Ab. Schumacher et al., Parity-forbidden excitations of Sr2CuO2Cl2 revealed by optical third-harmonic spectroscopy - art. no. 127006, PHYS REV L, 8712(12), 2001, pp. 7006
We present the first study of nonlinear optical third-harmonic generation (
THG) in the strongly correlated charge-transfer insulator Sr2CuO2Cl2. For f
undamental excitation in the. near infrared, the THG spectrum reveals a str
ongly resonant response for photon energies near 0.7 eV. Polarization analy
sis reveals this novel resonance to, be only partially accounted for by thr
ee-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.