Continuous carbon capture in an electrochemical solid-electrolyte reactor.

Electrochemical carbon-capture technologies, with renewable electricity as the energy input, are promising for carbon management but still suffer from low capture rates, oxygen sensitivity or system complexity1-6. Here we demonstrate a continuous electrochemical carbon-capture design by coupling oxygen/water (O2/H2O) redox couple with a modular solid-electrolyte reactor7. By performing oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) redox electrolysis, our device can efficiently absorb dilute carbon dioxide (CO2) molecules at the high-alkaline cathode-membrane interface to form carbonate ions, followed by a neutralization process through the proton flux from the anode to continuously output a high-purity (>99%) CO2 stream from the middle solid-electrolyte layer. No chemical inputs were needed nor side products generated during the whole carbon absorption/release process. High carbon-capture rates (440 mA cm-2, 0.137 mmolCO2 min-1 cm-2 or 86.7 kgCO2 day-1 m-2), high Faradaic efficiencies (>90% based on carbonate), high carbon-removal efficiency (>98%) in simulated flue gas and low energy consumption (starting from about 150 kJ per molCO2) were demonstrated in our carbon-capture solid-electrolyte reactor, suggesting promising practical applications.

A multifunctional copper single-atom electrocatalyst aerogel for smart sensing and producing ammonia from nitrate.

Despite modern chemistry's success in providing affordable fertilizers for feeding the population and supporting the ammonia industry, ineffective nitrogen management has led to pollution of water resources and air, contributing to climate change. Here, we report a multifunctional copper single-atom electrocatalyst-based aerogel (Cu SAA) that integrates the multiscale structure of coordinated single-atomic sites and 3D channel frameworks. The Cu SAA demonstrates an impressive faradaic efficiency of 87% for NH3 synthesis, as well as remarkable sensing performance with detection limits of 0.15 ppm for NO3- and 1.19 ppm for NH4+. These multifunctional features enable precise control and conversion of nitrate to ammonia in the catalytic process, facilitating accurate regulation of the ammonium and nitrate ratios in fertilizers. We thus designed the Cu SAA into a smart and sustainable fertilizing system (SSFS), a prototype device for on-site automatic recycling of nutrients with precisely controlled nitrate/ammonium concentrations. The SSFS represents a forward step toward sustainable nutrient/waste recycling, thus permitting efficient nitrogen utilization of crops and mitigating pollutant emissions. This contribution exemplifies how electrocatalysis and nanotechnology can be potentially leveraged to enable sustainable agriculture.

Thin-film lithium niobate electro-optic isolator fabricated by photolithography assisted chemo-mechanical etching.

We report an electro-optic isolator fabricated on thin-film lithium niobate by photolithography-assisted chemo-mechanical etching that shows an isolation of 39.50 dB and an overall fiber-to-fiber loss of 2.6 dB.

Learning Only on Boundaries: A Physics-Informed Neural Operator for Solving Parametric Partial Differential Equations in Complex Geometries.

Recently, deep learning surrogates and neural operators have shown promise in solving partial differential equations  (PDEs). However, they often require a large amount of training data and are limited to bounded domains. In this work, we present a novel physics-informed neural operator method to solve parameterized boundary value problems without labeled data. By reformulating the PDEs into boundary integral equations (BIEs), we can train the operator network solely on the boundary of the domain. This approach reduces the number of required sample points from O(Nd) to O(Nd-1), where d is the domain's dimension, leading to a significant acceleration of the training process. Additionally, our method can handle unbounded problems, which are unattainable for existing physics-informed neural networks (PINNs) and neural operators. Our numerical experiments show the effectiveness of parameterized complex geometries and unbounded problems.

Engineering vascularized skin-mimetic phantom for non-invasive Raman spectroscopy.

