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  • Mesophase Formation Stabilizes High-purity Magic-sized Clusters

    Nevers, Douglas R.; Williamson, Curtis B.; Savitzky, Benjamin H; Hadar, Ido; Banin, Uri; Kourkoutis, Lena F.; Hanrath, Tobias; Robinson, Richard D. (American Chemical Society (ACS), 2018-01-27)
    Magic-sized clusters (MSCs) are renowned for their identical size and closed-shell stability that inhibit conventional nanoparticle (NP) growth processes. Though MSCs have been of increasing interest, understanding the reaction pathways toward their nucleation and stabilization is an outstanding issue. In this work, we demonstrate that high concentration synthesis (1000 mM) promotes a well-defined reaction pathway to form high-purity MSCs (>99.9%). The MSCs are resistant to typical growth and dissolution processes. Based on insights from in-situ X-ray scattering analysis, we attribute this stability to the accompanying production of a large, hexagonal organic-inorganic mesophase (>100 nm grain size) that arrests growth of the MSCs and prevents NP growth. At intermediate concentrations (500 mM), the MSC mesophase forms, but is unstable, resulting in NP growth at the expense of the assemblies. These results provide an alternate explanation for the high stability of MSCs. Whereas the conventional mantra has been that the stability of MSCs derives from the precise arrangement of the inorganic structures (i.e., closed-shell atomic packing), we demonstrate that anisotropic clusters can also be stabilized by self-forming fibrous mesophase assemblies. At lower concentration (<200 mM or >16 acid-to-metal), MSCs are further destabilized and NPs formation dominates that of MSCs. Overall, the high concentration approach intensifies and showcases inherent concentration-dependent surfactant phase behavior that is not accessible in conventional (i.e., dilute) conditions. This work provides not only a robust method to synthesize, stabilize, and study identical MSC products, but also uncovers an underappreciated stabilizing interaction between surfactants and clusters.
  • Parity-Time Symmetric Photonics

    Zhao, Han; Feng, Liang (Oxford University Press (OUP), 2018-01-17)
    The establishment of non-Hermitian quantum mechanics (such as parity-time (PT) symmetry) stimulates a paradigmatic shift for studying symmetries of complex potentials. Owing to the convenient manipulation of optical gain and loss in analogy to the complex quantum potentials, photonics provides an ideal platform for visualization of many conceptually striking predictions from the non-Hermitian quantum theory. A rapidly developing field has emerged, namely, PT symmetric photonics, demonstrating intriguing optical phenomena including eigenstate coalescence and spontaneous PT symmetry breaking. The advance of quantum physics, as the feedback, provides photonics with brand-new paradigms to explore the entire complex permittivity plane for novel optical functionalities. Here, we review recent exciting breakthroughs in PT symmetric photonics while systematically presenting their underlying principles guided by non-Hermitian symmetries. The potential device applications for optical communication and computing, bio-chemical sensing, and healthcare are also discussed.
  • Dual Phase Change Thermal Diodes for Enhanced Rectification Ratios: Theory and Experiment

    Cottrill, Anton L.; Wang, Song; Liu, Albert Tianxiang; Wang, Wen-Jun; Strano, Michael S. (Wiley-Blackwell, 2018-01-15)
    Thermal diodes are materials that allow for the preferential directional transport of heat and are highly promising devices for energy conservation, energy harvesting, and information processing applications. One form of a thermal diode consists of the junction between a phase change and phase invariant material, with rectification ratios that scale with the square root of the ratio of thermal conductivities of the two phases. In this work, the authors introduce and analyse the concept of a Dual Phase Change Thermal Diode (DPCTD) as the junction of two phase change materials with similar phase boundary temperatures but opposite temperature coefficients of thermal conductivity. Such systems possess a significantly enhanced optimal scaling of the rectification ratio as the square root of the product of the thermal conductivity ratios. Furthermore, the authors experimentally design and fabricate an ambient DPCTD enabled by the junction of an octadecane-impregnated polystyrene foam, polymerized using a high internal phase emulsion template (PFH-O) and a poly(N-isopropylacrylamide) (PNIPAM) aqueous solution. The DPCTD shows a significantly enhanced thermal rectification ratio both experimentally (2.6) and theoretically (2.6) as compared with ideal thermal diodes composed only of the constituent materials.
  • Order enables efficient electron-hole separation at an organic heterojunction with a small energy loss

