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Signatures of nonlinear magnetoelectricity in second harmonic spectra of SU(2) symmetry broken quantum many-body systems

Quantum mechanical perturbative expressions for second order dynamical magnetoelectric (ME) susceptibilities have been derived and calculated for a small molecular system using the Hubbard Hamiltonian with SU(2) symmetry breaking in the form of spin-orbit coupling (SOC) or spin-phonon coupling. These susceptibilities will have signatures in second harmonic generation spectra. We show that SU(2) symmetry breaking is the key to generate these susceptibilities. We have calculated these ME coefficients by solving the Hamiltonian for low lying excited states using Lanczos method. Varying the Hubbard term along with SOC strength, we find spin and charge and both spin-charge dominated spectra of dynamical ME coefficients. We have shown that intensities of the peaks in the spectra are highest when the magnitudes of Hubbard term and SOC coupling term are in similar range.