Recent advances in Raman spectroscopy have shown great potential for non-invasive analyte sensing, but the lack of a standardized optical phantom for these measurements has hindered further progress. While many research groups have developed optical phantoms that mimic bulk optical absorption and scattering, these materials typically have strong Raman scattering, making it difficult to distinguish metabolite signals. As a result, solid tissue phantoms for spectroscopy have been limited to highly scattering tissues such as bones and calcifications, and metabolite sensing has been primarily performed using liquid tissue phantoms. To address this issue, we have developed a layered skin-mimetic phantom that can support metabolite sensing through Raman spectroscopy. Our approach incorporates millifluidic vasculature that mimics blood vessels to allow for diffusion akin to metabolite diffusion in the skin. Furthermore, our skin phantoms are mechanically mimetic, providing an ideal model for development of minimally invasive optical techniques. By providing a standardized platform for measuring metabolites, our approach has the potential to facilitate critical developments in spectroscopic techniques and improve our understanding of metabolite dynamics in vivo.

Emerging Electrochemical Techniques for Probing Site Behavior in Single-Atom Electrocatalysts.

Single-atom catalysts (SACs) have aroused tremendous interest over the past decade, particularly in the community of energy and environment-related electrocatalysis. A rapidly growing number of recent publications have recognized it as a promising candidate with maximum atomic utilization, distinct activity, and selectivity in comparison to bulk catalysts and nanocatalysts. However, the complexity of localized coordination environments and the dispersion of isolated sites lead to significant difficulties when it comes to gaining insight into the intrinsic behavior of electrocatalytic reactions. Furthermore, the low metal loadings of most SACs make conventional ensemble measurements less likely to be accurate on the subnanoscale. Thus, it remains challenging to probe the activity and properties of individual atomic sites by available commercial instruments and analytical methods. In spite of this, continuing efforts have lately focused on the development of advanced measurement methodologies, which are very useful to the fundamental understanding of SACs. There have recently been a number of in situ/operando techniques applied to SACs, such as electron microscopy, spectroscopy, and other analysis methods, which support relevant functions to identify the active sites and reaction intermediates and to investigate the dynamic behavior of localized structures of the catalytic sites.This Account aims to present recent electrochemical probing techniques which can be used to identify single-atomic catalytic sites within solid supports. First, we describe the basic principles of molecular probe methods for the study and analysis of electrocatalytic site behavior. In particular, the in situ probing technique enabled by surface interrogation scanning electrochemical microscopy (SI-SECM) can measure the active site density and kinetic rate with high resolution. An alternative electrochemical probing technique is further demonstrated on the basis of single-entity electrochemistry, which allows the unique electrochemical imaging of the size and catalytic rate of single atoms, molecules, and clusters. The merits and limitations of different electrochemical techniques are then discussed, along with perspectives for future prospects. Apart from this, we further showcase the powerful capability of emerging electrochemical probing techniques for determining significant effects and properties of SACs for various electrocatalytic reactions, including oxygen reduction and evolution, hydrogen evolution, and nitrate reduction. Overall, electrochemical techniques with atomic resolution have greatly increased opportunities for observing, measuring, and understanding the surface and interface chemistry during energy conversion. In the future, it is anticipated that the development of electrochemical probing techniques will be advanced with innovative perspectives on the behavior and features of SACs. We hope that this Account can contribute in several ways to promoting the fundamental knowledge and technical progress of emerging electrochemical measurements for studying SACs.

Data-driven inverse design of mode-locked fiber lasers.

The diverse applications of mode-locked fiber lasers (MLFLs) raise various demands on the output of the laser, including the pulse duration, energy, and shape. Simulation is an excellent method to guide the design and construction of an MLFL for on-demand laser output. Traditional simulation of an MLFL uses the split-step Fourier method (SSFM) to solve the nonlinear Schrödinger (NLS) equation, which suffers from high computational complexity. As a result, the inverse design of MLFLs via the traditional SSFM-based simulation method relies on the design experience. Here, a completely data-driven approach for the inverse design of MLFLs is proposed, which significantly reduces the computational complexity and achieves a fast automatic inverse design of MLFLs. We utilize a recurrent neural network to realize fast and accurate MLFL modeling, then the desired cavity settings meeting the output demands are searched via a deep-reinforcement learning algorithm. The results prove that the data-driven method enables the accurate inverse design of an MLFL to produce a preset target femtosecond pulse with a certain duration and pulse energy. In addition, the cavity settings generating soliton molecules with different target separations can also be located via the data-driven inverse design. With the GPU acceleration, the time consumption of the data-driven inverse design of an MLFL is less than 1.3 hours. The proposed data-driven approach is applicable to guide the inverse design of an MLFL to meet the different demands of various applications.

