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Solid-state batteries are considered the holy grail of next-generation battery technology, meeting the ever-increasing demand for energy storage that is affordable and safe, with high energy density and long cycle life. Materials and interfaces play a critical role for their eventual success and mass commercialization. This issue of MRS Bulletin focuses on the current state of the art of solid-state electrolytes and device architectures and provides a perspective into the various materials and interfacial challenges that limit its performance and stability.

Accurately identifying the local structural heterogeneity of complex, disordered amorphous materials such as amorphous silicon is crucial for accelerating technology development. However, short-range atomic ordering quantification and nanoscale spatial resolution over a large area on a-Si have remained major challenges and practically unexplored. We resolve phonon vibrational modes of a-Si at a lateral resolution of <60 nm by tip-enhanced Raman spectroscopy. To project the high dimensional TERS imaging to a two-dimensional manifold space and categorize amorphous silicon structure, we developed a multiresolution manifold learning algorithm. It allows for quantifying average Si-Si distortion angle and the strain free energy at nanoscale without a human-specified physical threshold. The multiresolution feature of the multiresolution manifold learning allows for distilling local defects of ultra-low abundance (< 0.3%), presenting a new Raman mode at finer resolution grids. This work promises a general paradigm of resolving nanoscale structural heterogeneity and updating domain knowledge for highly disordered materials. Short range atomic ordering quantification and nanoscale spatial resolution over a large area for amorphous materials is crucial for accelerating technology development but remain challenges. Here, the authors explore nanoscale heterogeneity of amorphous silicon by tip-enhanced Raman spectroscopy via multiresolution manifold learning.

Nanocrystal quantum dots have favourable light-emitting properties. They show photoluminescence with high quantum yields, and their emission colours depend on the nanocrystal size—owing to the quantum-confinement effect—and are therefore tunable. However, nanocrystals are difficult to use in optical amplification and lasing. Because of an almost exact balance between absorption and stimulated emission in nanoparticles excited with single electron–hole pairs (excitons), optical gain can only occur in nanocrystals that contain at least two excitons. A complication associated with this multiexcitonic nature of light amplification is fast optical-gain decay induced by non-radiative Auger recombination, a process in which one exciton recombines by transferring its energy to another. Here we demonstrate a practical approach for obtaining optical gain in the single-exciton regime that eliminates the problem of Auger decay. Specifically, we develop core/shell hetero-nanocrystals engineered in such a way as to spatially separate electrons and holes between the core and the shell (type-II heterostructures). The resulting imbalance between negative and positive charges produces a strong local electric field, which induces a giant (∼100 meV or greater) transient Stark shift of the absorption spectrum with respect to the luminescence line of singly excited nanocrystals. This effect breaks the exact balance between absorption and stimulated emission, and allows us to demonstrate optical amplification due to single excitons. Nanocrystals for lasers Semiconductor nanocrystals have very good light-emitting properties, so have potential as optical amplification media that can be easily processed with solution-based techniques: possible applications include optical interconnects in microelectronics, lab-on-a-chip technologies and quantum information processing. The problem with these structures is that at least two excitons (bound electron–hole pairs) need to be present in a nanocrystal before optical gain can be achieved, and this limits performance. In effect, the excitons annihilate each other before optical amplification can occur. This obstacle has now been overcome using nanocrystals with cores and shells made from different semiconductor materials, constructed in such a way that electrons and holes are separated from each other. This makes optical gain based on single excitons possible, significantly enhancing their promise as a practical optical material for laser applications. Semiconductor nanocrystals seem good candidates for 'soft' optical gain media, but optical gain and lasing is hard to achieve owing to a fundamental optical effect, which involves the problem that at least two excitons need to be present in a nanocrystal to achieve gain, and this limits performance. Here the problem is circumvented by designing nanocrystals with cores and shells made from different semiconductor materials, and in such a way that electrons and holes are separated from each other: this makes possible optical gain based on single excitons, thereby significantly enhancing the promise of semiconductor nanocrystals as practical optical materials for a wide range of lasing applications.

