Signatures of spin-triplet excitations in optical conductivity of valence bond solids

We show that the optical responses below the Mott gap can be used to probe the spin-triplet excitations in valence bond solid (VBS) phases in Mott insulators. The optical conductivity in this regime arises due to the electronic polarization mechanism via virtual electron-hopping processes. We apply this mechanism to the Hubbard model with spin-orbit couplings and/or the corresponding spin model with significant Dzyaloshinskii-Moriya (DM) interactions, and compute the optical conductivity of VBS states on both ideal and deformed Kagome lattices. In the case of the deformed Kagome lattice, we study the antiferromagnet Rb₂Cu₃SnF₁₂ with the pinwheel VBS state. In case of the ideal Kagome lattice, we explore the optical conductivity signatures of the spin-triplet excitations for three VBS states with (1) a 12-site unit cell, (2) a 36-site unit cell with six-fold rotation symmetry, and (3) a 36-site unit cell with three-fold rotation symmetry, respectively. We find that increasing the DM interactions generally leads to broad and smooth features in the optical conductivity with interesting experimental consequences. The optical conductivity reflects the features of the spin-triplet excitations that can be measured in future experiments.