Alkali metals have low optical losses in the visible to near-infrared (NIR) compared with noble metals. However, their high reactivity prohibits the exploration of their optical properties. Recently sodium (Na) has been experimentally demonstrated as a low-loss plasmonic material.
View Article and Find Full Text PDFSodium (Na) is predicted to be an ideal plasmonic material with ultralow optical loss across visible to near-infrared (NIR). However, there has been limited research on Na plasmonics. Here we develop a scalable fabrication method for Na nanostructures by combining phase-shift photolithography and a thermo-assisted spin-coating process.
View Article and Find Full Text PDFLithium intercalation of MoS is generally believed to introduce a phase transition from H phase (semiconducting) to T phase (metallic). However, during the intercalation process, a spatially sharp boundary is usually formed between the fully intercalated T phase MoS and non-intercalated H phase MoS. The intermediate state, i.
View Article and Find Full Text PDFNanoporous membranes with two-dimensional materials such as graphene oxide have attracted attention in volatile organic compounds (VOCs) and H adsorption because of their unique molecular sieving properties and operational simplicity. However, agglomeration of graphene sheets and low efficiency remain challenging. Therefore, we designed hierarchical nanoporous membranes (HNMs), a class of nanocomposites combined with a carbon sphere and graphene oxide.
View Article and Find Full Text PDFIn lithium-sulfur (Li-S) chemistry, the electrically/ionically insulating nature of sulfur and LiS leads to sluggish electron/ion transfer kinetics for sulfur species conversion. Sulfur and LiS are recognized as solid at room temperature, and solid-liquid phase transitions are the limiting steps in Li-S batteries. Here, we visualize the distinct sulfur growth behaviors on Al, carbon, Ni current collectors and demonstrate that (i) liquid sulfur generated on Ni provides higher reversible capacity, faster kinetics, and better cycling life compared to solid sulfur; and (ii) Ni facilitates the phase transition (e.
View Article and Find Full Text PDFManipulating liquids with tunable shape and optical functionalities in real time is important for electroactive flow devices and optoelectronic devices, but remains a great challenge. Here, we demonstrate electrotunable liquid sulfur microdroplets in an electrochemical cell. We observe electrowetting and merging of sulfur droplets under different potentiostatic conditions, and successfully control these processes via selective design of sulfiphilic/sulfiphobic substrates.
View Article and Find Full Text PDFIt has recently been shown that sulfur, a solid material in its elementary form S, can stay in a supercooled state as liquid sulfur in an electrochemical cell. We establish that this newly discovered state could have implications for lithium-sulfur batteries. Here, through in situ studies of electrochemical sulfur generation, we show that liquid (supercooled) and solid elementary sulfur possess very different areal capacities over the same charging period.
View Article and Find Full Text PDFTo date, effective control over the electrochemical reduction of CO to multicarbon products (C ≥ 2) has been very challenging. Here, we report a design principle for the creation of a selective yet robust catalytic interface for heterogeneous electrocatalysts in the reduction of CO to C oxygenates, demonstrated by rational tuning of an assembly of nitrogen-doped nanodiamonds and copper nanoparticles. The catalyst exhibits a Faradaic efficiency of ~63% towards C oxygenates at applied potentials of only -0.
View Article and Find Full Text PDFA variety of methods including tuning chemical compositions, structures, crystallinity, defects and strain, and electrochemical intercalation have been demonstrated to enhance the catalytic activity. However, none of these tuning methods provide direct dynamical control during catalytic reactions. Here we propose a new method to tune the activity of catalysts through solid-state ion gating manipulation and adjustment (SIGMA) using a catalysis transistor.
View Article and Find Full Text PDFLattice plasmon cavity modes combined with optical gain can exhibit directional and tunable lasing emission at room temperature. However, the mechanistic details governing the dynamics before lasing action are not understood. This paper describes how the long photon lifetimes of lattice plasmon modes can be correlated with the ultrafast dynamics of lasing action and amplified spontaneous emission.
