Abstract
This chapter discusses various aspects of hydrogen bonding in molecular magnetic materials with a focus on magnetic and exchange effects in π-conjugation organic nitroxide-based radicals where hydrogen bonding is important either to organize the molecules in the solid state, or as a direct electronic exchange linkage, or both. The attachment of phenolic groups to radical fragments provided some of the first examples of hydrogen-bond guided crystal assembly in organic magnetic materials. The balance of information indicates that 4HOPhNN acts as a quasi-2D or 3D organic ferromagnet. It is found that deuterium substitution on the OH groups of HQNN decreases the FM interaction, supporting an electronic role for the OH groups in the overall magnetic behavior. NMR measurements were used to deduce a negative spin density on the OH group that is ortho to the nitronylnitroxide group in HQNN. The chapter explains the bio-inspired molecular recognition for crystal assembly. The exchange and crystal assembly in nitronylnitroxides with hydrogen-bonding azaarenes is also elaborated.
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