Spectral broadening scheme for suppressing SBS effects based on time-domain optimized chirp-like signals.

We propose a novel (to our knowledge) driving scheme to suppress the stimulated Brillouin scattering (SBS) effect in master oscillator power amplification (MOPA) systems based on an external high-order phase modulation. Since seed sources with the linear chirp can uniformly broaden the SBS gain spectrum with a high SBS threshold, a chirp-like signal was designed by applying further editing and processing to the piecewise parabolic signal. Compared with the traditional piecewise parabolic signal, the chirp-like signal has similar linear chirp characteristics and can reduce the driving power and sampling rate requirements, enabling more efficient spectral spreading. The SBS threshold model is constructed theoretically based on the three-wave coupling equation. The spectrum modulated by the chirp-like signal is compared with the flat-top and Gaussian spectra in terms of the SBS threshold and the bandwidth-distribution normalized threshold, and a considerable improvement is demonstrated. Meanwhile, the experimental validation is carried out in a watt-class amplifier based on the MOPA structure. At a 3 dB bandwidth of ∼10 GHz, the SBS threshold of the seed source modulated by the chirp-like signal is improved by 35% compared to the flat-top spectrum and 18% compared to the Gaussian spectrum, respectively, and the normalized threshold is also the highest among them. Our study shows that the SBS suppression effect is not only related to the power distribution of the spectrum but also can be improved by the time domain design, which provides a new idea for analyzing and improving the SBS threshold of narrow-linewidth fiber lasers.

Erbium-ytterbium codoped thin-film lithium niobate integrated waveguide amplifier with a 27†dB internal net gain.

A photonic integrated waveguide amplifier fabricated on erbium-ytterbium (Er-Yb) codoped thin-film lithium niobate (TFLN) has been investigated in this work. A small-signal internal net gain of 27 dB is achieved at a signal wavelength of 1532 nm in the fabricated Er-Yb TFLN waveguide amplifier pumped by a diode laser at ≈980 nm. Experimental characterizations reveal the suitability of waveguide fabrication by the photolithography-assisted chemo-mechanical etching (PLACE) technique and also the gain in an Yb-sensitized-Er material. The demonstrated high-gain chip-scale TFLN amplifier is promising for interfacing with established lithium niobate integrated devices, greatly extending the spectrum of TFLN photonic applications.

On-chip single-mode thin-film lithium niobate Fabry-Perot resonator laser based on Sagnac loop reflectors.

We demonstrate an on-chip single-mode Er3+-doped thin-film lithium niobate (Er:TFLN) laser which consists of a Fabry-Perot (FP) resonator based on Sagnac loop reflectors (SLRs). The fabricated Er:TFLN laser has a footprint of 6.5 mm × 1.5 mm with a loaded quality (Q) factor of 1.6 × 105 and a free spectral range (FSR) of 63 pm. We generate the single-mode laser at 1544 nm wavelength with a maximum output power of 44.7 µW and a slope efficiency of 0.18%.

On-chip coherent beam combination of waveguide amplifiers on Er3+-doped thin film lithium niobate.

We demonstrate on-chip coherent beam combination of two waveguide amplifiers on Er3+-doped thin film lithium niobate (Er:TFLN) platform. Our device is built based on an electro-optic modulator fabricated on Er:TFLN. The output power of the coherently combined amplifiers is measured as high as 12.9 mW, surpassing that of previous single waveguide amplifiers based on an Er3+-doped thin film lithium niobate platform.

Structurally Dynamic Hydrogels for Biomedical Applications: Pursuing a Fine Balance between Macroscopic Stability and Microscopic Dynamics.

Owing to their unique chemical and physical properties, hydrogels are attracting increasing attention in both basic and translational biomedical studies. Although the classical hydrogels with static networks have been widely reported for decades, a growing number of recent studies have shown that structurally dynamic hydrogels can better mimic the dynamics and functions of natural extracellular matrix (ECM) in soft tissues. These synthetic materials with defined compositions can recapitulate key chemical and biophysical properties of living tissues, providing an important means to understanding the mechanisms by which cells sense and remodel their surrounding microenvironments. This review begins with the overall expectation and design principles of dynamic hydrogels. We then highlight recent progress in the fabrication strategies of dynamic hydrogels including both degradation-dependent and degradation-independent approaches, followed by their unique properties and use in biomedical applications such as regenerative medicine, drug delivery, and 3D culture. Finally, challenges and emerging trends in the development and application of dynamic hydrogels are discussed.