View Article and Find Full Text PDFFast-charging and high-energy-density batteries pose significant safety concerns due to high rates of heat generation. Understanding how localized high temperatures affect the battery is critical but remains challenging, mainly due to the difficulty of probing battery internal temperature with high spatial resolution. Here we introduce a method to induce and sense localized high temperature inside a lithium battery using micro-Raman spectroscopy.
View Article and Find Full Text PDFThe Mg/S battery is attractive because of its high theoretical energy density and the abundance of Mg and S on the earth. However, its development is hindered by the lack of understanding to the underlying electrochemical reaction mechanism of its charge-discharge processes. Here, using a unique in situ X-ray absorption spectroscopic tool, we systematically study the reaction pathways of the Mg/S cells in Mg(HMDS)-AlCl electrolyte.
View Article and Find Full Text PDFLithium (Li) metal has long been considered the "holy grail" of battery anode chemistry but is plagued by low efficiency and poor safety due to its high chemical reactivity and large volume fluctuation, respectively. Here we introduce a new host of wrinkled graphene cage (WGC) for Li metal. Different from recently reported amorphous carbon spheres, WGC show highly improved mechanical stability, better Li ion conductivity, and excellent solid electrolyte interphase (SEI) for continuous robust Li metal protection.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2019
Supercooled liquid sulfur microdroplets were directly generated from polysulfide electrochemical oxidation on various metal-containing electrodes. The sulfur droplets remain liquid at 155 °C below sulfur's melting point ( = 115 °C), with fractional supercooling change ( - )/ larger than 0.40.
View Article and Find Full Text PDFElectrochemical intercalation of ions into the van der Waals gap of two-dimensional (2D) layered materials is a promising low-temperature synthesis strategy to tune their physical and chemical properties. It is widely believed that ions prefer intercalation into the van der Waals gap through the edges of the 2D flake, which generally causes wrinkling and distortion. Here we demonstrate that the ions can also intercalate through the top surface of few-layer MoS and this type of intercalation is more reversible and stable compared to the intercalation through the edges.
View Article and Find Full Text PDFOutdoor heat stress poses a serious public health threat and curtails industrial labor supply and productivity, thus adversely impacting the wellness and economy of the entire society. With climate change, there will be more intense and frequent heat waves that further present a grand challenge for sustainability. However, an efficient and economical method that can provide localized outdoor cooling of the human body without intensive energy input is lacking.
View Article and Find Full Text PDFDoped semiconductors are the most important building elements for modern electronic devices . In silicon-based integrated circuits, facile and controllable fabrication and integration of these materials can be realized without introducing a high-resistance interface. Besides, the emergence of two-dimensional (2D) materials enables the realization of atomically thin integrated circuits.
View Article and Find Full Text PDFExcited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.
View Article and Find Full Text PDFAerosol-induced haze problem has become a serious environmental concern. Filtration is widely applied to remove aerosols from gas streams. Despite classical filtration theories, the nanoscale capture and evolution of aerosols is not yet clearly understood.
View Article and Find Full Text PDFCoherent light sources have been demonstrated based on a wide range of nanostructures, however, little effort has been devoted to probing their underlying coherence properties. Here, we report long-range spatial coherence of lattice plasmon lasers constructed from a periodic array of gold nanoparticles and a liquid gain medium at room temperature. By combining spatial and temporal interferometry, we demonstrate millimeter-scale (∼1 mm) spatial coherence and picosecond (∼2 ps) temporal coherence.
View Article and Find Full Text PDFSpace heating accounts for the largest energy end-use of buildings that imposes significant burden on the society. The energy wasted for heating the empty space of the entire building can be saved by passively heating the immediate environment around the human body. Here, we demonstrate a nanophotonic structure textile with tailored infrared (IR) property for passive personal heating using nanoporous metallized polyethylene.
View Article and Find Full Text PDFSingle band-edge states can trap light and function as high-quality optical feedback for microscale lasers and nanolasers. However, access to more than a single band-edge mode for nanolasing has not been possible because of limited cavity designs. Here, we describe how plasmonic superlattices-finite-arrays of nanoparticles (patches) grouped into microscale arrays-can support multiple band-edge modes capable of multi-modal nanolasing at programmed emission wavelengths and with large mode spacings.
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