Single-atom infrared emission in doped silicon nanocrystals.

Silicon luminescence, due to silicon being abundant, non-toxic and harmless, is a topic of pivotal importance in optoelectronics and biological imaging. However, a major challenge in developing high-efficiency silicon light sources is the relatively weak allowable transitions. This study focuses on single atom-doped silicon nanocrystals (Si NCs) and theoretically investigates the emission behavior of single atoms within a tetrahedral coordination field. Doping a single atom in Si NCs can result in a ∼102 times improvement at least in the squared transition dipole moment (TDM2), and induce a spectral shift towards near- and mid-infrared wavelengths. These findings offer a strong foundation for designing Si NCs for on-chip optical communication and single photon emitters.

Boosting the Photoluminescence Quantum Yield and Stability of Lead-Free CsEuCl3 Nanocrystals via Ni2+ Doping.

Colloidal CsPbX3 (X = Br, Cl, or I) perovskite nanocrystals (PNCs) have emerged as low-cost, high-performance light-emitting materials, whereas the toxicity of lead limits their applications. Europium halide perovskites offer promising alternatives to lead-based perovskites due to their narrow spectral width and high monochromaticity. Nonetheless, the photoluminescence quantum yields (PLQYs) of CsEuCl3 PNCs have been very low (∼2%). Herein, Ni2+-doped CsEuCl3 PNCs have been first reported, exhibiting bright blue emission centered at 430.6 ± 0.6 nm with a full width at half-maximum of 23.5 ± 0.3 nm and a PLQY of 19.7 ± 0.4%. To the best of our knowledge, this is the highest PLQY value reported for CsEuCl3 PNCs so far, an order of magnitude higher than in previous work. DFT calculations demonstrate that Ni2+ enhances PLQY by concurrently increasing the oscillator strength and removing Eu3+ which hinders the photorecombination process. B-site doping offers a promising approach to enhance the performance of lanthanide-based lead-free PNCs.

Boosting Hydrogen Evolution Reaction Activity of Amorphous Molybdenum Sulfide Under High Currents Via Preferential Electron Filling Induced by Tungsten Doping.

The lack of highly efficient, durable, and cost-effective electrocatalysts for the hydrogen evolution reaction (HER) working at high current densities poses a significant challenge for the large-scale implementation of hydrogen production from renewable energy. Herein, amorphous molybdenum tungsten sulfide/nitrogen-doped reduced graphene oxide nanocomposites (a-MoWSx /N-RGO) are synthesized by plasma treatment for use as high-performance HER catalysts. By adjusting the plasma treatment duration and chemical composition, an optimal a-MoWSx /N-RGO catalyst is obtained, which exhibits a low overpotential of 348 mV at a current density of 1000 mA cm-2 and almost no decay after 24 h of working at this current density, outperforming commercial platinum/carbon (Pt/C) and previously reported heteroatom-doped MoS2 -based catalysts. Based on density functional theory (DFT) calculations, it is found that with a reasonable tungsten doping level, the catalytic active site (2S2 - ) shows excellent catalytic performance working at high current densities because extra electrons preferentially fill at 2S2 - . The introduction of tungsten tends to lower the electronic structure energy, resulting in a closer-to-zero positive Δ G H ∗ $\Delta {G}_{{{\rm{H}}}^{\rm{*}}}$ . Excessive tungsten introduction, however, can lead to structural damage and a worse HER performance under high current densities. The work provides a route towards rationally designing high-performance catalysts for the HER at industrial-level currents using earth-abundant elements.

High-Efficiency Fast-Radiative Blue-Emitting Perovskite Nanoplatelets and Their Formation Mechanisms.

High-efficiency blue perovskite emitters with fast fluorescence radiation are not only crucial to achieving high-quality displays but also highly desired for optical wireless communications and quantum information technologies. Here, we demonstrate the preparation of blue-emitting Eu3+-, Sb3+-, and Ba2+-induced CsPbBr3 nanoplatelets with narrow spectral widths. Among them, Sb3+-doped CsPbBr3 NPLs can reach a photoluminescence quantum yield of 95%, with a very short fluorescence lifetime of 1.48 ns and greatly reduced ligand dosage. Through nuclear magnetic resonance analysis and density functional theory calculations, we find that the dopant-ligand interaction and dopant-induced growth energy barrier decide the growth kinetics of doped nanoplatelets. These mechanisms offer a fresh route to controlling the dimension of nanoscale perovskite emitters and benefit the development of fast-radiative perovskite emitters.

A nanoimprinted artificial engram device.

At present, mainstream neuromorphic hardware is based on artificial synapses; however, an engram, instead of a synapse, has recently been confirmed as the basic unit of memory, which verifies the engram theory proposed by Richard Semon in 1904. Here, we demonstrate an artificial engram device based on a nanoimprinted curable resin. The variation in the relative diffraction efficiency based on the asymmetric reversible topological change of the nanoimprinted resin enables the device to meet all the requirements for artificial engrams, including synaptic plasticity, long memory storage time, asymmetric memorizing-forgetting behaviour and measurable changes and responses. On this basis, we demonstrate the concept of realizing memory formation, memory manipulation and implantation, and memory consolidation using our artificial engram device in comparison with its biological counterpart.

Fabrication of Perovskite Film-Coated Hollow Capillary Fibers Using a Fast Solvent Exchange Method.

