This contribution summarizes some of the theoretical strategies developed in the recent past to study systems with an increasing size and complexity by means of accurate extended CI calculations. Some examples of the capabilities of these strategies are also given, concerning the evaluation of magnetic exchange constants, as well as many other effective interaction parameters, such as hopping integrals, on‐site Coulomb repulsion, four‐body exchange term, … on 2D and spin‐ladder cuprates, polyoxovanadates, as well as polynuclear molecular compounds.

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