Parity-Forbidden Excitations ofRevealed by Optical Third-Harmonic Spectroscopy
- 31 August 2001
- journal article
- research article
- Published by American Physical Society (APS) in Physical Review Letters
- Vol. 87 (12) , 127006
- https://doi.org/10.1103/physrevlett.87.127006
Abstract
We present the first study of nonlinear optical third-harmonic generation (THG) in the strongly correlated charge-transfer insulator . 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 symmetry, participates in the third-harmonic susceptibility.
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