The linear-scaling divide-and-conquer (DC) quantum chemical methodology is applied to the density-functional tight-binding (DFTB) theory to develop a massively parallel program that achieves on-the-fly molecular reaction dynamics simulations of huge systems from scratch. The functions to perform large scale geometry optimization and molecular dynamics with DC-DFTB potential energy surface are implemented to the program called DC-DFTB-K. A novel interpolation-based algorithm is developed for parallelizing the determination of the Fermi level in the DC method. The performance of the DC-DFTB-K program is assessed using a laboratory computer and the K computer. Numerical tests show the high efficiency of the DC-DFTB-K program, a single-point energy gradient calculation of a one-million-atom system is completed within 60 s using 7290 nodes of the K computer. © 2016 Wiley Periodicals, Inc.

Aqueous Na‐ or K‐ion batteries could virtually eliminate the safety and cost concerns raised from Li‐ion batteries, but their widespread applications have generally suffered from narrow electrochemical potential window (ca. 1.23 V) of aqueous electrolytes that leads to low energy density. Herein, by exploring optimized eutectic systems of Na and K salts with asymmetric imide anions, we discovered, for the first time, room‐temperature hydrate melts for Na and K systems, which are the second and third alkali metal hydrate melts reported since the first discovery of Li hydrate melt by our group in 2016. The newly discovered Na‐ and K‐ hydrate melts could significantly extend the potential window up to 2.7 and 2.5 V (at Pt electrode), respectively, owing to the merit that almost all water molecules participate in the Na+ or K+ hydration shells. As a proof‐of‐concept, a prototype Na3V2(PO4)2F3|NaTi2(PO4)3 aqueous Na‐ion full‐cell with the Na‐hydrate‐melt electrolyte delivers an average discharge voltage of 1.75 V, that is among the highest value ever reported for all aqueous Na‐ion batteries.

Carbon nanotubes have long been described as rolled-up graphene sheets. It is only fairly recently observed that longitudinal cleavage of carbon nanotubes, using chemical, catalytical and electrical approaches, unzips them into thin graphene strips of various widths, the so-called graphene nanoribbons. In contrast, rolling up these flimsy ribbons into tubes in a real experiment has not been possible. Theoretical studies conducted by Kit et al. recently demonstrated the tube formation through twisting of graphene nanoribbon, an idea very different from the rolling-up postulation. Here we report the first experimental evidence of a thermally induced self-intertwining of graphene nanoribbons for the preferential synthesis of (7, 2) and (8, 1) tubes within parent-tube templates. Through the tailoring of ribbon’s width and edge, the present finding adds a radically new aspect to the understanding of carbon nanotube formation, shedding much light on not only the future chirality tuning, but also contemporary nanomaterials engineering.