Revealing Intrinsic Anisotropy of Collective Magnetic Excitations in Twinned Crystals of a Kitaev-Heisenberg Quantum Magnet

Abstract

Quantum magnets with competing interactions often emerge from delicate balances among microscopic parameters, making it essential to disentangle intrinsic spin dynamics from extrinsic disorder effects. Here, we introduce a multimodal optical approach combining magneto-infrared spectroscopy with domain-resolved micro-Raman spectroscopy at high magnetic fields to reconstruct the intrinsic magnetic excitation spectrum of twinned crystals of the Kitaev-Heisenberg quantum magnet Na${}_3$Co${}_2$SbO${}_6$. Far-infrared spectroscopy reveals multiple field-tunable magnetic excitations, but the intrinsic response is obscured by replica features arising from twin domains. By correlating magneto-infrared and domain-resolved Raman spectra, we isolate the single-domain magnon response and uncover a pronounced twofold in-plane magnon anisotropy. This anisotropy far exceeds that expected from the measured in-plane g-factor anisotropy and is instead dominated by anisotropic bond-dependent exchange interactions. By unifying high-field, high-resolution and spatially selective optical probes, our work establishes a broadly applicable framework for revealing intrinsic spin dynamics and constraining the spin Hamiltonian in multidomain quantum magnets.