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The results of pseudopotential calculations of the band structure and related electronic and optical properties of quasi-binary (GaP)(ZnSe) crystals in the zinc blende structure are presented. Trends in bonding and ionicity are discussed in terms of electronic charge densities. Moreover, the composition dependence of the refractive index and dielectric constants are reported. The computed values are in reasonable agreement with experimental data. The results suggest that for a proper choice of the composition x, (GaP)(ZnSe) could provide more diverse opportunities to achieve the desired electronic and optical properties of the crystals which would improve the performances of devices fabricated on them. [ABSTRACT FROM AUTHOR]