The isomorphous series of complexes A,InX, . H,O (A = K, NH,, Rb, Cs; X = CI, Br) was investigated by "CI, 79*81Br, and '"In nuclear quadrupole resonance spectroscopy. For the bromine compounds the temperature dependence of the NQR spectra was studied in the range 77 5 T/K s 380. Solid state phase transitions are found for K,InBr5 . H 2 0 at T = 145.5 K and for (NH,),InBr, . H 2 0 at T = 82 K. The "Br NQR frequencies are observed between 65 and 80 MHz. At room temperature the "CI NQR frequencies are found in the range 9.8 sv (35Cl)/MHz 5 11.6. The nuclear quadrupole coupling constants 1e2 @z,Qh-l ("'In) [in the compounds vary between 60 MHz and 115 MHz. There is a marked dependence o f ) e 2 @ Q h -' ("'In)Jon cation radius rA and temperature. le2 @,Qh-' ("'In)lincreases with increasing rA. and such a dependence is observed for too. As a function of temperature, t]("'In) goes through 1. On the basis of the semiempirical MO model of Townes and Dailey the covalent character of the bond In-Halogen is estimated. From this the increase of le2 @,Qh-' ("'In) land of v('lBr) is understood to be due to small changes in the bond character with r A and with temperature... -730, Japan. times TI and T2 are very short, causing strong line broaden-Ber. Bunsenges. Phys. Chem. 87, 932-944 (1983) -0