Surface-Confined Disordered Hydrogen Bonds Enable Efficient Lithium Transport in All-Solid-State PEO-Based Lithium Battery.

Polyethylene oxide (PEO)-based electrolytes are essential to advance all-solid-state lithium batteries (ASSLBs) with high safety/energy density due to their inherent flexibility and scalability. However, the inefficient Li+ transport in PEO often leads to poor rate performance and diminished stability of the ASSLBs. The regulation of intermolecular H-bonds is regarded as one of the most effective approaches to enable efficient Li+ transport, while the practical performances are hindered by the electrochemical instability of free H-bond donors and the constrained mobility of highly ordered H-bonding structures.

Emulating "Curvature-Enhanced Adsorbate Coverage" for Superconformal and Orientated Zn Electrodeposition in Zinc-ion-Batteries.

Uneven Zn deposition and unfavorable side reactions have prevented the reversibility of the Zn anode. Herein, we design a rearranged (002) textured Zn anode inspired by a traditional curvature-enhanced adsorbate coverage (CEAC) process to realize the highly reversible Zn anode. The rearranged (002) textured structure directs superconformal Zn deposition by controlling the spatial deposition rate of the rearranged crystal planes, thereby promoting bottom-up "superfilling" of the 3D Zn skeletons.

Physics of band-filling correction in defect calculations of solid-state materials.

In solid-state physics/chemistry, a precise understanding of defect formation and its impact on the electronic properties of wide-bandgap insulators is a cornerstone of modern semiconductor technology. However, complexities arise in the electronic structure theory of defect formation when the latter triggers partial occupation of the conduction/valence band, necessitating accurate post-process correction to the energy calculations. Herein, we dissect these complexities, focusing specifically on the post-process band-filling corrections, a crucial element that often demands thorough treatment in defect formation studies.

New Emerging Fast Charging Microscale Electrode Materials.

Fast charging lithium (Li)-ion batteries are intensively pursued for next-generation energy storage devices, whose electrochemical performance is largely determined by their constituent electrode materials. While nanosizing of electrode materials enhances high-rate capability in academic research, it presents practical limitations like volumetric packing density and high synthetic cost. As an alternative to nanosizing, microscale electrode materials cannot only effectively overcome the limitations of the nanosizing strategy but also satisfy the requirement of fast-charging batteries.

van der Waals induced ice growth on partially melted ice nuclei in mist and fog.

Ice nucleation and formation play pivotal roles across various domains, from environmental science to food engineering. However, the exact ice formation mechanisms remain incompletely understood. This study introduces a novel ice formation process, which can be either heterogeneous or homogeneous, depending on the initial conditions.

Different pathways to anomalous stabilization of ice layers on methane hydrates.

We explore the Casimir-Lifshitz free-energy theory for surface freezing of methane gas hydrates near the freezing point of water. The theory enables us to explore different pathways, resulting in anomalous (stabilizing) ice layers on methane hydrate surfaces via energy minimization. Notably, we will contrast the gas hydrate material properties, under which thin ice films can form in water vapor, with those previously predicted to be required in the presence of liquid water.

Noble Gas Functional Defect with Unusual Relaxation Pattern in Solids.

The conventional understanding has always been that noble gases are chemically inert and do not affect materials properties. This belief has led to their use as a standard reference in various experimental applications through noble gas implantation. However, in our research, using first-principles calculations, we delve into the effects of noble gas defects on the properties of several functional oxides, thereby questioning this long-held assumption.

Spontaneous off-stoichiometry as the knob to control the dielectric properties of gapped metals.

Using first-principles calculations and LaTe as an example of an n-type gapped metal, we demonstrate that gapped metals can develop spontaneous defect formation resulting in off-stoichiometric compounds. Importantly, these compounds have different free carrier concentrations and can be realized by optimizing the synthesis conditions. The ability to tune the free carrier concentration allows the tailoring of the intraband and interband transitions, thus controlling the optoelectronic properties of materials in general.

Effect of pressure on the electronic structure of antiferromagnetic and paramagnetic YNiO: the role of disproportionation.

The dependence of electronic properties of quantum materials on external controls (, pressure and temperature) is one of the fundamentals of neuromorphic computing, sensors, Until recently, it has been believed that the theoretical description of such compounds cannot be accomplished using "traditional" density functional theory, and more advanced methods like dynamic mean-field theory should be utilized instead. Focusing here on the example of long-range ordered antiferromagnetic and paramagnetic YNiO phases, we show the interplay between spin and structural motifs under pressure and their impact on electronic properties. We successfully describe the insulating nature of both YNiO phases and the role of symmetry-breaking motifs in the band gap opening.

