Molecular engineering to control the magnetic interaction between single-chain magnets assembled in a two-dimensional network.

Two two-dimensional (2D) systems having the formula [{Fe(III)(dmbpy)(CN)(4)}(2)Co(II)L](n) [L = pyetNO (1), tvpNO (2)] and consisting of single-chain magnets connected through organic ligands (L) have been prepared, and their magnetic properties have been investigated. The overall magnetic behavior depends on the capacity of the organic pillars to transmit long-range magnetic interactions. 1 is the first example of a 2D compound exhibiting double relaxation of the magnetization, whereas 2 behaves as a metamagnet.