Computational predictions of energy materials using density functional theory

In the search for new functional materials, quantum mechanics is an exciting starting point. The fundamental laws that govern the behaviour of electrons have the possibility, at the other end of the scale, to predict the performance of a material for a targeted application. In some cases, this is achievable using density functional theory (DFT). In this Review, we highlight DFT studies predicting energy-related materials that were subsequently confirmed experimentally. The attributes and limitations of DFT for the computational design of materials for lithium-ion batteries, hydrogen production and storage materials, superconductors, photovoltaics and thermoelectric materials are discussed. In the future, we expect that the accuracy of DFT-based methods will continue to improve and that growth in computing power will enable millions of materials to be virtually screened for specific applications. Thus, these examples represent a first glimpse of what may become a routine and integral step in materials discovery

propnet: A Knowledge Graph for Materials Science

Discovering the ideal material for a new application involves determining its numerous properties, such as electronic, mechanical, or thermodynamic, to match those of its desired application. The rise of high-throughput computation has meant that large databases of material properties are now accessible to scientists. However, these databases contain far more information than might appear at first glance, since many relationships exist in the materials science literature to derive, or at least approximate, additional properties. propnet is a new computational framework designed to help scientists to automatically calculate additional information from their datasets. It does this by constructing a network graph of relationships between different materials properties and traversing this graph. Initially, propnet contains a catalog of over 100 property relationships but the hope is for this to expand significantly in the future, and contributions from the community are welcomed

Investigation of Solvent Type and Salt Addition in High Transference Number Nonaqueous Polyelectrolyte Solutions for Lithium Ion Batteries

High Li+ transference number electrolytes have attracted recent interest as a means to improve the energy density and rate capabilities of current lithium ion batteries. Here the viscosity and transport properties of a sulfonated polysulfone/poly(ethylene glycol) copolymer that displays both high transference number and high conductivity when dissolved in dimethyl sulfoxide (DMSO) are investigated for the first time in a battery-relevant solvent of nearly equivalent dielectric constant: mixed ethylene carbonate (EC)/dimethyl carbonate (DMC). The addition of a binary salt to each solution is investigated as a means to improve conductivity, and the diffusion coefficient of each species is tracked by pulse field gradient nuclear magnetic resonance (PFG-NMR). Through the 7Li NMR peak width and quantum chemistry calculations of the dissociation constant, it is shown that although the two solvent systems have nearly equivalent dielectric constants, the conductivity and transference number of the EC/DMC solutions are significantly lower as a result of poor dissociation of the sulfonate group on the polymer backbone. These results are the first study of polyelectrolyte properties in a battery-relevant solvent and clearly demonstrate the need to consider solvent properties other than the dielectric constant in the design of these electrolytes

Comparison of the tetrahedron method to smearing methods for the electronic density of states

The electronic density of states (DOS) highlights fundamental properties of materials that oftentimes dictate their properties, such as the band gap and Van Hove singularities. In this short note, we discuss how sharp features of the density of states can be obscured by smearing methods (such as the Gaussian and Fermi smearing methods) when calculating the DOS. While the common approach to reach a "converged" density of states of a material is to increase the discrete k-point mesh density, we show that the DOS calculated by smearing methods can appear to converge but not to the correct DOS. Employing the tetrahedron method for Brillouin zone integration resolves key features of the density of states far better than smearing methods

Universal Resistances of the Quantum RC circuit

We examine the concept of universal quantized resistance in the AC regime through the fully coherent quantum RC circuit comprising a cavity (dot) capacitively coupled to a gate and connected via a single spin-polarized channel to a reservoir lead. As a result of quantum effects such as the Coulomb interaction in the cavity and global phase coherence, we show that the charge relaxation resistance $R_q$ is identical for weak and large transmissions and it changes from $h/2e^2$ to $h/e^2$ when the frequency (times $\hbar$) exceeds the level spacing of the cavity; $h$ is the Planck constant and $e$ the electron charge. For large cavities, we formulate a correspondence between the charge relaxation resistance $h/e^2$ and the Korringa-Shiba relation of the Kondo model. Furthermore, we introduce a general class of models, for which the charge relaxation resistance is universal. Our results emphasize that the charge relaxation resistance is a key observable to understand the dynamics of strongly correlated systems.Comment: 12 pages, 3 figure

