This paper reports the synthesis, structure and properties of two coordinat
ion compounds which are transparent in the visible region and show a relati
vely strong nonlinear optical (NLO) effect. The first crystal, Zn(2-NH(2)py
)(2)Cl-2 (2-aminopyridine zinc dichloride, DAZC), shows a SHG (second harmo
nic generation) effect 8 times as strong as that of KDP. X-ray single cryst
al structure analysis reveals that the molecule possesses a tetrahedron con
figuration around the zinc atom, and ail the molecules are aligned in an al
most fully parallel direction. The second compound, Zn(acac)(2)(PhTU) (phen
ylthiourea zinc diacetylacetate, PZDA), shows a powder SHG effect as strong
as 10 times that of KDP. X-ray single crystal structure analysis shows tha
t the molecule possesses a square pyramidal configuration around the zinc i
on, and the molecules are aligned almost in a parallel arrangement in the l
attice. These two crystals may represent a novel strategy for designing new
transparent NLO materials.