Polarized Raman Response of Two-Dimensional Quasiperiodic Antiferromagnets: Configuration-Interaction versus Green's Function Approaches

We study Raman response of Heisenberg antiferromagnets on the $\mathbf{C}_\mathrm{5v}$ Penrose and $\mathbf{C}_\mathrm{8v}$ Ammann-Beenker lattices within and beyond the Loudon-Fleury second-order perturbation scheme intending to explore optical features peculiar to quasiperiodic magnets. Within the Loudon-Fleury mechanism, we find one and only Raman-active mode of $\mathrm{E}_2$ symmetry without any dependence on linear incident and scattered polarizations. Beyond the Loudon-Fleury mechanism, two more symmetry species $\mathrm{A}_1$ and $\mathrm{A}_2$ are activated via dynamic ring exchange and chiral spin fluctuations, respectively, which can be extracted by the use of circular as well as linear polarizations. We employ Green's functions on one hand and configuration-interaction wavefunctions on the other hand to calculate the multimagnon contributions to inelastic light scatterings. Demonstrating the great advantage of the configuration-interaction scheme, we reveal that a major portion of the Shastry-Shraiman fourth-order Raman intensity is mediated by multimagnon fluctuations.

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