Additive-Free, Low-Temperature Crystallization of Stable α-FAPbI3 Perovskite

Formamidinium lead triiodide (FAPbI3) is attractive for photovoltaic devices due to its optimal bandgap at around 1.45 eV and improved thermal stability compared with methylammonium‐based perovskites. Crystallization of phase‐pure α‐FAPbI3 conventionally requires high‐temperature thermal annealing at 150 °C whilst the obtained α‐FAPbI3 is metastable at room temperature. Here, aerosol‐assisted crystallization (AAC) is reported, which converts yellow δ‐FAPbI3 into black α‐FAPbI3 at only 100 °C using precursor solutions containing only lead iodide and formamidinium iodide with no chemical additives. The obtained α‐FAPbI3 exhibits remarkably enhanced stability compared to the 150 °C annealed counterparts, in combination with improvements in film crystallinity and photoluminescence yield. Using X‐ray diffraction, X‐ray scattering, and density functional theory simulation, it is identified that relaxation of residual tensile strains, achieved through the lower annealing temperature and post‐crystallization crystal growth during AAC, is the key factor that facilitates the formation of phase‐stable α‐FAPbI3. This overcomes the strain‐induced lattice expansion that is known to cause the metastability of α‐FAPbI3. Accordingly, pure FAPbI3 p–i–n solar cells are reported, facilitated by the low‐temperature (≤100 °C) AAC processing, which demonstrates increases of both power conversion efficiency and operational stability compared to devices fabricated using 150 °C annealed films

Fine-root turnover rates of European forests revisited: an analysis of data from sequential coring and ingrowth cores

Background and Aims Forest trees directly contribute to carbon cycling in forest soils through the turnover of their fine roots. In this study we aimed to calculate root turnover rates of common European forest tree species and to compare them with most frequently published values. Methods We compiled available European data and applied various turnover rate calculation methods to the resulting database. We used Decision Matrix and Maximum-Minimum formula as suggested in the literature. Results Mean turnover rates obtained by the combination of sequential coring and Decision Matrix were 0.86 yr−1 for Fagus sylvatica and 0.88 yr−1 for Picea abies when maximum biomass data were used for the calculation, and 1.11 yr−1 for both species when mean biomass data were used. Using mean biomass rather than maximum resulted in about 30 % higher values of root turnover. Using the Decision Matrix to calculate turnover rate doubled the rates when compared to the Maximum-Minimum formula. The Decision Matrix, however, makes use of more input information than the Maximum-Minimum formula. Conclusions We propose that calculations using the Decision Matrix with mean biomass give the most reliable estimates of root turnover rates in European forests and should preferentially be used in models and C reporting

Joint disorder; a contributory cause to reproductive failure in beef bulls?

The lame sire, unsound for breeding, can cause substantial economic loss due to reduced pregnancies in the beef-producing herd

Arid1b haploinsufficient mice reveal neuropsychiatric phenotypes and reversible causes of growth impairment.

Sequencing studies have implicated haploinsufficiency of ARID1B, a SWI/SNF chromatin-remodeling subunit, in short stature (Yu et al., 2015), autism spectrum disorder (O'Roak et al., 2012), intellectual disability (Deciphering Developmental Disorders Study, 2015), and corpus callosum agenesis (Halgren et al., 2012). In addition, ARID1B is the most common cause of Coffin-Siris syndrome, a developmental delay syndrome characterized by some of the above abnormalities (Santen et al., 2012; Tsurusaki et al., 2012; Wieczorek et al., 2013). We generated Arid1b heterozygous mice, which showed social behavior impairment, altered vocalization, anxiety-like behavior, neuroanatomical abnormalities, and growth impairment. In the brain, Arid1b haploinsufficiency resulted in changes in the expression of SWI/SNF-regulated genes implicated in neuropsychiatric disorders. A focus on reversible mechanisms identified Insulin-like growth factor (IGF1) deficiency with inadequate compensation by Growth hormone-releasing hormone (GHRH) and Growth hormone (GH), underappreciated findings in ARID1B patients. Therapeutically, GH supplementation was able to correct growth retardation and muscle weakness. This model functionally validates the involvement of ARID1B in human disorders, and allows mechanistic dissection of neurodevelopmental diseases linked to chromatin-remodeling