Microscopic Description of Electric and Magnetic Toroidal Multipoles in Hybrid Orbitals

We present a general formalism of multipole descriptions under the space-time inversion group. We elucidate that two types of atomic toroidal multipoles, i.e., electric and magnetic, are fundamental pieces to express electronic order parameters in addition to ordinary electric and magnetic multipoles. By deriving quantum-mechanical operators for both toroidal multipoles, we show that electric (magnetic) toroidal multipole higher than dipole (monopole) can become a primary order parameter in a hybridized-orbital system. We also demonstrate emergent cross-correlated couplings between electric, magnetic, and elastic degrees of freedom, such as magneto-electric and magneto(electro)-elastic couplings, under toroidal multipole orders.