Parity-forbidden excitations of Sr(2)CuO(2)Cl(2) revealed by optical third-harmonic spectroscopy |
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| Authors: | Schumacher A B Dodge J S Carnahan M A Kaindl R A Chemla D S Miller L L |
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| Institution: | Department of Physics, University of California at Berkeley, Berkeley, CA 94720, USA. |
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| Abstract: | We present the first study of nonlinear optical third-harmonic generation (THG) in the strongly correlated charge-transfer insulator Sr(2)CuO(2)Cl(2). 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 state at 2 eV, with a(1g) symmetry, participates in the third-harmonic susceptibility. |
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