Parity forbidden excitations of Sr2CuO2Cl2 revealed by optical third-harmonic spectroscopy

Abstract

We present the first study of nonlinear optical third harmonic generation in the strongly correlated charge-transfer insulator Sr2CuO2Cl2. For fundamental excitation in the near-infrared, the THG spectrum reveals a strongly resonant response for photon energies near 0.7 eV. Polarization analysis reveals this novel resonance to be only partially accounted for by three-photon excitation to the optical charge-transfer exciton, and indicates that an even-parity excitation at 2 eV, with a_1g symmetry, participates in the third harmonic susceptibility.

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References in corpus (2)

• Electronic Structure of Mott Insulators Studied by Inelastic X-ray Scattering
• Evidence of phonon mediated coupling between charge transfer and ligand field excitons in Sr${}_2$CuO${}_2$Cl${}_2$

Cited by in corpus (6)

• Optical study of orbital excitations in transition-metal oxides
• Dimensionality dependence of optical nonlinearity and relaxation dynamics in cuprates
• Nonlinear Optical Response in two-dimensional Mott Insulators
• Symmetry of Photoexcited States and Large-Shift Raman Scattering in Two-Dimensional Mott Insulators
• Implications of second harmonic generation for hidden order in Sr${}_2$CuO${}_2$Cl${}_2$
• Electronic Structure and Linear Optical Properties of Sr${}_2$CuO${}_2$Cl${}_2$ Studied from the First Principles Calculation