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Showing papers in "Nature Nanotechnology in 2017"


Journal ArticleDOI
TL;DR: The current understanding on Li anodes is summarized, the recent key progress in materials design and advanced characterization techniques are highlighted, and the opportunities and possible directions for future development ofLi anodes in applications are discussed.
Abstract: Lithium-ion batteries have had a profound impact on our daily life, but inherent limitations make it difficult for Li-ion chemistries to meet the growing demands for portable electronics, electric vehicles and grid-scale energy storage. Therefore, chemistries beyond Li-ion are currently being investigated and need to be made viable for commercial applications. The use of metallic Li is one of the most favoured choices for next-generation Li batteries, especially Li-S and Li-air systems. After falling into oblivion for several decades because of safety concerns, metallic Li is now ready for a revival, thanks to the development of investigative tools and nanotechnology-based solutions. In this Review, we first summarize the current understanding on Li anodes, then highlight the recent key progress in materials design and advanced characterization techniques, and finally discuss the opportunities and possible directions for future development of Li anodes in applications.

4,302 citations


Journal ArticleDOI
TL;DR: A synthetic strategy to grow Janus monolayers of transition metal dichalcogenides breaking the out-of-plane structural symmetry of MoSSe by means of scanning transmission electron microscopy and energy-dependent X-ray photoelectron spectroscopy is reported.
Abstract: Structural symmetry-breaking plays a crucial role in determining the electronic band structures of two-dimensional materials. Tremendous efforts have been devoted to breaking the in-plane symmetry of graphene with electric fields on AB-stacked bilayers or stacked van der Waals heterostructures. In contrast, transition metal dichalcogenide monolayers are semiconductors with intrinsic in-plane asymmetry, leading to direct electronic bandgaps, distinctive optical properties and great potential in optoelectronics. Apart from their in-plane inversion asymmetry, an additional degree of freedom allowing spin manipulation can be induced by breaking the out-of-plane mirror symmetry with external electric fields or, as theoretically proposed, with an asymmetric out-of-plane structural configuration. Here, we report a synthetic strategy to grow Janus monolayers of transition metal dichalcogenides breaking the out-of-plane structural symmetry. In particular, based on a MoS2 monolayer, we fully replace the top-layer S with Se atoms. We confirm the Janus structure of MoSSe directly by means of scanning transmission electron microscopy and energy-dependent X-ray photoelectron spectroscopy, and prove the existence of vertical dipoles by second harmonic generation and piezoresponse force microscopy measurements.

1,302 citations


Journal ArticleDOI
TL;DR: A simple scalable method is demonstrated to obtain graphene-based membranes with limited swelling, which exhibit 97% rejection for NaCl and decrease exponentially with decreasing sieve size, but water transport is weakly affected.
Abstract: Ion permeation and selectivity of graphene oxide membranes with sub-nm channels dramatically alters with the change in interlayer distance due to dehydration effects whereas permeation of water molecules remains largely unaffected. Graphene oxide membranes show exceptional molecular permeation properties, with promise for many applications1,2,3,4,5. However, their use in ion sieving and desalination technologies is limited by a permeation cutoff of ∼9 A (ref. 4), which is larger than the diameters of hydrated ions of common salts4,6. The cutoff is determined by the interlayer spacing (d) of ∼13.5 A, typical for graphene oxide laminates that swell in water2,4. Achieving smaller d for the laminates immersed in water has proved to be a challenge. Here, we describe how to control d by physical confinement and achieve accurate and tunable ion sieving. Membranes with d from ∼9.8 A to 6.4 A are demonstrated, providing a sieve size smaller than the diameters of hydrated ions. In this regime, ion permeation is found to be thermally activated with energy barriers of ∼10–100 kJ mol–1 depending on d. Importantly, permeation rates decrease exponentially with decreasing sieve size but water transport is weakly affected (by a factor of <2). The latter is attributed to a low barrier for the entry of water molecules and large slip lengths inside graphene capillaries. Building on these findings, we demonstrate a simple scalable method to obtain graphene-based membranes with limited swelling, which exhibit 97% rejection for NaCl.