Fermi-Level Instability as a Way to Tailor the Properties of LaTe.

Traditionally, the formation of off-stoichiometric compounds is believed to be the growth effect rather than the intrinsic tendency of the system. However, here, using the example of LaTe, we demonstrate that in n-type gapped metals having a large internal gap between principal band edges and the Fermi level inside of the principal conduction band, Fermi-level instability can develop, resulting in a decrease in the formation energy for acceptor defects. Specifically, La vacancies in LaTe form spontaneously to produce the acceptor states and remove a fraction of free carriers from the principal conduction band via electron-hole recombination.

Chemistry of Oxygen Ionosorption on SnO Surfaces.

Ionosorbed oxygen is the key player in reactions on metal-oxide surfaces. This is particularly evident for chemiresistive gas sensors, which operate by modulating the conductivity of active materials through the formation/removal of surface O-related acceptors. Strikingly though, the exact type of species behind the sensing response remains obscure even for the most common material systems.

Deep Cycling for High-Capacity Li-Ion Batteries.

As the practical capacity of conventional Li-ion batteries (LIBs) approaches the theoretical limit, which is determined by the rocking-chair cycling architecture, a new cycling architecture with higher capacity is highly demanded for future development and electronic applications. Here, a deep-cycling architecture intrinsically with a higher theoretical capacity limit than conventional rocking-chair cycling architecture is developed, by introducing a follow-up cycling process to contribute more capacity. The deep-cycling architecture makes full use of movable ions in both of the electrolyte and electrodes for energy storage, rather than in either the electrolyte or the electrodes.

Direct coherent multi-ink printing of fabric supercapacitors.

Coaxial fiber-shaped supercapacitors with short charge carrier diffusion paths are highly desirable as high-performance energy storage devices for wearable electronics. However, the traditional approaches based on the multistep fabrication processes for constructing the fiber-shaped energy device still encounter persistent restrictions in fabrication procedure, scalability, and mechanical durability. To overcome this critical challenge, an all-in-one coaxial fiber-shaped asymmetric supercapacitor (FASC) device is realized by a direct coherent multi-ink writing three-dimensional printing technology via designing the internal structure of the coaxial needles and regulating the rheological property and the feed rates of the multi-ink.

Understanding Doping of Quantum Materials.

Doping mobile carriers into ordinary semiconductors such as Si, GaAs, and ZnO was the enabling step in the electronic and optoelectronic revolutions. The recent emergence of a class of "quantum materials", where uniquely quantum interactions between the components produce specific behaviors such as topological insulation, unusual magnetism, superconductivity, spin-orbit-induced and magnetically induced spin splitting, polaron formation, and transparency of electrical conductors, pointed attention to a range of doping-related phenomena associated with chemical classes that differ from the traditional semiconductors. These include wide-gap oxides, compounds containing open-shell d electrons, and compounds made of heavy elements yet having significant band gaps.

Mechanically Reinforced Localized Structure Design to Stabilize Solid-Electrolyte Interface of the Composited Electrode of Si Nanoparticles and TiO Nanotubes.

Silicon anode with extremely high theoretical specific capacity (≈4200 mAh g ), experiences huge volume changes during Li-ion insertion and extraction, causing mechanical fracture of Si particles and the growth of a solid-electrolyte interface (SEI), which results in a rapid capacity fading of Si electrodes. Herein, a mechanically reinforced localized structure is designed for carbon-coated Si nanoparticles (C@Si) via elongated TiO nanotubes networks toward stabilizing Si electrode via alleviating mechanical strain and stabilizing the SEI layer. Benefited from the rational localized structure design, the carbon-coated Si nanoparticles/TiO nanotubes composited electrode (C@Si/TiNT) exhibits an ideal electrode thickness swelling, which is lower than 1% after the first cycle and increases to about 6.

Elementary models of the "flux driven anti-ripening" during nanobelt growth.

A stirring solution hydrothermal approach is widely used to rationally grow elongated oxide nanostructures with controllable aspect ratios. Depending on the synthesis conditions, the following are observed: (i) no nanostructure formation (the system exists as a pure liquid), (ii) formation of nanostructure starting from a critical powder/initial volume of the liquid solution, and (iii) monotonic increase in the nanostructure's aspect ratio (towards asymptotic value) with stirring rate. Despite these experimental observations, the theoretical understanding of the process is limited.

Energy, Phonon, and Dynamic Stability Criteria of Two-Dimensional Materials.

