Threshold-switching devices based on amorphous chalcogenides are considered for use as selector devices in 3D crossbar memories. However, the fundamental understanding of amorphous chalcogenide is hindered owing to the complexity of the local structures and difficulties in the trap analysis of multinary compounds. Furthermore, after threshold switching, the local structures gradually evolve to more stable energy states owing to the unstable homopolar bonds. Herein, based on trap analysis, DFT simulations, and operando XPS analysis, it is determined that the threshold switching mechanism is deeply related to the charged state of Se-Se homopolar defects. A threshold switching device is demonstrated with an excellent performance through the modification of the local structure via the addition of alloying elements and investigating the time-dependent trap evolution. The results concerning the trap dynamics of local atomic structures in threshold switching phenomena may be used to improve the design of amorphous chalcogenides.
Durability of high-energy throughput batteries is a prerequisite for electric vehicles to penetrate the market. Despite remarkable progresses in silicon anodes with high energy densities, rapid capacity fading of full cells with silicon-graphite anodes limits their use. In this work, we unveil degradation mechanisms such as Li+ crosstalk between silicon and graphite, consequent Li+ accumulation in silicon, and capacity depression of graphite due to silicon expansion. The active material properties, i.e. silicon particle size and graphite hardness, are then modified based on these results to reduce Li+ accumulation in silicon and the subsequent degradation of the active materials in the anode. Finally, the cycling performance is tailored by designing electrodes to regulate Li+ crosstalk. The resultant full cell with an areal capacity of 6 mAh cm-2 has a cycle life of >750 cycles the volumetric energy density of 800 Wh L-1 in a commercial cell format.
In most solution-processed organic devices, a poly(3,4-ethylenedioxythiophene) (PEDOT) polymerized with poly(4-styrenesulfonate) (PSS) film is inevitably affected by various conditions during the subsequent solution-coating processes. To investigate the effects of direct solvent exposure on the properties of PEDOT polymerized with PSS (PEDOT:PSS) films, photoemission spectroscopy-based analytical methods were used before and after solvent-coating processes. Our results clearly indicate that PEDOT: PSS films undergo a different transition mechanism depending on the solubility of the solvent in water. The water-miscible solvents induce the solvation of hydrophilic PSS chains. As a result, this process allows the solvent to diffuse into the PEDOT: PSS film, and a conformational change between PEDOT and PSS occurs. On the other hand, the water-immiscible organic solvents cause the partial adsorption of solvent molecules at the PE surface, which leads to changes in the surface properties, including work function. Based on our finding, we demonstrate that the energy-level alignments at the organic semiconductor/electrode interface for the PEDOT: PSS films can be controlled by simple solvent treatments.