1,297 citations


Journal ArticleDOI
TL;DR: The Ru@C2N electrocatalyst, made of Ru nanoparticles dispersed within a nitrogenated holey two-dimensional carbon structure, exhibits high turnover frequencies and superior stability in both acidic and alkaline media, comparable to, or even better than, the Pt/C catalyst for the HER.
Abstract: Ruthenium nanoparticles homogeneously dispersed in a nitrogenated, two-dimensional carbon matrix show high turnover frequency and small overpotential for hydrogen evolution reaction both in acidic and alkaline media. The hydrogen evolution reaction (HER) is a crucial step in electrochemical water splitting and demands an efficient, durable and cheap catalyst if it is to succeed in real applications1,2,3. For an energy-efficient HER, a catalyst must be able to trigger proton reduction with minimal overpotential4 and have fast kinetics5,6,7,8,9. The most efficient catalysts in acidic media are platinum-based, as the strength of the Pt–H bond10 is associated with the fastest reaction rate for the HER11,12. The use of platinum, however, raises issues linked to cost and stability in non-acidic media. Recently, non-precious-metal-based catalysts have been reported, but these are susceptible to acid corrosion and are typically much inferior to Pt-based catalysts, exhibiting higher overpotentials and lower stability13,14,15. As a cheaper alternative to platinum, ruthenium possesses a similar bond strength with hydrogen (∼65 kcal mol–1)16, but has never been studied as a viable alternative for a HER catalyst. Here, we report a Ru-based catalyst for the HER that can operate both in acidic and alkaline media. Our catalyst is made of Ru nanoparticles dispersed within a nitrogenated holey two-dimensional carbon structure (Ru@C2N). The Ru@C2N electrocatalyst exhibits high turnover frequencies at 25 mV (0.67 H2 s−1 in 0.5 M H2SO4 solution; 0.75 H2 s−1 in 1.0 M KOH solution) and small overpotentials at 10 mA cm–2 (13.5 mV in 0.5 M H2SO4 solution; 17.0 mV in 1.0 M KOH solution) as well as superior stability in both acidic and alkaline media. These performances are comparable to, or even better than, the Pt/C catalyst for the HER.

1,105 citations


Journal ArticleDOI
TL;DR: Encapsulated 2D InSe expands the family of graphene-like semiconductors and, in terms of quality, is competitive with atomically thin dichalcogenides and black phosphorus.
Abstract: Encapsulated few-layer InSe exhibits a remarkably high electronic quality, which is promising for the development of ultrathin-body high-mobility nanoelectronics. A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound1,2. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes3,4. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 103 cm2 V−1 s−1 and 104 cm2 V−1 s−1 at room and liquid-helium temperatures, respectively, allowing the observation of the fully developed quantum Hall effect. The conduction electrons occupy a single 2D subband and have a small effective mass. Photoluminescence spectroscopy reveals that the bandgap increases by more than 0.5 eV with decreasing the thickness from bulk to bilayer InSe. The band-edge optical response vanishes in monolayer InSe, which is attributed to the monolayer's mirror-plane symmetry. Encapsulated 2D InSe expands the family of graphene-like semiconductors and, in terms of quality, is competitive with atomically thin dichalcogenides5,6,7 and black phosphorus8,9,10,11.

985 citations


Journal ArticleDOI
TL;DR: The latest quantum dot-based single-Photon sources are edging closer to the ideal single-photon source, and have opened new possibilities for quantum technologies.
Abstract: Single photons are a fundamental element of most quantum optical technologies. The ideal single-photon source is an on-demand, deterministic, single-photon source delivering light pulses in a well-defined polarization and spatiotemporal mode, and containing exactly one photon. In addition, for many applications, there is a quantum advantage if the single photons are indistinguishable in all their degrees of freedom. Single-photon sources based on parametric down-conversion are currently used, and while excellent in many ways, scaling to large quantum optical systems remains challenging. In 2000, semiconductor quantum dots were shown to emit single photons, opening a path towards integrated single-photon sources. Here, we review the progress achieved in the past few years, and discuss remaining challenges. The latest quantum dot-based single-photon sources are edging closer to the ideal single-photon source, and have opened new possibilities for quantum technologies.

