Theory of inelastic light scattering in spin-1 systems: resonant regimes and detection of quadrupolar order

Abstract

Motivated by the lack of an obvious spectroscopic probe to investigate non-conventional order such as quadrupolar orders in spin S>1/2 systems, we present a theoretical approach to inelastic light scattering for spin-1 quantum magnets in the context of a two-band Hubbard model. In contrast to the S=1/2 case, where the only type of local excited state is a doubly occupied state of energy $U$, several local excited states with occupation up to 4 electrons are present. As a consequence, we show that two distinct resonating scattering regimes can be accessed depending on the incident photon energy. For $\hslash {\omega }_{in}\lesssim U$, the standard Loudon-Fleury operator remains the leading term of the expansion as in the spin-1/2 case. For $\hslash {\omega }_{in}\lesssim 4U$, a second resonant regime is found with a leading term that takes the form of a biquadratic coupling $\sim({\bf S}_{i}\cdot{\bf S}_{j)^{2}$. Consequences for the Raman spectra of S=1 magnets with magnetic or quadrupolar order are discussed. Raman scattering appears to be a powerful probe of quadrupolar order.

10 Pages, 6 Figures, Submitted to PRB

References in corpus (9)

• Inelastic Light Scattering From Correlated Electrons
• The quadrupolar phases of the S=1 bilinear-biquadratic Heisenberg model on the triangular lattice
• Three-sublattice ordering of the SU(3) Heisenberg model of three-flavor fermions on the square and cubic lattices
• Interplay of thermal and quantum spin fluctuations on the kagome lattice
• Microscopic origin of isotropic non-Heisenberg behavior in highly correlated systems
• Neel order, ring exchange and charge fluctuations in the half-filled Hubbard model
• How to detect weak emergent broken-symmetries of the Kagome antiferromagnet from Raman spectroscopy
• Theory of two magnon Raman scattering in antiferromagnetic iron pnictides
• Raman scattering in a Heisenberg {\boldmath $S=1/2$} antiferromagnet on the triangular lattice

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