Two novel charge-transfer (CT) heteropoly complexes, (C8HlzN2)5H7PMo1204o (i) and (Cs]rI12N2)3H 3-PMOlaO4o'5H:O (2), prepared by reacting pMezNC6H4NH 2 with the four-electron heteropoly blue HTPMo 12040 '12H20 and heteropoly acid H3PMo1204o . xH20, respectively, were characterized by elemental analysis, and u.v., i.r., XPS and e.s.r, spectroscopies. A sizable electron-transfer interaction occurs within the product molecules and the heteropoly anions retain their Keggin structure. Their third-order optical non-linearity coefficients were measured using the Z-scan technique ~)

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