, as in an electrical Dzyaloshinskii-Moryia interaction [T. A. Kaplan and S. D. Mahanti, Phys. Rev. B 83, 174432 (2011) and H. J. Zhao et al., Nat. Mat. 20, 341 (2021)]. Dirac multipoles contribute to the diffraction of both x-rays and neutrons, and a stringent test of the magnetic structure Cc2/m awaits future experiments. From symmetry-informed calculations we show that, the magnetic candidate permits Bragg spots that arise solely from Dirac multipoles. Stringent tests of Cc2/m can also be accomplished by performing resonant x-ray diffraction with signal enhancement from the chlorine K-edge. X-ray absorption spectra published for alpha-RuCl3 possess a significant low-energy feature [K. W. Plumb et al., Phys. Rev. B 90, 041112(R) (2014)]. Many experimental studies of other Cl-metal compounds concluded that identical features hallmark the chemical bond. Using a monoclinic Cc2/m structure, we predict the contribution to Bragg diffraction at the Cl K-edge absorption. Specifically, the variation of intensity of Bragg spots with rotation of the sample about the reflection vector. The two principal topics of our studies, polar magnetism and the chemical bond in alpha-RuCl3, are brought together in a minimal model of magnetic Ru ions in Cc2/m.