828 citations


Journal ArticleDOI
TL;DR: This work shows the successful fabrication of inflammation-free, highly gas-permeable, ultrathin, lightweight and stretchable sensors that can be directly laminated onto human skin for long periods of time, realized with a conductive nanomesh structure.
Abstract: Thin-film electronic devices can be integrated with skin for health monitoring and/or for interfacing with machines. Minimal invasiveness is highly desirable when applying wearable electronics directly onto human skin. However, manufacturing such on-skin electronics on planar substrates results in limited gas permeability. Therefore, it is necessary to systematically investigate their long-term physiological and psychological effects. As a demonstration of substrate-free electronics, here we show the successful fabrication of inflammation-free, highly gas-permeable, ultrathin, lightweight and stretchable sensors that can be directly laminated onto human skin for long periods of time, realized with a conductive nanomesh structure. A one-week skin patch test revealed that the risk of inflammation caused by on-skin sensors can be significantly suppressed by using the nanomesh sensors. Furthermore, a wireless system that can detect touch, temperature and pressure is successfully demonstrated using a nanomesh with excellent mechanical durability. In addition, electromyogram recordings were successfully taken with minimal discomfort to the user.

733 citations


Journal ArticleDOI
TL;DR: This Review discusses the progress and the prospects of integrated miniaturized supercapacitors, and discusses their power performances and emphasize the need of a three-dimensional design to boost their energy-storage capacity.
Abstract: The push towards miniaturized electronics calls for the development of miniaturized energy-storage components that can enable sustained, autonomous operation of electronic devices for applications such as wearable gadgets and wireless sensor networks. Microsupercapacitors have been targeted as a viable route for this purpose, because, though storing less energy than microbatteries, they can be charged and discharged much more rapidly and have an almost unlimited lifetime. In this Review, we discuss the progress and the prospects of integrated miniaturized supercapacitors. In particular, we discuss their power performances and emphasize the need of a three-dimensional design to boost their energy-storage capacity. This is obtainable, for example, through self-supported nanostructured electrodes. We also critically evaluate the performance metrics currently used in the literature to characterize microsupercapacitors and offer general guidelines to benchmark performances towards prospective applications.

706 citations


Journal ArticleDOI
TL;DR: The basic principles, advantages and limitations of the most common AFM bioimaging modes are reviewed, including the popular contact and dynamic modes, as well as recently developed modes such as multiparametric, molecular recognition, multifrequency and high-speed imaging.
Abstract: Atomic force microscopy (AFM) is a powerful, multifunctional imaging platform that allows biological samples, from single molecules to living cells, to be visualized and manipulated. Soon after the instrument was invented, it was recognized that in order to maximize the opportunities of AFM imaging in biology, various technological developments would be required to address certain limitations of the method. This has led to the creation of a range of new imaging modes, which continue to push the capabilities of the technique today. Here, we review the basic principles, advantages and limitations of the most common AFM bioimaging modes, including the popular contact and dynamic modes, as well as recently developed modes such as multiparametric, molecular recognition, multifrequency and high-speed imaging. For each of these modes, we discuss recent experiments that highlight their unique capabilities.

649 citations


Journal ArticleDOI
TL;DR: It is experimentally demonstrated that the electronic structure of few-layer phosphorene varies significantly with the number of layers, in good agreement with theoretical predictions, and the interband optical transitions cover a wide, technologically important spectral range.
Abstract: Phosphorene, a single atomic layer of black phosphorus, has recently emerged as a new two-dimensional (2D) material that holds promise for electronic and photonic technologies. Here we experimentally demonstrate that the electronic structure of few-layer phosphorene varies significantly with the number of layers, in good agreement with theoretical predictions. The interband optical transitions cover a wide, technologically important spectral range from the visible to the mid-infrared. In addition, we observe strong photoluminescence in few-layer phosphorene at energies that closely match the absorption edge, indicating that they are direct bandgap semiconductors. The strongly layer-dependent electronic structure of phosphorene, in combination with its high electrical mobility, gives it distinct advantages over other 2D materials in electronic and opto-electronic applications.

