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We have investigated the transient third-order optical nonlinearity of the solutions of Metal(dmit)2/(mnt)2 salts in acetone by employing femtosecond optical Kerr gate measurement at 830 nm wavelength. An order of enhancement on the second-order hyperpolarizability is found for the above salts with central atoms of Cu and Ni. We have suggested an explanation for the enhancement based on the extension of electronic conjugation by the centring Cu or Ni atom.