    Menke, S. Matthew; Cheminal, Alexandre; Conaghan, Patrick; Ran, Niva A.; Greehnam, Neil C.; Bazan, Guillermo C.; Nguyen, Thuc-Quyen; Rao, Akshay; Friend, Richard H. (Springer Nature, 2018-01-12)
    Donor–acceptor organic solar cells often show low open-circuit voltages (VOC) relative to their optical energy gap (Eg) that limit power conversion efficiencies to ~12%. This energy loss is partly attributed to the offset between Eg and that of intermolecular charge transfer (CT) states at the donor–acceptor interface. Here we study charge generation occurring in PIPCP:PC61BM, a system with a very low driving energy for initial charge separation (Eg−ECT ~ 50 meV) and a high internal quantum efficiency (ηIQE ~ 80%). We track the strength of the electric field generated between the separating electron-hole pair by following the transient electroabsorption optical response, and find that while localised CT states are formed rapidly (<100 fs) after photoexcitation, free charges are not generated until 5 ps after photogeneration. In PIPCP:PC61BM, electronic disorder is low (Urbach energy <27 meV) and we consider that free charge separation is able to outcompete trap-assisted non-radiative recombination of the CT state.
  • The importance of OH − transport through anion exchange membrane in microbial electrolysis cells

    Ye, Yaoli; Logan, Bruce (Elsevier BV, 2018-01-11)
    In two-chamber microbial electrolysis cells (MECs) with anion exchange membranes (AEMs), a phosphate buffer solution (PBS) is typically used to avoid increases in catholyte pH as Nernst equation calculations indicate that high pHs adversely impact electrochemical performance. However, ion transport between the chambers will also impact performance, which is a factor not included in those calculations. To separate the impacts of pH and ion transport on MEC performance, a high molecular weight polymer buffer (PoB), which was retained in the catholyte due to its low AEM transport and cationic charge, was compared to PBS in MECs and abiotic electrochemical half cells (EHCs). In MECs, catholyte pH control was less important than ion transport. MEC tests using the PoB catholyte, which had a higher buffer capacity and thus maintained a lower catholye pH (<8), resulted in a 50% lower hydrogen production rate (HPR) than that obtained using PBS (HPR = 0.7 m3-H2 m−3 d−1) where the catholyte rapidly increased to pH = 12. The main reason for the decreased performance using PoB was a lack of hydroxide ion transfer into the anolyte to balance pH. The anolyte pH in MECs rapidly decreased to 5.8 due to a lack of hydroxide ion transport, which inhibited current generation by the anode, whereas the pH was maintained at 6.8 using PBS. In abiotic tests in ECHs, where the cathode potential was set at −1.2 V, the HPR was 133% higher using PoB than PBS due to catholyte pH control, as the anolyte pH was not a factor in the performance. These results show that maintaining charge transfer to control anolyte pH is more important than obtaining a more neutral pH catholyte.
  • High-Performance Single-Crystalline Perovskite Thin-Film Photodetector