625 citations


Journal ArticleDOI
TL;DR: It is found that evaporation from centimetre-sized carbon black sheets can reliably generate sustained voltages of up to 1 V under ambient conditions.
Abstract: Water evaporation from the surface of cheap carbon-black materials can be used to generate sustained voltages of up to 1 V under ambient conditions.

Journal ArticleDOI
TL;DR: It is shown that NEs carrying liposomes that contain paclitaxel (PTX) can penetrate the brain and suppress the recurrence of glioma in mice whose tumour has been resected surgically, and this NE-mediated delivery of drugs efficiently slows the recurrent growth of tumours.
Abstract: Cell-mediated drug-delivery systems have received considerable attention for their enhanced therapeutic specificity and efficacy in cancer treatment. Neutrophils (NEs), the most abundant type of immune cells, are known to penetrate inflamed brain tumours. Here we show that NEs carrying liposomes that contain paclitaxel (PTX) can penetrate the brain and suppress the recurrence of glioma in mice whose tumour has been resected surgically. Inflammatory factors released after tumour resection guide the movement of the NEs into the inflamed brain. The highly concentrated inflammatory signals in the brain trigger the release of liposomal PTX from the NEs, which allows delivery of PTX into the remaining invading tumour cells. We show that this NE-mediated delivery of drugs efficiently slows the recurrent growth of tumours, with significantly improved survival rates, but does not completely inhibit the regrowth of tumours.

Journal ArticleDOI
TL;DR: A minimalist nanovaccine by a simple physical mixture of an antigen with a synthetic polymeric nanoparticle, PC7A NP, which generated a strong cytotoxic T cell response with low systemic cytokine expression is reported, suggesting generation of long-term antitumor memory.
Abstract: The generation of tumour-specific T cells is critically important for cancer immunotherapy. A major challenge in achieving a robust T-cell response is the spatiotemporal orchestration of antigen cross-presentation in antigen-presenting cells with innate stimulation. Here, we report a minimalist nanovaccine, comprising a simple physical mixture of an antigen and a synthetic polymeric nanoparticle, PC7A NP, which generates a strong cytotoxic T-cell response with low systemic cytokine expression. Mechanistically, the PC7A NP achieves efficient cytosolic delivery of tumour antigens to antigen-presenting cells in draining lymph nodes, leading to increased surface presentation while simultaneously activating type I interferon-stimulated genes. This effect is dependent on stimulator of interferon genes (STING), but not the Toll-like receptor or the mitochondrial antiviral-signalling protein (MAVS) pathway. The nanovaccine led to potent tumour growth inhibition in melanoma, colon cancer and human papilloma virus-E6/E7 tumour models. The combination of the PC7A nanovaccine and an anti-PD-1 antibody showed great synergy, with 100% survival over 60 days in a TC-1 tumour model. Rechallenging of these tumour-free animals with TC-1 cells led to complete inhibition of tumour growth, suggesting the generation of long-term antitumour memory. The STING-activating nanovaccine offers a simple, safe and robust strategy in boosting anti-tumour immunity for cancer immunotherapy.

Journal ArticleDOI
TL;DR: A Joule-heated graphene-wrapped sponge (GWS) to clean-up viscous crude oil at a high sorption speed by reducing in situ the viscosity of the crude oil and increasing the oil-diffusion coefficient in the pores of the GWS, which speeded up theOil-sorption rate.
Abstract: The clean-up of viscous crude-oil spills is a global challenge. Hydrophobic and oleophilic oil sorbents have been demonstrated as promising candidates for oil-spill remediation. However, the sorption speeds of these oil sorbents for viscous crude oil are rather limited. Herein we report a Joule-heated graphene-wrapped sponge (GWS) to clean-up viscous crude oil at a high sorption speed. The Joule heat of the GWS reduced in situ the viscosity of the crude oil, which prominently increased the oil-diffusion coefficient in the pores of the GWS and thus speeded up the oil-sorption rate. The oil-sorption time was reduced by 94.6% compared with that of non-heated GWS. Besides, the oil-recovery speed was increased because of the viscosity decrease of crude oil. This in situ Joule self-heated sorbent design will promote the practical application of hydrophobic and oleophilic oil sorbents in the clean-up of viscous crude-oil spills.