Metal halide perovskites have been successfully applied in a variety of fields such as LEDs, lasers and solar cells, thanks to their excellent optoelectronic properties. Capillary fibers can further expand the range of perovskite applications and at the same time improve its stability by encapsulating the perovskite inside the capillary. However, the high-quality perovskite film-coated hollow capillary fibers have yet to be realized. Here, we introduce a fast solvent exchange method which is used for the preparation of neat and smooth perovskite films deposited on the inner surface of capillary fibers. We demonstrate that this fast solvent exchange method is superior to the commonly used spontaneous diffusion-based precipitation method. The obtained hollow capillary fibers show a narrowed spectral width of 4.9 nm under pulse excitation due to the optical cavity effect. This new fabrication method can facilitate the development of perovskites in the fields of capillary lasing, microfluidic sensing, flexible LEDs and luminous fabrics.

Highly Efficient Blue-Emitting CsPbBr3 Perovskite Nanocrystals through Neodymium Doping.

Colloidal CsPbX3 (X = Br, Cl, and I) perovskite nanocrystals exhibit tunable bandgaps over the entire visible spectrum and high photoluminescence quantum yields in the green and red regions. However, the lack of highly efficient blue-emitting perovskite nanocrystals limits their development for optoelectronic applications. Herein, neodymium (III) (Nd3+) doped CsPbBr3 nanocrystals are prepared through the ligand-assisted reprecipitation method at room temperature with tunable photoemission from green to deep blue. A blue-emitting nanocrystal with a central wavelength at 459 nm, an exceptionally high photoluminescence quantum yield of 90%, and a spectral width of 19 nm is achieved. First principles calculations reveal that the increase in photoluminescence quantum yield upon doping is driven by an enhancement of the exciton binding energy due to increased electron and hole effective masses and an increase in oscillator strength due to shortening of the Pb-Br bond. Putting these results together, an all-perovskite white light-emitting diode is successfully fabricated, demonstrating that B-site composition engineering is a reliable strategy to further exploit the perovskite family for wider optoelectronic applications.

Morphology-Tailored Gold Nanoraspberries Based on Seed-Mediated Space-Confined Self-Assembly.

Raspberry-like structure, providing a high degree of symmetry and strong interparticle coupling, has received extensive attention from the community of functional material synthesis. Such structure constructed in the nanoscale using gold nanoparticles has broad applicability due to its tunable collective plasmon resonances, while the synthetic process with precise control of the morphology is critical in realizing its target functions. Here, we demonstrate a synthetic strategy of seed-mediated space-confined self-assembly using the virus-like silica (V-SiO2) nanoparticles as the templates, which can yield gold nanoraspberries (AuNRbs) with uniform size and controllable morphology. The spikes on V-SiO2 templates serve dual functions of providing more growth sites for gold nanoseeds and activating the space-confined effect for gold nanoparticles. AuNRbs with wide-range tunability of plasmon resonances from the visible to near infrared (NIR) region have been successfully synthesized, and how their geometric configurations affect their optical properties is thoroughly discussed. The close-packed AuNRbs have also demonstrated huge potential in Raman sensing due to their abundant "built-in" hotspots. This strategy offers a new route towards synthesizing high-quality AuNRbs with the capability of engineering the morphology to achieve target functions, which is highly desirable for a large number of applications.

All-inorganic perovskite-based distributed feedback resonator.

Halide perovskite materials have rapidly emerged as outstanding optoelectronic materials for solar cells, light-emitting diodes (LEDs), and lasers. Compared to hybrid organic-inorganic perovskites, all-inorganic perovskites have shown unique merits that may contribute to the ultimate goal of developing electrically-pumped lasers. In this paper, we demonstrate a distributed feedback (DFB) resonator using an all-inorganic perovskite thin film as the gain medium. The film has a gain coefficient of 161.1 cm-1 and a loss coefficient of 30.9 cm-1. Excited by picosecond pulses, the microstructured all-inorganic perovskite film exhibits a single-mode emission at 654 nm with a threshold of 33 µJ/cm2. The facile fabrication process provides a promising route towards low-cost single-mode visible lasers for many practical applications.

Nanopatterned luminescent concentrators for visible light communications.

Visible light communication (VLC) is a promising candidate for high-speed wireless communication with numerous unlicensed spectrum. To achieve high-speed data communication, it requires intense light signals concentrated on a tiny fast photodiode. The common way of using focusing optics reduces the field of view (FoV) of the photodiode due to the conservation of étendue. Luminescent solar concentrators (LSC) provide a solution to enhance the signals without affecting the FoV. In this paper we demonstrate nanopatterned LSCs fabricated on flexible plastics that achieve a doubling of optical gain compared to its traditional rectangular counterparts. These LSCs can free VLC detectors from complex active pointing and tracking systems, making them compatible with smart mobile terminals in a simple fashion.

ZnO nanopowder induced light scattering for improved visualization of emission sites in carbon nanotube films and arrays.

We report on ZnO nanopowder induced light scattering for improved visualization of emission sites in carbon nanotube films and arrays. We observed a significant reduction of the internal multiple light scattering phenomena, which are characteristic for ZnO micropowders. The microsized grains of the commercially available ZnO:Zn (P 15) were reduced to the nanometre scale by pulsed laser ablation at an oxygen ambient pressure of 10 kPa. Our investigations show no crystalline change and no shift of the broad green emission peak at 500 nm for the ZnO nanopowder. For the application in field emission displays, we demonstrate the possibility of achieving cathodoluminescence with a fine pitch size of 100 microm of the patterned pixels without requiring additional electron beam focusing and without a black matrix. Moreover, the presented results show the feasibility of employing ZnO nanopowder as a detection material for the phosphorus screen method, which is able to localize emission sites of carbon nanotube films and arrays with an accuracy comparable to scanning anode field emission microscopy.