    Yang, Zhenqian; Deng, Yuhao; Zhang, Xiaowei; Wang, Suo; Chen, Huazhou; Yang, Sui; Khurgin, Jacob; Fang, Nicholas X.; Zhang, Xiang; Ma, Renmin (Wiley-Blackwell, 2018-01-10)
    The best performing modern optoelectronic devices rely on single-crystalline thin-film (SC-TF) semiconductors grown epitaxially. The emerging halide perovskites, which can be synthesized via low-cost solution-based methods, have achieved substantial success in various optoelectronic devices including solar cells, lasers, light-emitting diodes, and photodetectors. However, to date, the performance of these perovskite devices based on polycrystalline thin-film active layers lags behind the epitaxially grown semiconductor devices. Here, a photodetector based on SC-TF perovskite active layer is reported with a record performance of a 50 million gain, 70 GHz gain-bandwidth product, and a 100-photon level detection limit at 180 Hz modulation bandwidth, which as far as we know are the highest values among all the reported perovskite photodetectors. The superior performance of the device originates from replacing polycrystalline thin film by a thickness-optimized SC-TF with much higher mobility and longer recombination time. The results indicate that high-performance perovskite devices based on SC-TF may become competitive in modern optoelectronics.
  • Fabrication of 3D heteroatom-doped porous carbons from self-assembly of chelate foams via a solid state method

    Wang, Yu; Pan, Ying; Zhu, Liangkui; Guo, Ningning; Wang, Runwei; Zhang, Zongtao; Qiu, Shilun (Royal Society of Chemistry (RSC), 2018-01-09)
    A novel 3D foam-like porous carbon architectures with homogeneous N doping and unique mesopore-in-macropore structures have been fabricated from metal-organic complex via a facile template-free solid state method, which show high specific surface area (2732 m2 g-1), large pore volume (3.31 cm3 g-1), interconnected hierarchical pore structures with macro/meso/micro multimodal distribution and abundant surface functionality N doping (5.36 wt%). These characteristics afford high catalytic performance for oxygen reduction with an onset potential of 0.98 V (vs RHE) and a half-wave potential of 0.83 V (vs RHE) in alkaline media, which are comparable with those of the commercial 20 wt% Pt/C catalyst and many state-of-the-art noble-metal-free catalysts. These results demonstrate the significant advantages of the unique mesopore-in-macropore porous structures with efficient heteroatom doping, which provides abundant of accessible active sites for highly mass and charge transports. The present work pave a new facile and environmentally benign synthesis strategy for the preparation of 3D porous carbon architectures as efficient electrochemical energy devices and give deep insights into fabricating advanced nanostructured materials.
  • Low-Mach number simulations of transcritical flows

    Lapenna, Pasquale E.; Lamioni, Rachele; Ciottoli, Pietro Paolo; Creta, Francesco (American Institute of Aeronautics and Astronautics, 2018-01-08)
    A numerical framework for the direct simulation, in the low-Mach number limit, of reacting and non-reacting transcritical flows is presented. The key feature are an efficient and detailed representation of the real fluid properties and an high-order spatial discretization. The latter is of fundamental importance to correctly resolve the largely non-linear behavior of the fluid in the proximity of the pseudo-boiling. The validity of the low-Mach number assumptions is assessed for a previously developed non-reacting DNS database of transcritical and supercritical mixing. Fully resolved DNS data employing high-fidelity thermodynamical models are also used to investigate the spectral characteristic as well as the differences between transcritical and supercritical jets.
  • Effects of moderate pump and Stokes chirp on chirped-probe pulse femtosecond coherent anti-Stokes Raman scattering thermometry

