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Abstract Spin-orbit coupling is an important ingredient to regulate the many-body physics, especially for many spin liquid candidate materials such as rare-earth magnets and Kitaev materials. The rare-earth chalcogenides Equation missing<#comment/>(Ch = O, S, Se) is a congenital frustrating system to exhibit the intrinsic landmark of spin liquid by eliminating both the site disorders between Equation missing<#comment/>and Equation missing<#comment/>ions with the big ionic size difference and the Dzyaloshinskii-Moriya interaction with the perfect triangular lattice of the Equation missing<#comment/>ions. The temperature versus magnetic-field phase diagram is established by the magnetization, specific heat, and neutron-scattering measurements. Notably, the neutron diffraction spectra and the magnetization curve might provide microscopic evidence for a series of spin configuration for in-plane fields, which include the disordered spin liquid state, 120° antiferromagnet, and one-half magnetization state. Furthermore, the ground state is suggested to be a gapless spin liquid from inelastic neutron scattering, and the magnetic field adjusts the spin orbit coupling. Therefore, the strong spin-orbit coupling in the frustrated quantum magnet substantially enriches low-energy spin physics. This rare-earth family could offer a good platform for exploring the quantum spin liquid ground state and quantum magnetic transitions. 

Sodium- and potassium-ion batteries are one of the most promising electrical energy storage devices at low cost, but their inferior rate and capacity have hampered broader applications such as electric vehicles and grids. Carbon nanomaterials have been demonstrated to have ultrafast surface-dominated ion uptake to drastically increase the rate and capacity, but trial-and-error approaches are usually used to find desired anode materials from numerous candidates. Here, we developed guiding principles to rationally screen pseudocapacitive anodes from numerous candidate carbon materials to create ultrafast Na- and K-ion batteries. The transition from pseudocapacitive to metal-battery mechanisms on heteroatom-doped graphene in charging process was revealed by the density functional theory methods. The results show that the graphene substrate can guide the preferential growth of K and Na along graphene plane, which inhibits dendrite development effectively in the batteries. An intrinsic descriptor is discovered to establish a volcano-shaped relationship that correlates the capacity with the intrinsic physical qualities of the doping structures, from which the best anode materials could be predicted. The predictions are in good agreement with the experimental results. The strategies for enhancing both the power and energy densities are proposed based on the predictions and experiments for the batteries. 

Abstract Graphene oxide (GO)‐based all‐solid‐state supercapacitors (GO‐A3Ss) are superior over liquid electrolyte‐based supercapacitors and capable of being integrated on a single chip in various geometry shapes for the use of future smart wearable electronics field as a fast energy storage device, but their capacitance need to be improved. Here, a new approach has been developed for enhancing the capacitive capability of the supercapacitors through molecular dynamics simulations with the first‐principle input. A theoretical model of charge storage is developed to understand the unique capacitive enhancement mechanism and to predict the capacitance of the GO‐A3Ss, which agrees well with the experimental observations. A novel supercapacitor with GO and reduced graphene oxide (rGO) alternatively layered structures is designed based on the model, and its energy density is the highest among conventional supercapacitors using liquid electrolytes and all‐solid‐state supercapacitors using aerogels or hydrogels as the solid‐state electrolyte. Based on the predictions, two new types of high‐performance GO/rGO multilayered capacitors are proposed to meet different practical applications. The results of this work provide an approach for the design of high‐performance all‐solid‐state supercapacitors based on GO and rGO materials. 

Abstract Although tremendous efforts have been devoted to understanding the origin of boosted charge storage on heteroatom‐doped carbons, none of the present studies has shown a whole landscape. Herein, by both experimental evidence and theoretical simulation, it is demonstrated that heteroatom doping not only results in a broadened operating voltage, but also successfully promotes the specific capacitance in aqueous supercapacitors. In particular, the electrolyte cations adsorbed on heteroatom‐doped carbon can effectively inhibit hydrogen evolution reaction, a key step of water decomposition during the charging process, which broadens the voltage window of aqueous electrolytes even beyond the thermodynamic limit of water (1.23 V). Furthermore, the reduced adsorption energy of heteroatom‐doped carbon consequently leads to more stored cations on the heteroatom‐doped carbon surface, thus yielding a boosted charge storage performance.