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Physica B Condensed Matter

Resonant two-magnon Raman scattering in two-dimensional Mott insulators

H. Onodera, Kenji Tsutsui, Takami Tohyama, Sadamichi Maekawa

Published Feb 28, 2003• 1 citation
Publisher
DOI
10.1016/s0921-4526(02)02526-7

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We investigate the resonant two-magnon Raman scattering in two-dimensional (2D) Mott insulators by using a half-filled 2D Hubbard model in the strong coupling limit. By performing numerical diagonalization calculations for small clusters, we find that the Raman intensity is enhanced when the incoming photon energy is not near the optical absorption edge but well above it, being consistent with experimental data. The absence of resonance near the gap edge is associated with the presence of background spins, while photoexcited states for resonance are found to be characterized by the charge degree of freedom. The resonance mechanism is different from those proposed previously.
Abstract Photoexcitation of a Mott insulator on a square lattice has weakened the intensity of both single- and two-magnon as observed in time-resolved resonant-inelastic x-ray scattering and time-resolved Raman scattering. However, the spectral change in low-energy regions below the magnons has not been clarified so far. To uncover the nature of photoinduced low-energy magnetic excitations of the Mott insulator, we numerically investigate transient magnetic dynamics in a photoexcited half-filled Hubbard model on the square lattice. After turning off a pump pulse tuned for an absorption edge, new magnetic signals clearly emerge well below magnon energy in both single- and two-magnon excitations. We find that the low-energy excitations are predominantly created via excitonic states at the absorption edge. These exciton-assisted magnetic excitations may provide a possible explanation for low-energy spectral weight in a recent time-resolved two-magnon Raman scattering experiment for insulating YBa2Cu3O6.1.
We investigate the excitation spectrum of a two-dimensional resonating valence bond (RVB) state. Treating the pi-flux phase with antiferromagnetic correlations as a variational ground state, we recover the long wavelength magnon as an "RVB exciton." However, this excitation does not exhaust the entire spectral weight and the high-energy spectrum is dominated by fermionic excitations. The latter can be observed directly by inelastic neutron scattering, and we predict their characteristic energy scales along different high symmetry directions in the magnetic Brillouin zone. We also interpret experimental results on two magnon Raman scattering and midinfrared absorption within this scenario.