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For GaAs we have determined j 2 xyz ÿ2!; !; !j in second-harmonic generation experiments using two-photon energies between 2 and 5 eV. In addition to the E 1 , E 1 1 , E 0 0 , and E 2 critical-point bulk transitions of GaAs, a surprisingly strong surface transition at 3.35 eV was observed for natively oxidized GaAs(001) samples. A detailed comparison with theoretical predictions reveals that calculations that include many-particle effects at the level of the "scissors" approximation candoi:10.1103/physrevlett.90.036801 pmid:12570514 fatcat:57o2elo5xvepjc2vkv3y5btmka