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We present the first study of nonlinear optical third harmonic generation inthe strongly correlated charge-transfer insulator Sr2CuO2Cl2. For fundamentalexcitation in the near-infrared, the THG spectrum reveals a strongly resonantresponse for photon energies near 0.7 eV. Polarization analysis reveals thisnovel resonance to be only partially accounted for by three-photon excitationto the optical charge-transfer exciton, and indicates that an even-parityexcitation at 2 eV, with a_1g symmetry, participates in the third harmonicsusceptibility.Comment: Requires RevTeX v4.0beta

physical review letters

Parity-Forbidden Excitations of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi>Sr</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mrow><mml:mi>CuO</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mrow><mml:mi>Cl</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>Revealed by Optical…

Parity-Forbidden Excitations ofSr2CuO2Cl2Revealed by Optical…