  A comparison is made between the degree of spin polarization of electrons
excited by one- and two-photon absorption of circularly polarized light in bulk
zincblende semiconductors. Time- and polarization-resolved experiments in
(001)-oriented GaAs reveal an initial degree of spin polarization of 49% for
both one- and two-photon spin injection at wavelengths of 775 and 1550 nm, in
agreement with theory. The macroscopic symmetry and microscopic theory for
two-photon spin injection are reviewed, and the latter is generalized to
account for spin-splitting of the bands. The degree of spin polarization of
one- and two-photon optical orientation need not be equal, as shown by
calculations of spectra for GaAs, InP, GaSb, InSb, and ZnSe using a 14x14 k.p
Hamiltonian including remote band effects. By including the higher conduction
bands in the calculation, cubic anisotropy and the role of allowed-allowed
transitions can be investigated. The allowed-allowed transitions do not
conserve angular momentum and can cause a high degree of spin polarization
close to the band edge; a value of 78% is calculated in GaSb, but by varying
the material parameters it could be as high as 100%. The selection rules for
spin injection from allowed-allowed transitions are presented, and interband
spin-orbit coupling is found to play an important role.
