Raman scattering study of multimagnon (bi- and tri-magnon) excitations and rotonlike points in the distorted triangular lattice antiferromagnet

Abstract

We investigate the experimental signatures of Raman spectroscopy of bi- and tri-magnon excitations in the distorted triangular lattice antiferromagnets alpha-LCr2O4 (L=Sr, Ca). We utilize spin wave theory to analyze the nearly 120 degree spin-3/2 spiral ordered antiferromagnetic ground state to compute the single-magnon density of states, single-magnon dispersion, and bimagnon and trimagnon Raman spectra (polarized and unpolarized). It is found that Raman scattering is capable of capturing the effect of the rotonlike M and M' points on the bimagnon Raman spectrum. Our calculation confirms the connection between single-magnon rotonlike excitation energy and bimagnon Raman excitation spectrum observed experimentally. The roton energy minimum in momentum space is half of the energy of a bimagnon excitation signal. The experimental magnetic Raman scattering result displays two peaks which have a Raman shift of 15 meV and 40 meV, respectively. Theoretical modeling and analysis of the experimental spectrum of alpha-SrCr2O4 within our distorted Heisenberg Hamiltonian lattice suggests that the low-energy peak at 15 meV is associated with the bimagnon excitation, whereas the high-energy peak around 40 meV is primarily a trimagnon excitation. Based on our fitting procedure we propose a new set of magnetic interaction parameters for alpha-SrCr2O4. These parameters reproduce not only the experimental Raman spectrum, but also the inelastic neutron scattering response (including capturing high energy magnon branches). We also compute the unpolarized bimagnon and trimagnon Raman spectra for alpha-CaCr2O4. Furhtermore, we found that the polarization sensitivity of Raman spectrum can be utilized to distinguish the bi- and tri-magnon excitation channels.