Scientists are searching for the goal-directed methods to synthesize graphene nanoribbons (GNRs) with a particular edge type and width, which determines their electronic transport properties. A series of Li zigzag GNRs (ZGNRs) with different widths were predicted under high pressure with a stoichiometric ratio of Lin+1C2n, which indicates a route to prepare ultranarrow GNRs. Here, with thermodynamics and ab initio Gibbs free-energy calculations by quasi-harmonic approximation, we investigated the phase stabilities of the Li GNR compounds under high pressure and high temperature. We have also identified Li graphenide LiC2 (n =infinity) and Li polyacenide Li3C4 (n = 2) experimentally at the predicted pressure and temperature conditions using in situ X-ray diffraction, which can be recognized as the two end members of Lin+1C2n, with the widest and narrowest ZGNR structures. High temperature and the temperature gradient increased the degree of polymerization and facilitated the formation of wider GNR or carbon slices. This suggests that by controlling temperature and pressure, we may get ultranarrow Li ZGNRs composed of a limited number of parallel carbon chains, such as 3- or 4-zigzag GNR, which is ready to be protonated or functionalized to form atomically ordered ZGNRs.

Knowledge of the structure and properties of silicate magma under extreme pressure plays an important role in understanding the nature and evolution of Earth's deep interior. Here we report the structure of MgSiO3 glass, considered an analog of silicate melts, up to 111 GPa. The first (r1) and second (r2) neighbor distances in the pair distribution function change rapidly, with r1 increasing and r2 decreasing with pressure. At 53-62 GPa, the observed r1 and r2 distances are similar to the Si-O and Si-Si distances, respectively, of crystalline MgSiO3 akimotoite with edge-sharing SiO6 structural motifs. Above 62 GPa, r1 decreases, and r2 remains constant, with increasing pressure until 88 GPa. Above this pressure, r1 remains more or less constant, and r2 begins decreasing again. These observations suggest an ultrahigh-pressure structural change around 88 GPa. The structure above 88 GPa is interpreted as having the closest edge-shared SiO6 structural motifs similar to those of the crystalline postperovskite, with densely packed oxygen atoms. The pressure of the structural change is broadly consistent with or slightly lower than that of the bridgmanite-to-postperovskite transition in crystalline MgSiO3. These results suggest that a structural change may occur in MgSiO3 melt under pressure conditions corresponding to the deep lower mantle.

To study systems-level properties of the cell, it is necessary to go beyond individual regulators and target genes to study the regulatory network among transcription factors (TFs). However, it is difficult to directly dissect the TFs mediated genome-wide gene regulatory network (GRN) by experiment. Here, we proposed a hierarchical graphical model to estimate TF activity from mRNA expression by building TF complexes with protein cofactors and inferring TF's downstream regulatory network simultaneously. Then we applied our model on flower development and circadian rhythm processes in Arabidopsis thaliana. The computational results show that the sequence specific bHLH family TF HFR1 recruits the chromatin regulator HAC1 to flower development master regulator TF AG and further activates AG's expression by histone acetylation. Both independent data and experimental results supported this discovery. We also found a flower tissue specific H3K27ac ChIP-seq peak at AG gene body and a HFR1 motif in the center of this H3K27ac peak. Furthermore, we verified that HFR1 physically interacts with HAC1 by yeast two-hybrid experiment. This HFR1-HAC1-AG triplet relationship may imply that flower development and circadian rhythm are bridged by epigenetic regulation and enrich the classical ABC model in flower development. In addition, our TF activity network can serve as a general method to elucidate molecular mechanisms on other complex biological regulatory processes.

Multicomponent alloying has displayed extraordinary potential for producing exceptional structural and functional materials. However, the synthesis of single-phase, multi-principal covalent compounds remains a challenge. Here, we present a diffusion-controlled alloying strategy for the realization of covalent multi-principal transition metal carbides (MPTMCs) with a single face-centered cubic phase. The increased interfacial diffusion promoted by the addition of a nonstoichiometric compound leads to rapid formation of the single phase at much lower sintering temperature. Direct atomic-level observations via scanning transmission electron microscopy demonstrate that MPTMCs are composed of a single phase with a random distribution of all cations, which holds the key to the unique combinations of improved fracture toughness, superior Vickers hardness, and extremely lower thermal diffusivity achieved in MPTMCs. The present discovery provides a promising approach toward the design and synthesis of next-generation high-performance materials. Published under license by AIP Publishing.