Journal ArticleDOI
TL;DR: T theoretical and experimental developments in the emerging field of nanoporous atomically thin membranes are discussed, focusing on the fundamental mechanisms of gas- and liquid-phase transport, membrane fabrication techniques and advances towards practical application.
Abstract: Graphene and other two-dimensional materials offer a new approach to controlling mass transport at the nanoscale. These materials can sustain nanoscale pores in their rigid lattices and due to their minimum possible material thickness, high mechanical strength and chemical robustness, they could be used to address persistent challenges in membrane separations. Here we discuss theoretical and experimental developments in the emerging field of nanoporous atomically thin membranes, focusing on the fundamental mechanisms of gas- and liquid-phase transport, membrane fabrication techniques and advances towards practical application. We highlight potential functional characteristics of the membranes and discuss applications where they are expected to offer advantages. Finally, we outline the major scientific questions and technological challenges that need to be addressed to bridge the gap from theoretical simulations and proof-of-concept experiments to real-world applications.

Journal ArticleDOI
TL;DR: It is shown that AC-NPs deliver tumour-specific proteins to antigen-presenting cells (APCs) and significantly improve the efficacy of αPD-1 (anti-programmed cell death 1) treatment using the B16F10 melanoma model, generating up to a 20% cure rate compared with 0% without AC- NPs.
Abstract: Immunotherapy holds tremendous promise for improving cancer treatment. To administer radiotherapy with immunotherapy has been shown to improve immune responses and can elicit the 'abscopal effect'. Unfortunately, response rates for this strategy remain low. Herein we report an improved cancer immunotherapy approach that utilizes antigen-capturing nanoparticles (AC-NPs). We engineered several AC-NP formulations and demonstrated that the set of protein antigens captured by each AC-NP formulation is dependent on the NP surface properties. We showed that AC-NPs deliver tumour-specific proteins to antigen-presenting cells (APCs) and significantly improve the efficacy of αPD-1 (anti-programmed cell death 1) treatment using the B16F10 melanoma model, generating up to a 20% cure rate compared with 0% without AC-NPs. Mechanistic studies revealed that AC-NPs induced an expansion of CD8+ cytotoxic T cells and increased both CD4+T/Treg and CD8+T/Treg ratios (Treg, regulatory T cells). Our work presents a novel strategy to improve cancer immunotherapy with nanotechnology.

Journal ArticleDOI
TL;DR: It is demonstrated that DNA-carrying nanoparticles can efficiently introduce leukaemia-targeting CAR genes into T-cell nuclei, thereby bringing about long-term disease remission and may provide a practical, broadly applicable treatment that can generate anti-tumour immunity 'on demand' for oncologists in a variety of settings.
Abstract: An emerging approach for treating cancer involves programming patient-derived T cells with genes encoding disease-specific chimeric antigen receptors (CARs), so that they can combat tumour cells once they are reinfused. Although trials of this therapy have produced impressive results, the in vitro methods they require to generate large numbers of tumour-specific T cells are too elaborate for widespread application to treat cancer patients. Here, we describe a method to quickly program circulating T cells with tumour-recognizing capabilities, thus avoiding these complications. Specifically, we demonstrate that DNA-carrying nanoparticles can efficiently introduce leukaemia-targeting CAR genes into T-cell nuclei, thereby bringing about long-term disease remission. These polymer nanoparticles are easy to manufacture in a stable form, which simplifies storage and reduces cost. Our technology may therefore provide a practical, broadly applicable treatment that can generate anti-tumour immunity 'on demand' for oncologists in a variety of settings.

Journal ArticleDOI
TL;DR: In this paper, air-stable, non-encapsulated Bi2O2Se ultrathin films grown by chemical vapour deposition display high electron mobility and exceptional semiconducting transport properties.
Abstract: Air-stable, non-encapsulated Bi2O2Se ultrathin films grown by chemical vapour deposition display high electron mobility and exceptional semiconducting transport properties, making the observation of quantum oscillations possible and suggesting potential applications in electronics.