    Gu, Mingming; Satija, Aman; Lucht, Robert P. (American Institute of Aeronautics and Astronautics, 2018-01-08)
    The effects of moderate levels of chirp in the pump and Stokes pulses on chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CPP fs CARS) were investigated. The frequency chirp in the pump and Stokes pulses was introduced by placing SF11 glass disks with thicknesses of 10 mm or 20 mm in the optical path for these beams. The magnitude of the chirp in the probe beam was much greater and was induced by placing a 30-cm rod of SF10 glass in the beam path. The temperature measurements were performed in hydrogen/air non-premixed flames stabilized on a Hencken burner at equivalence ratios of 0.3, 0.5, 0.7, and 1.0. We performed measurements with no disks in pump and Stokes beam paths, and then with disks of 10 mm and 20 mm placed in both beam paths. The spectrum of the nonresonant background four-wave mixing signal narrowed considerably with increasing pump and Stokes chirp, while the resonant CARS signal was relatively unaffected. Consequently, the interference of the nonresonant background with the resonant CARS signal in the frequency-spread dephasing region of the spectrum was minimized. The increased rate of decay of the resonant CARS signal with increasing temperature was thus readily apparent. We have started to analyze the CPP fs CARS thermometry data and initial results indicate improved accuracy and precision are obtained due to moderate chirp in the pump and Stokes laser pulses.
  • Small angle X-ray scattering and cross-linking for data assisted protein structure prediction in CASP 12 with prospects for improved accuracy

    Ogorzalek, Tadeusz L.; Hura, Greg L.; Belsom, Adam; Burnett, Kathryn H.; Kryshtafovych, Andriy; Tainer, John A.; Rappsilber, Juri; Tsutakawa, Susan E.; Fidelis, Krzysztof (Wiley-Blackwell, 2018-01-04)
    Experimental data offers empowering constraints for structure prediction. These constraints can be used to filter equivalently scored models or more powerfully within optimization functions toward prediction. In CASP12, Small Angle X-ray Scattering (SAXS) and Cross-Linking Mass Spectrometry (CLMS) data, measured on an exemplary set of novel fold targets, were provided to the CASP community of protein structure predictors. As HT, solution-based techniques, SAXS and CLMS can efficiently measure states of the full-length sequence in its native solution conformation and assembly. However, this experimental data did not substantially improve prediction accuracy judged by fits to crystallographic models. One issue, beyond intrinsic limitations of the algorithms, was a disconnect between crystal structures and solution-based measurements. Our analyses show that many targets had substantial percentages of disordered regions (up to 40%) or were multimeric or both. Thus, solution measurements of flexibility and assembly support variations that may confound prediction algorithms trained on crystallographic data and expecting globular fully-folded monomeric proteins. Here, we consider the CLMS and SAXS data collected, the information in these solution measurements, and the challenges in incorporating them into computational prediction. As improvement opportunities were only partly realized in CASP12, we provide guidance on how data from the full-length biological unit and the solution state can better aid prediction of the folded monomer or subunit. We furthermore describe strategic integrations of solution measurements with computational prediction programs with the aim of substantially improving foundational knowledge and the accuracy of computational algorithms for biologically-relevant structure predictions for proteins in solution. This article is protected by copyright. All rights reserved.
  • Environmental and economic assessment of hybrid FO-RO/NF system with selected inorganic draw solutes for the treatment of mine impaired water

    Kim, Jung Eun; Phuntsho, Sherub; Chekli, Laura; Choi, Joon Yong; Shon, Ho Kyong (Elsevier BV, 2018-01-01)
    A hybrid forward osmosis (FO) and reverse osmosis (RO)/nanofiltration (NF) system in a closed-loop operation with selected draw solutes was evaluated to treat coal mine impaired water. This study provides an insight of selecting the most suitable draw solution (DS) by conducting environmental and economic life cycle assessment (LCA). Baseline environmental LCA showed that the dominant components to energy use and global warming are the DS recovery processes (i.e. RO or NF processes) and FO membrane materials, respectively. When considering the DS replenishment in FO, the contribution of chemical use to the overall global warming impact was significant for all hybrid systems. Furthermore, from an environmental perspective, the FO-NF hybrid system with Na2SO4 shows the lowest energy consumption and global warming with additional considerations of final product water quality and FO brine disposal. From an economic perspective, the FO-NF with Na2SO4 showed the lowest total operating cost due to its lower DS loss and relatively low solute cost. In a closed-loop system, FO-NF with NaCl and Na2SO4 had the lowest total water cost at optimum NF recovery rates of 90 and 95%, respectively. FO-NF with Na2SO4 had the lowest environmental and economic impacts. Overall, draw solute performances and cost in FO and recovery rate in RO/NF play a crucial role in determining the total water cost and environmental impact of FO hybrid systems in a closed-loop operation.
  • Non-destructive reversible resistive switching in Cr doped Mott insulator Ca2RuO4: Interface vs bulk effects

