High-throughput computational materials design is an emerging area of materials science. By combining advanced thermodynamic and electronic-structure methods with intelligent data mining and database construction, and exploiting the power of current supercomputer architectures, scientists generate, manage and analyse enormous data repositories for the discovery of novel materials. In this Review we provide a current snapshot of this rapidly evolving field, and highlight the challenges and opportunities that lie ahead.

Few-layer black phosphorus (BP) is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of environmental stability severely limits its synthesis and processing. Here we demonstrate that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP). Nanosheets are surprisingly stable in CHP, probably due to the solvation shell protecting the nanosheets from reacting with water or oxygen. Experiments, supported by simulations, show reactions to occur only at the nanosheet edge, with the rate and extent of the reaction dependent on the water/oxygen content. We demonstrate that liquid-exfoliated BP nanosheets are potentially useful in a range of applications from ultrafast saturable absorbers to gas sensors to fillers for composite reinforcement.

The ability to manipulate electron spin in organic molecular materials offers a new and extremely tantalizing route towards spin electronics, both from fundamental and technological points of view. This is mainly due to the unquestionable advantage of weak spin-orbit and hyperfine interactions in organic molecules, which leads to the possibility of preserving spin-coherence over times and distances much longer than in conventional metals or semiconductors. Here we demonstrate theoretically that organic spin valves, obtained by sandwiching an organic molecule between magnetic contacts, can show a large bias-dependent magnetoresistance and that this can be engineered by an appropriate choice of molecules and anchoring groups. Our results, obtained through a combination of state-of-the-art non-equilibrium transport methods and density functional theory, show that although the magnitude of the effect varies with the details of the molecule, large magnetoresistance can be found both in the tunnelling and the metallic limit.

The electron spin made its debut in the device world only two decades ago but today our ability of detecting the spin state of a moving electron underpins the entire magnetic data storage industry. This technological revolution has been driven by a constant improvement in our understanding on how spins can be injected, manipulated and detected in the solid state, a field which is collectively named Spintronics. Recently a number of pioneering experiments and theoretical works suggest that organic materials can offer similar and perhaps superior performances in making spin-devices than the more conventional inorganic metals and semiconductors. Furthermore they can pave the way for radically new device concepts. This is Molecular Spintronics, a blossoming research area aimed at exploring how the unique properties of the organic world can marry the requirements of spin-devices. Importantly, after a first phase, where most of the research was focussed on exporting the concepts of inorganic spintronics to organic materials, the field has moved to a more mature age, where the exploitation of the unique properties of molecules has begun to emerge. Molecular spintronics now collects a diverse and interdisciplinary community ranging from device physicists to synthetic chemists to surface scientists. In this critical review, I will survey this fascinating, rapidly evolving, field with a particular eye on new directions and opportunities. The main differences and challenges with respect to standard spintronics will be discussed and so will be the potential cross-fertilization with other fields (177 references).

Ab initio computational methods for electronic transport in nanoscaled systems are an invaluable tool for the design of quantum devices. We have developed a flexible and efficient algorithm for evaluating I-V characteristics of atomic junctions, which integrates the nonequilibrium Green's function method with density functional theory. This is currently implemented in the package SMEAGOL. The heart of SMEAGOL is our scheme for constructing the surface Green's functions describing the current-voltage probes. It consists of a direct summation of both open and closed scattering channels together with a regularization procedure of the Hamiltonian and provides great improvements over standard recursive methods. In particular it allows us to tackle material systems with complicated electronic structures, such as magnetic transition metals. Here we present a detailed description of SMEAGOL together with an extensive range of applications relevant for the two burgeoning fields of spin and molecular electronics.

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The hybrid halide perovskite CH3NH3PbI3 has enabled solar cells to reach an efficiency of about 20%, demonstrating a pace for improvements with no precedents in the solar energy arena. Despite such explosive progress, the microscopic origin behind the success of such material is still debated, with the role played by the organic cations in the light-harvesting process remaining unclear. Here van der Waals-corrected density functional theory calculations reveal that the orientation of the organic molecules plays a fundamental role in determining the material electronic properties. For instance, if CH3NH3 orients along a (011)-like direction, the PbI6 octahedral cage will distort and the bandgap will become indirect. Our results suggest that molecular rotations, with the consequent dynamical change of the band structure, might be at the origin of the slow carrier recombination and the superior conversion efficiency of CH3NH3PbI3.

Abstract:We have studied the dispersion and exfoliation of four inorganic layered compounds, WS 2 , We found that the dispersed concentration of each material falls exponentially with  as predicted by solution thermodynamics. This work shows that solution thermodynamics and specifically solubility parameter analysis can be used as a framework to understand the dispersion of 2-dimensional materials. Finally, we note that in good solvents such as 2 cyclohexylpyrrolidone, the dispersions are temporally stable with >90% of material remaining dispersed after 100 hours. ToC figOver the last decade, 2-dimensional nanomaterials have become one of the most studied subfields of nanoscience. These developments have been spearheaded by research into graphene, a material that is unique due to its combination of thermal, electronic, optical and mechanical properties. 1-5 However, over the last few years, it has become clear that a range of other inorganic layered compounds can be mechanically exfoliated in small quantities to give 2-dimensional nanosheets with interesting properties. 6-10 For example, exfoliated hexagonal boron nitride has been used as a dielectric support in graphene-based transistors 11 while MoS 2 has been fabricated into sensors 10, 12 , transistors 13-15 and integrated circuits. 16 The availability of a wide range of 2-dimensional materials is important as it allows access to a broad palette of physical and chemical properties. A good example is provided by the family of transition metal dichalcogenides (TMDs). These materials have the chemical composition MX 2 where M is a transition metal (commonly, but not limited to Ti, Nb, Ta, Mo, W) and X is a chalcogen (i.e. S, Se, Te). As in graphite, these atoms are covalently bonded into nanosheets which stack into 3-dimensional crystals by van der Waals interactions. These materials are of particular interest because, depending on the combination of metal and chalcogen, the material can be semiconducting or metallic. 17 In addition, the bandgap can vary from a few hundred meV to a few eV, 17 suggesting these materials have potential as versatile electronic device materials.Furthermore, these materials have interesting electrochemical properties which make them suitable for applications such as battery electrodes. 18,19 As with graphene, many applications will require relatively large quantities of material suggesting that a solution processing route is required. 20 A number of possibilities exist. For example, it has been known for many years that materials such as MoS 2 can be exfoliated by 3 lithium intercalation. 21 However, such a route tends to result in structural deformations in some TMDs leading to considerably altered electronic properties. 22 Alternatively, TMDs can be synthesised in the liquid phase. 7,8 Probably the simplest route to liquid exfoliation of layered compounds is sonication assisted exfoliation in solvents [23][24][25][26][27][28][29] or aqueous surfactant solutions. 19,[30][31][32] Here, sonication results in the exfoliation of the ...