Functionalization of Pentacene: A Facile and Versatile Approach to Contorted Polycyclic Aromatic Hydrocarbons.

In this work, a facile and versatile strategy for the synthesis of contorted polycyclic aromatic hydrocarbons (PAHs) starting from the functionalized pentacene was established. A series of novel PAHs 1-4 and their derivatives were synthesized through a simple two-step synthesis procedure involving an intramolecular reductive Friedel-Crafts cyclization of four newly synthesized pentacene aldehydes 5-8 as a key step. All the molecules were confirmed by single-crystal X-ray diffraction and their photophysical and electrochemical properties were studied in detail. Interestingly, the most striking feature of 1-4 is their highly contorted carbon structures and the accompanying helical chirality. In particular, the optical resolution of 2 was successfully achieved by chiral-phase HPLC, and the enantiomers were characterized by circular dichroism and circularly polarized luminescence spectroscopy. Despite the highly nonplanar conformations, these contorted PAHs exhibited emissive properties with moderate-to-good fluorescence quantum yields, implying the potential utility of this series PAHs as high-quality organic laser dyes. By using a self-assembly method with the help of epoxy resin, a bottle microlaser based on 3 a was successfully illustrated with a lasing wavelength of 567.8 nm at a threshold of 0.3 mJ/cm2 . We believe that this work will shed light on the chemical versatility of pentacene and its derivatives in the construction of novel functionalized PAHs.

Laser diode-pumped compact hybrid lithium niobate microring laser.

We demonstrate a compact hybrid lithium niobate microring laser by butt coupling a commercial 980-nm pump laser diode chip with a high-quality Er3+-doped lithium niobate microring chip. Single-mode lasing emission at 1531-nm wavelength from the Er3+-doped lithium niobate microring can be observed with the integrated 980-nm laser pumping. The compact hybrid lithium niobate microring laser occupies the chip size of 3 mm × 4 mm × 0.5 mm. The threshold pumping laser power is 6 mW and the threshold current is 0.5 A (operating voltage 1.64 V) at atmospheric temperature. The spectrum featuring single-mode lasing with small linewidth of 0.05 nm is observed. This work explores a robust hybrid lithium niobate microring laser source which has potential applications in coherent optical communication and precision metrology.

Hydrogels and Hydrogel-Derived Materials for Energy and Water Sustainability.

Energy and water are of fundamental importance for our modern society, and advanced technologies on sustainable energy storage and conversion as well as water resource management are in the focus of intensive research worldwide. Beyond their traditional biological applications, hydrogels are emerging as an appealing materials platform for energy- and water-related applications owing to their attractive and tailorable physiochemical properties. In this review, we highlight the highly tunable synthesis of various hydrogels, involving key synthetic elements such as monomer/polymer building blocks, cross-linkers, and functional additives, and discuss how hydrogels can be employed as precursors and templates for architecting three-dimensional frameworks of electrochemically active materials. We then present an in-depth discussion of the structure-property relationships of hydrogel materials based on fundamental gelation chemistry, ultimately targeting properties such as enhanced ionic/electronic conductivities, mechanical strength, flexibility, stimuli-responsiveness, and desirable swelling behavior. The unique interconnected porous structures of hydrogels enable fast charge/mass transport while offering large surface areas, and the polymer-water interactions can be regulated to achieve desirable water retention, absorption, and evaporation within hydrogels. Such structure-derived properties are also intimately coordinated to realize multifunctionality and stability for different target devices. The plethora of stimulating examples is expounded with a focus on batteries, supercapacitors, electrocatalysts, solar water purification, and atmospheric water harvesting, which showcase the unprecedented technological potential enabled by hydrogels and hydrogel-derived materials. Finally, we study the challenges and potential ways of tackling them to reveal the underlying mechanisms and transform the current development of hydrogel materials into sustainable energy and water technologies.

Defect engineering of metal-oxide interface for proximity of photooxidation and photoreduction.