    Shen, Shida; Williamson, Morgan; Cao, Gang; Zhou, Jianshi; Goodenough, John; Tsoi, Maxim (AIP Publishing, 2017-12-29)
    A non-destructive reversible resistive switching is demonstrated in single crystals of Cr-doped Mott insulator Ca2RuO4. An applied electrical bias was shown to reduce the DC resistance of the crystal by as much as 75%. The original resistance of the sample could be restored by applying an electrical bias of opposite polarity. We have studied this resistive switching as a function of the bias strength, applied magnetic field, and temperature. A combination of 2-, 3-, and 4-probe measurements provide a means to distinguish between bulk and interfacial contributions to the switching and suggests that the switching is mostly an interfacial effect. The switching was tentatively attributed to electric-field driven lattice distortions which accompany the impurity-induced Mott transition. This field effect was confirmed by temperature-dependent resistivity measurements which show that the activation energy of this material can be tuned by an applied DC electrical bias. The observed resistance switching can potentially be used for building non-volatile memory devices like resistive random access memory.
  • Superluminal plasmons with resonant gain in population inverted bilayer graphene

    Low, Tony; Chen, Pai-Yen; Basov, D. N. (arXiv, 2017-12-28)
    AB-stacked bilayer graphene with a tunable electronic bandgap in excess of the optical phonon energy presents an interesting active medium, and we consider such theoretical possibility in this work. We argue the possibility of a highly resonant optical gain in the vicinity of the asymmetry gap. Associated with this resonant gain are strongly amplified plasmons, plasmons with negative group velocity and superluminal effects, as well as directional leaky modes.
  • The persistent signature of tropical cyclones in ambient seismic noise

    Gualtieri, Lucia; Camargo, Suzana J.; Pascale, Salvatore; Pons, Flavio M.E.; Ekström, Göran (Elsevier BV, 2017-12-28)
    The spectrum of ambient seismic noise shows strong signals associated with tropical cyclones, yet a detailed understanding of these signals and the relationship between them and the storms is currently lacking. Through the analysis of more than a decade of seismic data recorded at several stations located in and adjacent to the northwest Pacific Ocean, here we show that there is a persistent and frequency-dependent signature of tropical cyclones in ambient seismic noise that depends on characteristics of the storm and on the detailed location of the station relative to the storm. An adaptive statistical model shows that the spectral amplitude of ambient seismic noise, and notably of the short-period secondary microseisms, has a strong relationship with tropical cyclone intensity and can be employed to extract information on the tropical cyclones.
  • One ligand capable of in situ reaction in a mixed-ligand system with two new different frameworks

    Wang, Xiaofang; Wang, Runwei; Liu, Xiaofang; Zhu, Pinwen; Qiu, Shilun (Informa UK Limited, 2017-12-24)
    The in situ ligand 2,3-pyrazinedicarboxylic acid (2,3-H2pzdc) mixed with 1,1′-(1,4-butanediyl)bis(benzimidazole) (bbbi) is used to form two coordination polymers ([Cd(2,3-pzdc)(bbbi)] (1) and [Cd2Cl3(2-pzc)(bbbi)2] (2)) under hydrothermal conditions. Complex 1 was obtained in the absence of in situ reaction and 2 was synthesized with 2,3-H2pzdc in situ generating 2-pyrazinecarboxylate (2-pzc−). The structural details reveal that 1 has a 3D framework with dia topology, and 2 is a 2D layer structure and develops a 3D supramolecular structure via strong π⋯π stacking interactions. The ligand effects were compared for the two frameworks. In addition, fluorescence properties and thermal stabilities of 1 and 2 in the solid were studied.
  • 3DRISM-HI-D2MSA: an improved analytic theory to compute solvent structure around hydrophobic solutes with proper treatment of solute–solvent electrostatic interactions

