Six RT-substituted derivatives of 2-methyl-4-nitroaniline (MNA) and tw
o N-substituted derivatives of 4-nitroaniline were synthesized and the
ir physical and optical properties were examined in the search for non
linear optical materials with a sufficiently large second harmonic (SH
) activity and applicability to practical use. Some derivatives produc
ed single crystals and their structures were determined by X-ray cryst
allography. The trends of the SH intensity of these materials could be
qualitatively explained based on the b tensor (the effective molecula
r hyperpolarizability in the crystal). Amongst the derivatives examine
d in this investigation, N-benzyl-MNA showed the highest SH activity (
up to twice that of MNA), thermostability and phase-matching ability.