The literature has shown numerous contributions on the synthesis and physicochemical properties of persistent organic radicals but there are a lesser number of reports about their use as building blocks for obtaining molecular magnetic materials exhibiting an additional and useful physical property or function. These materials show promise for applications in spintronics as well as bistable memory devices and sensing materials. This critical review provides an up-to-date survey to this new generation of multifunctional magnetic materials. For this, a detailed revision of the most common families of persistent organic radicals—nitroxide, triphenylmethyl, verdazyl, phenalenyl, and dithiadiazolyl—so far reported will be presented, classified into three different sections: materials with magnetic, conducting and optical properties. An additional section reporting switchable materials based on these radicals is presented (257 references).

Playing with organic radicals as building blocks for functional molecular materials

Publisher Summary Over the past 15–20 years, the non-linear optical (NLO) response of organic molecules has been of wide interest to organic and physical chemists, as well as physicists and chemical engineers. This interest arises from the possible use of such organic materials. In principle, photonics or the hybrid technology optoelectronics, both based on non-linear optical phenomena, can supersede electronics in communication technology. These technologies allow many operations that are currently effected with electron conduction to be replaced by operations based on light conduction. Many problems are encountered when it comes to the translation of a molecular property into a bulk property. It has transpired that some of these problems are not easy to solve with classical NLO-phores that mostly belong chemically to the class of merocyanine dyes. New design strategies for organic molecules and their respective bulk structures, crystals or oriented composite materials like polymers, are needed. Only a more fundamental understanding of these issues will allow rational optimization of molecular and bulk properties. This chapter surveys second-order molecular polarizabilities of organic molecules. Emphasis is given to the underlying of physical principles of non-linear optics (e.g. molecular topology), and to the establishment of structure–property relationships.

Organic Materials for Second-Order Non-Linear Optics

The second-order nonlinear optical properties of a family of rare-earth-based single chain magnets are presented (using a fundamental field at wavelength λ = 766 nm), together with an analysis of the origin of the second-harmonic generation (SHG) process. By studying the fundamental crystal symmetries and the geometrical arrangement of the constituting elements of the system in the unit cell we show that the main contribution to the nonlinear process arises from intermolecular π-stacking interactions.

Evidence of intermolecular π-stacking enhancement of second-harmonic generation in a family of single chain magnets

Multi-property materials: Magnetism and NLO properties

Static second hyperpolarizabilities γ of nitroxide radical and formaldehyde: evaluation of spatial contributions to γ by a hyperpolarizability density analysis

Hyperpolarizability of new nitro-aromatic-N-oxide species: nonlinear optical properties of a ferromagnetic organic material

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Hyperpolarizability of new nitro-aromatic-N-oxide species: nonlinear optical properties of a ferromagnetic organic material