Journal ArticleDOI
TL;DR: A general approach to achieve inkjet-printable, water-based, two-dimensional crystal formulations, which also provide optimal film formation for multi-stack fabrication and in vitro dose-escalation cytotoxicity assays confirm the biocompatibility of the inks, extending their possible use to biomedical applications.
Abstract: Exploiting the properties of two-dimensional crystals requires a mass production method able to produce heterostructures of arbitrary complexity on any substrate. Solution processing of graphene allows simple and low-cost techniques such as inkjet printing to be used for device fabrication. However, the available printable formulations are still far from ideal as they are either based on toxic solvents, have low concentration, or require time-consuming and expensive processing. In addition, none is suitable for thin-film heterostructure fabrication due to the re-mixing of different two-dimensional crystals leading to uncontrolled interfaces and poor device performance. Here, we show a general approach to achieve inkjet-printable, water-based, two-dimensional crystal formulations, which also provide optimal film formation for multi-stack fabrication. We show examples of all-inkjet-printed heterostructures, such as large-area arrays of photosensors on plastic and paper and programmable logic memory devices. Finally, in vitro dose-escalation cytotoxicity assays confirm the biocompatibility of the inks, extending their possible use to biomedical applications. Device fabrication can be realized via inkjet printing of water-based 2D crystals.

Journal ArticleDOI
TL;DR: It is shown that dextran-coated superparamagnetic iron oxide core-shell nanoworms incubated in human serum and plasma are rapidly opsonized with the third complement component (C3) via the alternative pathway, showing important insight into dynamics of protein adsorption and complement opsonization of nanomedicines.
Abstract: Immune proteins bind to protein corona on core-shell nanoparticles and undergo dynamic exchange in vivo.

Journal ArticleDOI
TL;DR: It is shown how an in-plane magnetic field can brighten the dark excitons in monolayer WSe2 and permit their properties to be observed experimentally and the fine spin-splitting at the conduction band edges is revealed.
Abstract: Monolayer transition metal dichalcogenide crystals, as direct-gap materials with strong light-matter interactions, have attracted much recent attention. Because of their spin-polarized valence bands and a predicted spin splitting at the conduction band edges, the lowest-lying excitons in WX2 (X = S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark excitons. Here, we show how an in-plane magnetic field can brighten the dark excitons in monolayer WSe2 and permit their properties to be observed experimentally. Precise energy levels for both the neutral and charged dark excitons are obtained and compared with ab initio calculations using the GW-BSE approach. As a result of their spin configuration, the brightened dark excitons exhibit much-increased emission and valley lifetimes. These studies directly probe the excitonic spin manifold and reveal the fine spin-splitting at the conduction band edges.

Journal ArticleDOI
TL;DR: A novel approach to defining nanomechanical modes is introduced, which simultaneously provides strong spatial confinement, full isolation from the substrate, and dilution of the resonator material’s intrinsic dissipation by five orders of magnitude.
Abstract: The small mass and high coherence of nanomechanical resonators render them the ultimate mechanical probe, with applications that range from protein mass spectrometry and magnetic resonance force microscopy to quantum optomechanics. A notorious challenge in these experiments is the thermomechanical noise related to the dissipation through internal or external loss channels. Here we introduce a novel approach to define the nanomechanical modes, which simultaneously provides a strong spatial confinement, full isolation from the substrate and dilution of the resonator material's intrinsic dissipation by five orders of magnitude. It is based on a phononic bandgap structure that localizes the mode but does not impose the boundary conditions of a rigid clamp. The reduced curvature in the highly tensioned silicon nitride resonator enables a mechanical Q > 108 at 1 MHz to yield the highest mechanical Qf products (>1014 Hz) yet reported at room temperature. The corresponding coherence times approach those of optically trapped dielectric particles. Extrapolation to 4.2 K predicts quanta per milliseconds heating rates, similar to those of trapped ions. Soft phononic clamping dilutes the intrinsic dissipation of a mechanical resonator's material by five orders of magnitude, enabling a record value of the product between frequency and quality factor at room temperature, and mechanical coherence times otherwise only available in optical or Paul traps.

