CuInSe2 single crystals were epitaxially grown on (001) GaP, (001) GaA
s, and (110) GaP by the halogen transport Method. The orientation rela
tionships in the growth on the (001) and (110) faces were (a) [001]CuI
nSc2 parallel-to [001]sub and [100]CuInSe2 parallel-to [100]sub (c-axi
s orientation growth), and (b) [110]CuInSe2 parallel-to [110]sub and [
001]CuInSe2 parallel-to [001]sub, respectively. On (001) InP, the orie
ntation relationships between the layer and substrate consist of two s
ets: (c) [100]CuInSe2 parallel-to [001]sub and [001]CuInSe2 parallel-t
o [010]sub, and (d) [100]CuInSe2 parallel-to [001]sub and [001]CuInSe2
parallel-to [100BAR]sub (a-axis orientation growth). The above result
s, i.e., c-axis growth on (001) GaP and (001) GaAs and a-axis growth o
n (001) InP, could be explained by a criterion of the minimum lattice
mismatch between grown layers and substrates. A series of growth exper
iments on (001) GaAs indicated that appropriate gas etching of the sub
strate surface and growth temperature were required for obtaining twin
-free single-crystal epitaxial CuInSe2.