Novel functional materials are urgently needed to help combat the major global challenges facing humanity, such as climate change and resource scarcity. Yet, the traditional experimental materials discovery process is slow and the material space at our disposal is too vast to effectively explore using intuition-guided experimentation alone. Most experimental materials discovery programs necessarily focus on exploring the local space of known materials, so we are not fully exploiting the enormous potential material space, where more novel materials with unique properties may exist. Computation, facilitated by improvements in open-source software and databases, as well as computer hardware has the potential to significantly accelerate the rational development of materials, but all too often is only used to postrationalize experimental observations. Thus, the true predictive power of computation, where theory leads experimentation, is not fully utilized. Here, we discuss the challenges to successful implementation of computation-driven materials discovery workflows, and then focus on the progress of the field, with a particular emphasis on the challenges to reaching novel materials.

Chiral π-conjugated molecules bring new functionality to technological applications and represent an exciting, rapidly expanding area of research. Their functional properties, such as the absorption and emission of circularly polarised light or the transport of spin-polarised electrons, are highly anisotropic. As a result, the orientation of chiral molecules critically determines the functionality and efficiency of chiral devices. Here we present a strategy to control the orientation of a small chiral molecule (2,2'-dicyano[6]helicene, CN6H): the use of organic and inorganic templating layers. Such templating layers can either force CN6H molecules to adopt a face-on orientation and self-assemble into upright supramolecular columns oriented with their helical axis perpendicular to the substrate, or an edge-on orientation with parallel-lying supramolecular columns. Through such control, we show that low-and high-energy chiroptical responses can be independently 'turned on' or 'turned off'.The templating methodologies described here provide a simple way to engineer orientational control, and by association, anisotropic functional properties of chiral molecular systems for a range of emerging technologies. Main textConjugated organic materials have enabled considerable advances in consumer electronics, in part due to their low cost, tunable optical and electronic properties, and compatibility with flexible, large-area device architectures. The performance of such devices is not only influenced by molecular structure, but how these molecules assemble in the solid state, and how the resultant molecular assemblies are oriented with respect to device-relevant interfaces. Molecular chirality is increasingly recognised as a strategy to expand the functionality of such devices, enabling the realisation of next-generation displays, polarisation selective photodetectors, enantioselective biosensors and room-temperature spintronic devices. [1][2][3][4][5][6] When considering appropriate chiral conjugated small molecule materials for such applications, the archetypal example is the family of fused aromatics called the helicenes.These molecules are comprised of n≥5 ortho-fused angularly arranged benzene rings, which give rise to a non-planar screw-shaped skeleton. [7] The intrinsically chiral and fully conjugated molecular structure of the helicenes affords them outstanding anisotropic chiroptical and charge transport properties, as well as the ability to filter electron spins at room temperature. [8][9][10][11][12][13]

Amorphous metal–organic frameworks (aMOFs) are a class of disordered framework materials with a defined local order given by the connectivity between inorganic nodes and organic linkers, but absent long-range order. The rational development of function for aMOFs is hindered by our limited understanding of the underlying structure–property relationships in these systems, a consequence of the absence of long-range order, which makes experimental characterization particularly challenging. Here, we use a versatile modeling approach to generate in silico structural models for an aMOF based on Fe trimers and 1,3,5-benzenetricarboxylate (BTC) linkers, Fe-BTC. We build a phase space for this material that includes nine amorphous phases with different degrees of defects and local order. These models are analyzed through a combination of structural analysis, pore analysis, and pair distribution functions. Therefore, we are able to systematically explore the effects of the variation of each of these features, both in isolation and combined, for a disordered MOF system, something that would not be possible through experiment alone. We find that the degree of local order has a greater impact on structure and properties than the degree of defects. The approach presented here is versatile and allows for the study of different structural features and MOF chemistries, enabling the derivation of design rules for the rational development of aMOFs.

The existence of correlated disorder in molecular frameworks is an obvious mechanism by which unusual cooperative phenomena might be realised. We show that the use of local-symmetry lowering approaches can...