Heterogeneity in Earth's mantle is a record of chemical and dynamic processes over Earth's history. The geophysical signatures of heterogeneity can only be interpreted with quantitative constraints on effects of major elements such as iron on physical properties including density, compressibility, and electrical conductivity. However, deconvolution of the effects of multiple valence and spin states of iron in bridgmanite (Bdg), the most abundant mineral in the lower mantle, has been challenging. Here we show through a study of a ferric-iron-only (Mg0.46Fe0.533+)(Si0.49Fe0.513+)O-3 Bdg that Fe3+ in the octahedral site undergoes a spin transition between 43 and 53 GPa at 300 K. The resolved effects of the spin transition on density, bulk sound velocity, and electrical conductivity are smaller than previous estimations, consistent with the smooth depth profiles from geophysical observations. For likely mantle compositions, the valence state of iron has minor effects on density and sound velocities relative to major cation composition.

The discovery of iron-based superconductors (FeSCs), with the highest transition temperature (T-c) up to 55 K, has attracted worldwide research efforts over the past ten years. So far, all these FeSCs structurally adopt FeSe-type layers with a square iron lattice and superconductivity can be generated by either chemical doping or external pressure. Herein, we report the observation of superconductivity in an iron-based honeycomb lattice via pressure-driven spin-crossover. Under compression, the layered FePX3 (X = S, Se) simultaneously undergo large in-plane lattice collapses, abrupt spin-crossovers, and insulator-metal transitions. Superconductivity emerges in FePSe3 along with the structural transition and vanishing of magnetic moment with a starting T-c similar to 2.5 K at 9.0 GPa and the maximum T-c similar to 5.5 K around 30 GPa. The discovery of superconductivity in iron-based honeycomb lattice provides a demonstration for the pursuit of transition-metal-based superconductors via pressure-driven spin-crossover.

Searching for excellent polyanionic cathode materials for Na-ion batteries attract considerable attention in recent years. Herein, a new polyanionic cathode candidate Na0.48Mn1.22PO4, crystallizing in the space group R-3 with the unit cell parameters of a = 15.3672 (17) angstrom, c = 43.503 (5) angstrom and V = 8896.91 (2) angstrom(3), belonging to the Fillowite-type structure, is reported for the first time. In the structure of Na0.48Mn1.22PO4, the Mn-O connectivity exhibits three-dimensional Mn-O-Mn network. More interestingly, some Mn5O6 clusters embed in the network. Electrochemical tests revealed that Na0.48Mn1.22PO4 can be very effectively cycled against a Na metal electrode with an average voltage of 3.35 V. In addition, The XANES and magnetic tests were also employed for the characterization of the material. (C) 2017 Elsevier B.V. All rights reserved.

Global terrestrial nitrogen (N) and phosphorus (P) cycles are coupled to the global carbon (C) cycle for net primary production (NPP), plant C allocation, and decomposition of soil organic matter, but N and P have distinct pathways of inputs and losses. Current C-nutrient models exhibit large uncertainties in their estimates of pool sizes, fluxes, and turnover rates of nutrients, due to a lack of consistent global data for evaluating the models. In this study, we present a new model-data fusion framework called the Global Observation-based Land-ecosystems Utilization Model of Carbon, Nitrogen and Phosphorus (GOLUM-CNP) that combines the CARbon DAta MOdel fraMework (CAR-AMOM) data-constrained C-cycle analysis with spatially explicit data-driven estimates of N and P inputs and losses and with observed stoichiometric ratios. We calculated the steady-state N- and P-pool sizes and fluxes globally for large biomes. Our study showed that new N inputs from biological fixation and deposition supplied >20% of total plant uptake in most forest ecosystems but accounted for smaller fractions in boreal forests and grasslands. New P inputs from atmospheric deposition and rock weathering supplied a much smaller fraction of total plant uptake than new N inputs, indicating the importance of internal P recycling within ecosystems to support plant growth. Nutrient-use efficiency, defined as the ratio of gross primary production (GPP) to plant nutrient uptake, were diagnosed from our model results and compared between biomes. Tropical forests had the lowest N-use efficiency and the highest P-use efficiency of the forest biomes. An analysis of sensitivity and uncertainty indicated that the NPP-allocation fractions to leaves, roots, and wood contributed the most to the uncertainties in the estimates of nutrient-use efficiencies. Correcting for biases in NPP-allocation fractions produced more plausible gradients of N- and P-use efficiencies from tropical to boreal ecosystems and highlighted the critical role of accurate measurements of C allocation for understanding the N and P cycles.