Close proximity between different catalytic sites is crucial for accelerating or even enabling many important catalytic reactions. Photooxidation and photoreduction in photocatalysis are generally separated from each other, which arises from the hole-electron separation on photocatalyst surface. Here, we show with widely studied photocatalyst Pt/[Formula: see text] as a model, that concentrating abundant oxygen vacancies only at the metal-oxide interface can locate hole-driven oxidation sites in proximity to electron-driven reduction sites for triggering unusual reactions. Solar hydrogen production from aqueous-phase alcohols, whose hydrogen yield per photon is theoretically limited below 0.5 through conventional reactions, achieves an ultrahigh hydrogen yield per photon of 1.28 through the unusual reactions. We demonstrated that such defect engineering enables hole-driven CO oxidation at the Pt-[Formula: see text] interface to occur, which opens up room-temperature alcohol decomposition on Pt nanoparticles to [Formula: see text] and adsorbed CO, accompanying with electron-driven proton reduction on Pt to [Formula: see text].

On-chip tunable microdisk laser fabricated on Er3+-doped lithium niobate on insulator.

We demonstrate a C-band wavelength-tunable microlaser with an Er3+-doped high quality (∼1.8×106) lithium niobate microdisk resonator. With a 976 nm continuous-wave pump laser, lasing action can be observed at a pump power threshold lower than 400 µW at room temperature. Furthermore, the microdisk laser wavelength can be tuned by varying the pump laser power, showing a tuning efficiency of ∼-17.03pm/mW at low pump power below 13 mW, and 10.58 pm/mW at high pump power above 13 mW.

On-chip microdisk laser on Yb3+-doped thin-film lithium niobate.

We demonstrate an on-chip Yb3+-doped lithium niobate (LN) microdisk laser. The intrinsic quality factors of the fabricated Yb3+-doped LN microdisk resonator are measured up to 3.79×105 at a 976 nm wavelength and 1.1×106 at a 1514 nm wavelength. The multi-mode laser emissions are obtained in a band from 1020 to 1070 nm pumped by a 984 nm laser and with the low threshold of 103µW, resulting in a slope efficiency of 0.53% at room temperature. Furthermore, both the second-harmonic frequency of pump light and the sum frequency of the pump light and laser emissions are generated in the on-chip Yb3+-doped LN microdisk, benefiting from the strong χ(2) nonlinearity of LN. These microdisk lasers are expected to contribute to the high-density integration of a lithium niobate on insulator-based photonic chip.

Electro-optically tunable microring laser monolithically integrated on lithium niobate on insulator.

We demonstrate monolithic integration of an electro-optically (EO) tunable microring laser on lithium niobate on insulator (LNOI) platform. The device is fabricated by photolithography assisted chemo-mechanical etching, and the pump laser is evanescently coupled into the erbium (${\rm{E}}{{\rm{r}}^{3 +}}$)-doped lithium niobate (LN) microring laser using an undoped LN waveguide mounted above the microring. The quality factor of the LN microring resonator is measured as high as ${1.54} \times {{1}}{{{0}}^5}$ at the wavelength of 1542 nm. Lasing action can be observed at a pump power threshold below 3.5 mW using a 980 nm continuous-wave pump laser. Finally, tuning of the laser wavelength is achieved by varying the electric voltage on the microelectrodes fabricated in the vicinity of a microring waveguide, showing an EO coefficient of 0.33 pm/V.

Effects of early cold stress on gene expression in Chlamydomonas reinhardtii.

Cold stress imposes a great impact on the growth of nearly all photosynthetic organisms, including Chlamydomonas reinhardtii (C. reinhardtii). Despite prior studies on the mechanism of stress acclimation in plants, little has been done on the early events of cold sensing in C. reinhardtii. Here, we used C. reinhardtii as a model to study early events of cold signal transduction. By analyzing transcriptomic changes of C. reinhardtii exposed to cold, we found that 3471 genes were differentially expressed after 1 h of cold exposure. These genes were associated with a wide range of biological events and processes such as protein synthesis, cell cycle and protein kinase-based phosphorylation. Besides, the promoter of one gene (named as crAP2) which belongs to AP2/EREBP family and was significantly induced by cold was cloned, and functional analysis was conducted using GUS activity analysis through Agrobacterium-mediated transient assay in tobacco leaves.