    Cao, Siqin; Zhu, Lizhe; Huang, Xuhui (Informa UK Limited, 2017-12-22)
    The 3D reference interaction site model (3DRISM) is a powerful tool to study the thermodynamic and structural properties of liquids. However, for hydrophobic solutes, the inhomogeneity of the solvent density around them poses a great challenge to the 3DRISM theory. To address this issue, we have previously introduced the hydrophobic-induced density inhomogeneity theory (HI) for purely hydrophobic solutes. To further consider the complex hydrophobic solutes containing partial charges, here we propose the D2MSA closure to incorporate the short-range and long-range interactions with the D2 closure and the mean spherical approximation, respectively. We demonstrate that our new theory can compute the solvent distributions around real hydrophobic solutes in water and complex organic solvents that agree well with the explicit solvent molecular dynamics simulations.
  • Epitaxial Single-Layer MoS2 on GaN with Enhanced Valley Helicity

    Wan, Yi; Xiao, Jun; Li, Jingzhen; Fang, Xin; Zhang, Kun; Fu, Lei; Li, Pan; Song, Zhigang; Zhang, Hui; Wang, Yilun; Zhao, Mervin; Lu, Jing; Tang, Ning; Ran, Guangzhao; Zhang, Xiang; Ye, Yu; Dai, Lun (Wiley-Blackwell, 2017-12-19)
    Engineering the substrate of 2D transition metal dichalcogenides can couple the quasiparticle interaction between the 2D material and substrate, providing an additional route to realize conceptual quantum phenomena and novel device functionalities, such as realization of a 12-time increased valley spitting in single-layer WSe2 through the interfacial magnetic exchange field from a ferromagnetic EuS substrate, and band-to-band tunnel field-effect transistors with a subthreshold swing below 60 mV dec−1 at room temperature based on bilayer n-MoS2 and heavily doped p-germanium, etc. Here, it is demonstrated that epitaxially grown single-layer MoS2 on a lattice-matched GaN substrate, possessing a type-I band alignment, exhibits strong substrate-induced interactions. The phonons in GaN quickly dissipate the energy of photogenerated carriers through electron–phonon interaction, resulting in a short exciton lifetime in the MoS2/GaN heterostructure. This interaction enables an enhanced valley helicity at room temperature (0.33 ± 0.05) observed in both steady-state and time-resolved circularly polarized photoluminescence measurements. The findings highlight the importance of substrate engineering for modulating the intrinsic valley carriers in ultrathin 2D materials and potentially open new paths for valleytronics and valley-optoelectronic device applications.
  • Micro-light-emitting diodes with III–nitride tunnel junction contacts grown by metalorganic chemical vapor deposition

    Hwang, David; Mughal, Asad J.; Wong, Matthew S.; Alhassan, Abdullah I.; Nakamura, Shuji; DenBaars, Steven P. (Japan Society of Applied Physics, 2017-12-13)
    Micro-light-emitting diodes (µLEDs) with tunnel junction (TJ) contacts were grown entirely by metalorganic chemical vapor deposition. A LED structure was grown, treated with UV ozone and hydrofluoric acid, and reloaded into the reactor for TJ regrowth. The silicon doping level of the n++-GaN TJ was varied to examine its effect on voltage. µLEDs from 2.5 × 10−5 to 0.01 mm2 in area were processed, and the voltage penalty of the TJ for the smallest µLED at 20 A/cm2 was 0.60 V relative to that for a standard LED with indium tin oxide. The peak external quantum efficiency of the TJ LED was 34%.
  • Deep learning enhanced mobile-phone microscopy