Journal ArticleDOI
TL;DR: The zeptolitre sensing volume of bilayer-coated solid-state nanopores can be used to determine the approximate shape, volume, charge, rotational diffusion coefficient and dipole moment of individual proteins.
Abstract: Established methods for characterizing proteins typically require physical or chemical modification steps or cannot be used to examine individual molecules in solution. Ionic current measurements through electrolyte-filled nanopores can characterize single native proteins in an aqueous environment, but currently offer only limited capabilities. Here we show that the zeptolitre sensing volume of bilayer-coated solid-state nanopores can be used to determine the approximate shape, volume, charge, rotational diffusion coefficient and dipole moment of individual proteins. To do this, we developed a theory for the quantitative understanding of modulations in ionic current that arise from the rotational dynamics of single proteins as they move through the electric field inside the nanopore. The approach allows us to measure the five parameters simultaneously, and we show that they can be used to identify, characterize and quantify proteins and protein complexes with potential implications for structural biology, proteomics, biomarker detection and routine protein analysis.

Journal ArticleDOI
TL;DR: A series of Li-containing foils inheriting the desirable properties of alloy anodes and pure metal anodes are shown, consisting of densely packed LixM (M = Si, Sn, or Al) nanoparticles encapsulated by large graphene sheets.
Abstract: Lithium alloy nanoparticles are encased inside few-layer graphene to yield a chemically stable, high-capacity anode with promising performance in a full-cell configuration.

Journal ArticleDOI
TL;DR: Greater enhanced valley spitting in monolayer WSe2 is shown, utilizing the interfacial magnetic exchange field (MEF) from a ferromagnetic EuS substrate, which may enable valleytronic and quantum-computing applications.
Abstract: Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition-metal dichalcogenide (TMDC) with a broken inversion symmetry possesses two degenerate yet inequivalent valleys, which offers unique opportunities for valley control through the helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest (∼0.2 meV T-1). Here we show greatly enhanced valley spitting in monolayer WSe2, utilizing the interfacial magnetic exchange field (MEF) from a ferromagnetic EuS substrate. A valley splitting of 2.5 meV is demonstrated at 1 T by magnetoreflectance measurements and corresponds to an effective exchange field of ∼12 T. Moreover, the splitting follows the magnetization of EuS, a hallmark of the MEF. Utilizing the MEF of a magnetic insulator can induce magnetic order and valley and spin polarization in TMDCs, which may enable valleytronic and quantum-computing applications.

Journal ArticleDOI
TL;DR: This discovery highlights the size precision in the body’s response to nanoparticles and opens a new pathway to develop nanomedicines for many diseases associated with glycocalyx dysfunction.
Abstract: The glomerulus can use its glycocalyx layer to precisely control renal clearance and tumour targeting of sub-nm gold nanoclusters with size differences of just a few atoms.

Journal ArticleDOI
TL;DR: The utility of hybrid core-shell nanostructures in which a core plasmonic metal harvests visible-light photons can selectively channel that energy into catalytically active centres on the nanostructure shell is demonstrated.
Abstract: It has been shown that photoexcitation of plasmonic metal nanoparticles (Ag, Au and Cu) can induce direct photochemical reactions. However, the widespread application of this technology in catalysis has been limited by the relatively poor chemical reactivity of noble metal surfaces. Despite efforts to combine plasmonic and catalytic metals, the physical mechanisms that govern energy transfer from plasmonic metals to catalytic metals remain unclear. Here we show that hybrid core-shell nanostructures in which a core plasmonic metal harvests visible-light photons can selectively channel that energy into catalytically active centres on the nanostructure shell. To accomplish this, we developed a synthetic protocol to deposit a few monolayers of Pt onto Ag nanocubes. This model system allows us to conclusively separate the optical and catalytic functions of the hybrid nanomaterial and determine that the flow of energy is strongly biased towards the excitation of energetic charge carriers in the Pt shell. We demonstrate the utility of these nanostructures for photocatalytic chemical reactions in the preferential oxidation of CO in excess H2. Our data demonstrate that the reaction occurs exclusively on the Pt surface.

