Lithium metal is considered as the most prospective electrode for next‐generation energy storage systems due to high capacity and the lowest potential. However, uncontrollable spatial growth of lithium dendrites and the crack of solid electrolyte interphase still hinder its application. Herein, Schottky defects are motivated to tune the 4f‐center electronic structures of catalysts to provide active sites to accelerate Li transport kinetics. As experimentally and theoretically confirmed, the electronic density is redistributed and affected by the Schottky defects, offering numerous active catalytic centers with stronger ion diffusion capability to guide the horizontal lithium deposition against dendrite growth. Consequently, the Li electrode with artificial electronic‐modulation layer remarkably decreases the barriers of desolvation, nucleation, and diffusion, extends the dendrite‐free plating lifespan up to 1200 h, and improves reversible Coulombic efficiency. With a simultaneous catalytic effect on the conversions of sulfur species at the cathodic side, the integrated Li–S full battery exhibits superior rate performance of 653 mA h g −1 at 5 C, high long‐life capacity retention of 81.4% at 3 C, and a high energy density of 2264 W h kg −1 based on sulfur in a pouch cell, showing the promising potential toward high‐safety and long‐cycling lithium metal batteries.

Hydride ions (H-) have an appropriate size for fast transport, which makes the conduction of H- attractive. In this work, the H- transport properties of BaH2 have been investigated under pressure using in situ impedance spectroscopy measurements up to 11.2 GPa and density functional theoretical calculations. The H- transport properties, including ionic migration resistance, relaxation frequency, and relative permittivity, change significantly with pressure around 2.3 GPa, which can be attributed to the structural phase transition of BaH2. The ionic migration barrier energy of the P63/mmc phase decreases with pressure, which is responsible for the increased ionic conductivity. A huge dielectric constant at low frequencies is observed, which is related to the polarization of the H- dipoles. The current study establishes general guidelines for developing high-energy storage and conversion devices based on hydride ion transportation.

The self-trapped state (STS) of the interlayer exciton (IX) has aroused enormous interest owing to its significant impact on the fundamental properties of the van der Waals heterostructures (vdWHs). Nevertheless, the microscopic mechanisms of STS are still controversial. Herein, we study the corrections of the binding energies of the IXs stemming from the exciton−interface optical phonon coupling in four kinds of vdWHs and find that these IXs are in the STS for the appropriate ratio of the electron and hole effective masses. We show that these self-trapped IXs could be classified into type  with the increasing binding energy in the tens of millielectronvolts range, which are very agreement with the red-shift of the IX spectra in experiments, and type  with the decreasing binding energy, which provides a possible explanation for the blue-shift and broad line width of the IX's spectra at low temperatures. Moreover, these two types of exciton states could be transformed into each other by adjusting the structural parameters of vdWHs. These results not only provide an in-depth understanding for the self-trapped mechanism but also shed light on the modulations of IXs in vdWHs.

Further efficiency boost of organic-inorganic perovskite solar cells is hampered by limited knowledge on ion migration, inductive loops, and the relationship between structures and properties in organometal halide perovskites. In this work, in situ alternating current impedance spectroscopy measurements on CH(NH2)2PbBr3 (FAPbBr3) have been carried out under high pressure up to 4.8 GPa. The inductive loop has been discovered at low frequencies and can be tuned dramatically by applying pressure, which is attributed to large FA ion migration in FAPbBr3. Two discontinuous changes are observed in both ionic and electronic resistances around phase transition pressure. The pressure dependent photoresponse of FAPbBr3 has also been studied by in situ photocurrent measurements under high pressure up to 3.8 GPa. It indicates that the photocurrent of FAPbBr3 can be enhanced remarkably at 1.3 GPa and the largest photocurrent value in FAPbBr3 is nearly 10 times larger than that in CH3NH3PbBr3 and about 3 times larger than that in CH3NH3PbI3.