In addition to possessing strong optical nonlinearity, the (-)-2-(alpha-met
hylbenzylamino)-5-nitropyridine (MBANP) crystal has been shown to have unus
ual linear optical properties. Two methyl derivatives of MBANP have now bee
n synthesized and grown as large single crystals; their refractive indices
have been measured as a function of frequency and second-harmonic generatio
n, including the determination of the phase matching loci has been investig
ated. Data is also available on the racemic form of crystalline MBANP. The
properties of this family of crystals have been reviewed and an attempt is
made to relate the experimental responses of the crystals to their molecula
r structure and the calculated properties of the molecules.