Crystal Structure Prediction

In most NMR crystallography applications experimental techniques are used to build an appropriate structural model, which can be later refined using quantum-chemical calculations. In some cases, this can be viewed as an obstacle, in particular when structural constraints extracted from the experimental data are ambiguous or not abundant enough. One of the most promising solutions to this problem is crystal structure prediction (CSP). On the other hand, for complicated, flexible and/or multicomponent systems the number of degrees of freedom (DOF) which need to be accounted for in CSP starts to be overwhelming, thus limiting the applicability of this computational method. In such instances, structural constraints extracted from solid-state NMR spectra can help to reduce this vast number to a perfectly manageable number of DOFs, making a combination of NMR crystallography and CSP calculations a very powerful approach. This chapter focuses on the applicability of CSP in the context of NMR crystallography, including a brief overview of modern CSP approaches, together with their advantages and limitations.