    Rivenson, Yair; Koydemir, Hatice Ceylan; Wang, Hongda; Wei, Zhensong; Ren, Zhengshuang; Gunaydin, Harun; Zhang, Yibo; Gorocs, Zoltan; Liang, Kyle; Tseng, Derek; Ozcan, Aydogan (arXiv, 2017-12-12)
    Mobile-phones have facilitated the creation of field-portable, cost-effective imaging and sensing technologies that approach laboratory-grade instrument performance. However, the optical imaging interfaces of mobile-phones are not designed for microscopy and produce spatial and spectral distortions in imaging microscopic specimens. Here, we report on the use of deep learning to correct such distortions introduced by mobile-phone-based microscopes, facilitating the production of high-resolution, denoised and colour-corrected images, matching the performance of benchtop microscopes with high-end objective lenses, also extending their limited depth-of-field. After training a convolutional neural network, we successfully imaged various samples, including blood smears, histopathology tissue sections, and parasites, where the recorded images were highly compressed to ease storage and transmission for telemedicine applications. This method is applicable to other low-cost, aberrated imaging systems, and could offer alternatives for costly and bulky microscopes, while also providing a framework for standardization of optical images for clinical and biomedical applications.
  • Electrochemical Interphases for High-Energy Storage Using Reactive Metal Anodes

    Wei, Shuya; Choudhury, Snehashis; Tu, Zhengyuan; Zhang, Kaihang; Archer, Lynden A. (American Chemical Society (ACS), 2017-12-11)
    Conspectus Stable electrochemical interphases play a critical role in regulating transport of mass and charge in all electrochemical energy storage (EES) systems. In state-of-the-art rechargeable lithium ion batteries, they are rarely formed by design but instead spontaneously emerge from electrochemical degradation of electrolyte and electrode components. High-energy secondary batteries that utilize reactive metal anodes (e.g., Li, Na, Si, Sn, Al) to store large amounts of charge by alloying and/or electrodeposition reactions introduce fundamental challenges that require rational design in order to stabilize the interphases. Chemical instability of the electrodes in contact with electrolytes, morphological instability of the metal–electrolyte interface upon plating and stripping, and hydrodynamic-instability-induced electroconvection of the electrolyte at high currents are all known to cause metal electrode–electrolyte interfaces to continuously evolve in morphology, uniformity, and composition. Additionally, metal anodes undergo large changes in volume during lithiation and delithiation, which means that even in the rare cases where spontaneously formed solid electrode–electrolyte interphases (SEIs) are in thermodynamic equilibrium with the electrode, the SEI is under dynamic strain, which inevitably leads to cracking and/or rupture during extended battery cycling. There is an urgent need for interphases that are able to overcome each of these sources of instability with minimal losses of electrolyte and electrode components. Complementary chemical synthesis strategies are likewise urgently needed to create self-limited and mechanically durable SEIs that are able to flex and shrink to accommodate volume change. These needs are acute for practically relevant cells that cannot utilize large excesses of anode and electrolyte as employed in proof-of-concept-type experiments reported in the scientific literature. This disconnect between practical needs and research practices makes it difficult to translate promising literature results, underscoring the importance of research designed to reveal principles for good interphase design. This Account considers the fundamental processes involved in interphase formation, stability, and failure and on that basis identifies design principles, synthesis procedures, and characterization methods for enabling stable metal anode–electrolyte interfaces for EES. We first review results from experimental, continuum theoretical, and computational analyses of interfacial transport to identify fundamental connections between the composition of the SEI at metal–electrolyte interfaces and stability. Design principles and tools for creating stable artificial solid–electrolyte interphases (ASEIs) based on polymers, ionic liquids, ceramics, nanoparticles, salts, and their combinations are subsequently discussed. Interphases composed of a second electrochemically active material that stores charge by different processes from the underlying metal electrode emerge as particularly attractive routes toward so-called hybrid electrodes that enable facile scale-up of ASEI designs for commercially relevant EES.

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