The last decade has been characterized by a growing interest in liquid crystalline materials of increasing complexity (ferroelectrics, biaxial nematics, elastomers, dendrimers, etc.). The fundamental research on these materials, showing an optimal response to external stimula (e.g. electric and magnetic fields), is aimed to prepare the way to new technological breakthroughs. This book provides an extensive overview of how ab initio calculations combined with Nuclear Magnetic Resonance can be an indispensable tool to understand the relation among specific molecular structures, orientational ordering and the resulting magnetic, electrical and optical anisotropic responses shown by the mesophases formed. The integrated use of quantum-mechanical methods and NMR techniques clearly shows that the modeling is not only extremely useful to support the measurements but it becomes compulsory to go beyond the observable towards a deeper molecular-based knowledge of materials. This volume is aimed at graduate students, novices, librarians and experts around the world. It, indeed, provides a good reference material for readers interested in the liquid crystal research.