Plasmons in graphene 1 , 2 , 3 , 4 can be tuned by using electrostatic gating or chemical doping 5 , 6 , 7 , and the ability to confine plasmons in very small regions could have applications in optoelectronics 8 , 9 , plasmonics 10 , 11 and transformation optics 12 . However, little is known about how atomic-scale defects influence the plasmonic properties of graphene. Moreover, the smallest localized plasmon resonance observed in any material to date has been limited to around 10 nm (refs  13 , 14 , 15 ). Here, we show that surface plasmon resonances in graphene can be enhanced locally at the atomic scale. Using electron energy-loss spectrum imaging in an aberration-corrected scanning transmission electron microscope, we find that a single point defect can act as an atomic antenna in the petahertz (10 15  Hz) frequency range, leading to surface plasmon resonances at the subnanometre scale. A single point defect in graphene can act as an atomic antenna in the petahertz frequency range, leading to surface plasmon resonances at the subnanometre scale.

Electrolyte stability can be improved by incorporating complexing agents that bind key decomposition intermediates and slow down decomposition. We show that hexamethyl-phosphoramide (HMPA) extends both the thermal stability threshold of sodium hexafluorophosphate (NaPF6) in dimethoxyethane (DME) electrolyte and the cycle life of double-layer capacitors. HMPA forms a stable complex with PF5, an intermediate in PF6 anion thermal degradation. Unbound, this intermediate leads to autocatalytic degradation of the electrolyte solution. The results of electrochemical impedance spectroscopy (EIS) and galvanostatic cycling measurements show large changes in the cell without the presence of HMPA at higher temperatures (≥60 °C). Fourier transform infrared spectroscopy (FTIR) on the liquid and gas phase of the electrolyte shows without HMPA the formation of measurable amounts of PF5 and HF. The complimentary results of these measurements proved the usefulness of using Lewis bases such as HMPA to inhibit the degradation of the electrolyte solution at elevated temperatures and potentially lead to improve cycle life of a nonaqueous capacitor. The results showed a large increase in capacitance retention during cycling (72% retention after 750,000 cycles). The results also provide evidence of major decomposition processes (0% capacitance retention after 100,000 cycles) that take place at higher temperatures without the additive of a thermal stability additive such as HMPA.

Traditionally, lithium-ion battery cathodes face a trade-off between the energy density afforded by high-voltage anion reduction−oxidation and long-term stability. Now, incorporating polyanion motifs into a disordered oxide crystal structure is shown to stabilize the oxygen sublattice, improving capacity retention at high energy densities.

Traditionally, lithium-ion battery cathodes face a trade-off between the energy density afforded by high-voltage anion reduction−oxidation and long-term stability. Now, incorporating polyanion motifs into a disordered oxide crystal structure is shown to stabilize the oxygen sublattice, improving capacity retention at high energy densities.

Low negative electrode potential and high reactivity makes lithium (Li) ideal candidate for obtaining highest possible energy density among other materials. In this work we show a novel route with which the overall electrode potential could significantly be enhanced through selection of cluster size. Using first principles density functional theory and continuum dielectric model, we studied free energy and redox potential as well as investigated relative stability of Li n (n ≤ 8) clusters in both gas phase and solution. We found that Li 3 has the lowest negative redox potential (thereby highest overall electrode potential) suggesting that cluster based approach could provide a novel way of engineering the next generation battery technology. The microscopic origin of Li 3 cluster’s superior performance is related to two major factors: gas phase ionization and difference between solvation free energy for neutral and positive ion. Taken together, the present study provides insight into the engineering of redox potential in battery and could stimulate further work in this direction.

We present a new class of catalysts, InMo-ZSM-5, which can be prepared by indium impregnation of Mo-ZSM-5. The incorporation of indium dramatically decreases coke formation during methane dehydroaromatization. The benzene and C2 hydrocarbons selectivity among total hydrocarbons over InMo-ZSM-5 remains comparable to that of Mo-ZSM-5 despite reduced methane conversion due to decreased coke formation. We found 1 wt% indium to be optimal loading for reducing coke selectivity to half that of Mo-ZSM-5. Characterization methods were not helpful in discerning the interaction of In with Mo but experiments with bimetallic 1In2Mo-ZSM-5 and mechanical mixture 1In+2Mo-ZSM-5 suggest that In and Mo need to be in close proximity to suppress coke formation. This is supported by temperature programmed reduction experiments which show that In incorporation leads to lower Mo reduction temperature in In2Mo-ZMS-5. Graphical Abstract