Journal ArticleDOI
TL;DR: The SPP-based near-field spectroscopy significantly improves experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials, thus opening up new avenues for realizing active metasurfaces and robust optoelectronic systems, with potential applications in information processing and communication.
Abstract: Near-field coupling to surface plasmon polaritons enables the observation of spin-forbidden dark excitonic states in monolayer WSe2. Transition metal dichalcogenide (TMD) monolayers with a direct bandgap feature tightly bound excitons, strong spin–orbit coupling and spin–valley degrees of freedom1,2,3,4. Depending on the spin configuration of the electron–hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark5,6,7,8. Dark excitons involve nominally spin-forbidden optical transitions with a zero in-plane transition dipole moment9, making their detection with conventional far-field optical techniques challenging. Here, we introduce a method for probing the optical properties of two-dimensional materials via near-field coupling to surface plasmon polaritons (SPPs). This coupling selectively enhances optical transitions with dipole moments normal to the two-dimensional plane, enabling direct detection of dark excitons in TMD monolayers. When a WSe2 monolayer is placed on top of a single-crystal silver film10, its emission into near-field-coupled SPPs displays new spectral features whose energies and dipole orientations are consistent with dark neutral and charged excitons. The SPP-based near-field spectroscopy significantly improves experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials, thus opening up new avenues for realizing active metasurfaces and robust optoelectronic systems, with potential applications in information processing and communication11.

Journal ArticleDOI
TL;DR: It is shown that an injectable polymer-modified magnesium silicide (Mg2Si) nanoparticle can act as a DOA by scavenging oxygen in tumours and form by-products that block tumour capillaries from being reoxygenated.
Abstract: A material that rapidly absorbs molecular oxygen (known as an oxygen scavenger or deoxygenation agent (DOA)) has various industrial applications, such as in food preservation, anticorrosion of metal and coal deoxidation. Given that oxygen is vital to cancer growth, to starve tumours through the consumption of intratumoral oxygen is a potentially useful strategy in fighting cancer. Here we show that an injectable polymer-modified magnesium silicide (Mg2Si) nanoparticle can act as a DOA by scavenging oxygen in tumours and form by-products that block tumour capillaries from being reoxygenated. The nanoparticles are prepared by a self-propagating high-temperature synthesis strategy. In the acidic tumour microenvironment, the Mg2Si releases silane, which efficiently reacts with both tissue-dissolved and haemoglobin-bound oxygen to form silicon oxide (SiO2) aggregates. This in situ formation of SiO2 blocks the tumour blood capillaries and prevents tumours from receiving new supplies of oxygen and nutrients.

Journal ArticleDOI
TL;DR: In this paper, a waveguide-integrated light source and photodetector based on a p-n junction of bilayer MoTe2, a two-dimensional transition-metal dichalcogenides (TMD) with an infrared bandgap is presented.
Abstract: One of the current challenges in photonics is developing high-speed, power-efficient, chip-integrated optical communications devices to address the interconnects bottleneck in high-speed computing systems. Silicon photonics has emerged as a leading architecture, in part because of the promise that many components, such as waveguides, couplers, interferometers and modulators, could be directly integrated on silicon-based processors. However, light sources and photodetectors present ongoing challenges. Common approaches for light sources include one or few off-chip or wafer-bonded lasers based on III-V materials, but recent system architecture studies show advantages for the use of many directly modulated light sources positioned at the transmitter location. The most advanced photodetectors in the silicon photonic process are based on germanium, but this requires additional germanium growth, which increases the system cost. The emerging two-dimensional transition-metal dichalcogenides (TMDs) offer a path for optical interconnect components that can be integrated with silicon photonics and complementary metal-oxide-semiconductors (CMOS) processing by back-end-of-the-line steps. Here, we demonstrate a silicon waveguide-integrated light source and photodetector based on a p-n junction of bilayer MoTe2, a TMD semiconductor with an infrared bandgap. This state-of-the-art fabrication technology provides new opportunities for integrated optoelectronic systems.