Exploration beyond the known phase space of thermodynamically stable compounds into the realm of metastable materials is a frontier of materials chemistry. The application of high pressure in experiment and theory provides a powerful vector by which to explore this uncharted phase space, allowing discovery of complex new structures and bonding in the solid state. We harnessed this approach for the Cu-Bi system, where the realization of new phases offers potential for exotic properties such as superconductivity. This potential is due to the presence of bismuth, which, by virtue of its status as one of the heaviest stable elements, forms a critical component in emergent materials such as superconductors and topological insulators. To fully investigate and understand the Cu-Bi system, we welded theoretical predictions with experiment to probe the Cu-Bi system under high pressures. By employing the powerful approach of in situ X-ray diffraction in a laser-heated diamond anvil cell (LHDAC), we thoroughly explored the high-pressure and high temperature (high-PT) phase space to gain insight into the formation of intermetallic compounds at these conditions. We employed density functional theory (DFT) calculations to calculate a pressure versus temperature phase diagram, which correctly predicts that CuBi is stabilized at lower pressures than Cu11Bi7, and allows us to uncover the thermodynamic contributions responsible for the stability of each phase. Detailed comparisons between the NiAs structure type and the two high-pressure Cu-Bi phases, Cu11Bi7 and CuBi, reveal the preference for elemental segregation within the Cu-Bi phases, and highlight the unique channels and layers formed by ordered Cu vacancies. The electron localization function from DFT calculations account for the presence of these "voids" as a manifestation of the lone pair orientation on the Bi atoms. Our study demonstrates the power of joint experimental computational work in exploring the chemistry occurring at high-PT conditions. The existence of multiple high-pressure-stabilized phases in the Cu Bi binary system, which can be readily identified with in situ techniques, offers promise for other systems in which no ambient pressure phases are known to exist.

We present a multi-messenger measurement of the Hubble constant H-0 using the binary-black-hole merger GW170814 as a standard siren, combined with a photometric redshift catalog from the Dark Energy Survey (DES). The luminosity distance is obtained from the gravitational wave signal detected by the Laser Interferometer Gravitational-Wave Observatory (LIGO)/Virgo Collaboration (LVC) on 2017 August 14, and the redshift information is provided by the DES Year 3 data. Black hole mergers such as GW170814 are expected to lack bright electromagnetic emission to uniquely identify their host galaxies and build an object-by-object Hubble diagram. However, they are suitable for a statistical measurement, provided that a galaxy catalog of adequate depth and redshift completion is available. Here we present the first Hubble parameter measurement using a black hole merger. Our analysis results in H-0 = 75(-32)(+40) km s(-1) Mpc(-1) , which is consistent with both SN Ia and cosmic microwave background measurements of the Hubble constant. The quoted 68% credible region comprises 60% of the uniform prior range [20, 140] km s(-1) Mpc(-1) , and it depends on the assumed prior range. If we take a broader prior of [10, 220] km s(-1) Mpc(-1) , we find H-0 = 78(-24)(+96) km s(-1) Mpc(-1) (57% of the prior range). Although a weak constraint on the Hubble constant from a single event is expected using the dark siren method, a multifold increase in the LVC event rate is anticipated in the coming years and combinations of many sirens will lead to improved constraints on H-0.