First-principles calculations have become a powerful tool to exclude the Edisonian approach in search of novel two-dimensional (2D) materials. However, no universal first-principles criteria to examine the realizability of hypothetical 2D materials have been established in the literature yet. Because of this, and as the calculations are always performed in an artificial simulation environment, one can unintentionally study compounds that do not exist in experiments.

Identifying the Origin and Contribution of Surface Storage in TiO (B) Nanotube Electrode by In Situ Dynamic Valence State Monitoring.

Fundamental insight into the surface charging mechanism of TiO (B) nanomaterials is limited due to the complicated nature of lithiation behavior, as well as the limitations of available characterization tools that can directly probe surface charging process. Here, an in situ approach is reported to monitor the dynamic valence state of TiO (B) nanotube electrodes, which utilizes in situ X-ray absorption spectroscopy (XAS) to identify the origin and contribution of surface storage. A real-time correlation is elucidated between the rate-dependent electrode performance and dynamic Ti valence-state change.

Suppression of surfaces states at cubic perovskite (001) surfaces by CO adsorption.

By using first-principles approach, the interaction of CO2 with (001) surfaces of six cubic ABO3 perovskites (A = Ba, Sr and B = Ti, Zr, Hf) is studied in detail. We show that CO2 adsorption results in the formation of highly stable CO3-like complexes with similar geometries for all investigated compounds. This reaction leads to the suppression of the surfaces states, opening the band gaps of the slab systems up to the corresponding bulk energy limits.

Distance-Dependent Sign Reversal in the Casimir-Lifshitz Torque.

The Casimir-Lifshitz torque between two biaxially polarizable anisotropic planar slabs is shown to exhibit a nontrivial sign reversal in its rotational sense. The critical distance a_{c} between the slabs that marks this reversal is characterized by the frequency ω_{c}∼c/2a_{c} at which the in-planar polarizabilities along the two principal axes are equal. The two materials seek to align their principal axes of polarizabilities in one direction below a_{c}, while above a_{c} their axes try to align rotated perpendicular relative to their previous minimum energy orientation.

Tailoring electronic properties of multilayer phosphorene by siliconization.

Controlling the thickness dependence of electronic properties for two-dimensional (2d) materials is among the primary goals for their large-scale applications. Herein, employing a first-principles computational approach, we predict that Si interaction with multilayer phosphorene (2d-P) can result in the formation of highly stable 2d-SiP and 2d-SiP compounds with a weak interlayer interaction. Our analysis demonstrates that these systems are semiconductors with band gap energies that can be governed by varying the thicknesses and stacking arrangements.

Reducing the Charge Carrier Transport Barrier in Functionally Layer-Graded Electrodes.

Lithium-ion batteries (LIBs) are primary energy storage devices to power consumer electronics and electric vehicles, but their capacity is dramatically decreased at ultrahigh charging/discharging rates. This mainly originates from a high Li-ion/electron transport barrier within a traditional electrode, resulting in reaction polarization issues. To address this limitation, a functionally layer-graded electrode was designed and fabricated to decrease the charge carrier transport barrier within the electrode.

Water-Soluble Sericin Protein Enabling Stable Solid-Electrolyte Interphase for Fast Charging High Voltage Battery Electrode.

Spinel LiNi Mn O (LNMO) is the most promising cathode material for achieving high energy density lithium-ion batteries attributed to its high operating voltage (≈4.75 V). However, at such high voltage, the commonly used battery electrolyte is suffered from severe oxidation, forming unstable solid-electrolyte interphase (SEI) layers.

Band gap modulation of SrTiO upon CO adsorption.

Herein, CO chemisorption on SrTiO(001) surfaces is studied using ab initio calculations to establish new chemical sensing mechanisms. It was found that CO adsorption opens the band gap of the material. However, the mechanisms are different: the CO adsorption on the TiO-terminated surface neutralizes the surface states at the valence band (VB) maximum, whereas for the SrO-terminated surface it suppresses the conduction band (CB) minimum.

Stability and electronic properties of phosphorene oxides: from 0-dimensional to amorphous 2-dimensional structures.

Combining the screening by first-principles calculations and Born-Oppenheimer molecular dynamics simulations, we fully reconsider phosphorene oxidation and the formation of low-dimensional phosphorus oxides (PO). It is found that the previously reported 2-dimensional PO (2d-PO) structures cannot provide a full understanding of 2d-PO properties. We show that the P-O interaction can result in highly stable 0d-PO and 2d-PO structures with close energetics, but a noticeable difference in band-gap energies.