Plasticity in single-crystalline Mg3Bi2 thermoelectric material.

Most of the state-of-the-art thermoelectric materials are inorganic semiconductors. Owing to the directional covalent bonding, they usually show limited plasticity at room temperature1,2, for example, with a tensile strain of less than five per cent. Here we discover that single-crystalline Mg3Bi2 shows a room-temperature tensile strain of up to 100 per cent when the tension is applied along the (0001) plane (that is, the ab plane). Such a value is at least one order of magnitude higher than that of traditional thermoelectric materials and outperforms many metals that crystallize in a similar structure. Experimentally, slip bands and dislocations are identified in the deformed Mg3Bi2, indicating the gliding of dislocations as the microscopic mechanism of plastic deformation. Analysis of chemical bonding reveals multiple planes with low slipping barrier energy, suggesting the existence of several slip systems in Mg3Bi2. In addition, continuous dynamic bonding during the slipping process prevents the cleavage of the atomic plane, thus sustaining a large plastic deformation. Importantly, the tellurium-doped single-crystalline Mg3Bi2 shows a power factor of about 55 microwatts per centimetre per kelvin squared and a figure of merit of about 0.65 at room temperature along the ab plane, which outperforms the existing ductile thermoelectric materials3,4.

Nearly diffraction-limited picosecond pulse amplification from LMA fluoride fiber at 2.8 µm.

We demonstrated the generation of a nearly diffraction-limited picosecond pulse from a large-mode-area (LMA) fluoride fiber amplifier. Seeded with a mode-locked fiber oscillator at 2.8 µm, the LMA Er:ZBLAN fiber amplifier delivered the pulse of 16 µJ with a duration of 70 ps at 5 kHz. The nearly diffraction-limited beam was obtained from the 50 µm LMA fiber using the fundamental mode excitation technique, with a measured M2 value of 1.25 for x axis and 1.27 for y axis, respectively. This high-beam-quality high-energy picosecond fiber-based system of 2.8 µm exhibits a great potential in the high-precision biomaterial processing.

A Conceptual Framework to Understand the Self-Assembly of Chemically Active Colloids.

Colloids that generate chemicals, or "chemically active colloids", can interact with their neighbors and generate patterns via forces arising from such chemical gradients. Examples of such assemblies of chemically active colloids are abundant in the literature, but a unified theoretical framework is needed to rationalize the scattered results. Combining experiments, theory, Brownian dynamics, and finite element simulations, we present here a conceptual framework for understanding how immotile, yet chemically active, colloids assemble. This framework is based on the principle of ionic diffusiophoresis and diffusioosmosis and predicts that a chemically active colloid interacts with its neighbors through short- and long-range interactions that can be either repulsive or attractive, depending on the relative diffusivity of the released cations and anions, and the relative zeta potential of a colloidal particle and the planar surface on which it resides. As a result, 4 types of pairwise interactions arise, leading to 4 different types of colloidal assemblies with distinct patterns. Using short-range attraction and long-range attraction (SALR) systems as an example, we show quantitative agreement between the framework and experiments. The framework is then applied to rationalize a wide range of patterns assembled from chemically active colloids in the literature exhibiting other types of pairwise interactions. In addition, the framework can predict what the assembly looks like with minimal experimental information and help infer ionic diffusivity and zeta potential values in systems where these values are inaccessible. Our results represent a solid step toward building a complete theory for understanding and controlling chemically active colloids, from the molecular level to their mesoscopic superstructures and ultimately to the macroscopic properties of the assembled materials.

Self-Floating Nanoporous High-Entropy Oxides with Tunable Bandgap for Efficient Solar Seawater Desalination.

Nanoporous high-entropy oxide (np-HEO) powders with tunable composition are integrated with a poly(vinylidene fluoride) network to create self-floating solar absorber films for seawater desalination. By progressively increasing the element count, we obtain an optimized 9-component AlNiCoFeCrMoVCuTi-Ox. Density functional theory (DFT) calculations reveal a remarkable reduction in its bandgap, facilitating the light-induced migration of electrons to conduction bands to generate electron-hole pairs, which recombine to produce heat. Simultaneously, the intricate light reflection and refraction pathways, shaped by the nanoporous structure, coupled with the reduced thermal conductivity attributed to the suboptimal crystalline quality of the np-HEO ensure an effective conversion of captured light into thermal energy. Consequently, all these films demonstrate an impressive absorbance rate exceeding 93% across the 250-2500 nm spectral range. Under one sun, the surface temperature of the 9-component film rapidly rises to 110 °C within 90 s with a high pure water evaporation rate of 2.16 kg m-2 h-1.

Sub-picosecond tunable mid-infrared light source for driving high-efficiency optical rectification.

Optical rectification (OR) is a popular way to generate coherent terahertz radiation. Here, we develop a sub-picosecond mid-infrared (mid-IR) light source with a tailored wavelength and pulse duration for enhancing the OR efficiency. Numerical simulations for a LiNbO3-based OR with tilted pulse-front excitation are first conducted to determine the optimal parameters of pump wavelength and pulse duration, demonstrating that the OR efficiency pumped by 4-µm sub-picosecond (0.5-0.6 ps) pulses is approximately twice the value with 0.8-µm pump at the same conditions. Guided by the simulation results, we build a BaGa4Se7-based optical parametric chirped-pulse amplification system with 1030-nm thin-disk pump and broadband mid-IR seeds. The output performances of >200-µJ pulse energy, ∼600-fs pulse duration and 1-kHz pulse repetition rate are achieved in a spectral range tunable from 3.5 to 5 µm. The large energy scalability and high parameter tunability make the light source attractive to high-efficiency OR in various materials.

Efficient continuous wave and passively Q switched Er:GdScO3 laser using Fe:ZnSe at 2.8 µm.

We report on diode-pumped continuous wave and passively Q switched Er:GdScO3 crystal lasers at around 2.8 µm. A continuous wave output power of 579 mW was obtained with a slope efficiency of 16.6%. Using Fe:ZnSe as a saturable absorber, a passively Q switched laser operation was realized. A maximum output power of 32 mW was generated with the shortest pulse duration of 286 ns at a repetition rate of 157.3 kHz, leading to a pulse energy of 204 nJ and a pulse peak power of 0.7 W.

Eight-Component Nanoporous High-Entropy Oxides with Low Ru Contents as High-Performance Bifunctional Catalysts in Zn-Air Batteries.

One major challenge in heterogeneous catalysis is to reduce the usage of noble metals while maintaining the overall catalytic stability and efficiency in various chemical environments. In this work, a series of high-entropy catalysts are synthesized by a chemical dealloying method and find the increased entropy effect and non-noble metal contents would facilitate the formation of complete oxides with low crystallinity. Importantly, an optimal eight-component high-entropy oxide (HEO, Al-Ni-Co-Ru-Mo-Cr-Fe-Ti) is identified, which exhibits further enhanced catalytic activity for the oxygen evolution reaction (OER) as compared to the previously reported quinary AlNiCoRuMo and the widely-used commercial RuO2 catalysts, and at the same time similar catalytic activity for the oxygen reduction reaction (ORR) as the commercial Pt/C with a half-wave potential of 0.87 V. Such high-performance bi-functional catalysts, however, only require a half loading amount of Ru as compared to the quinary AlNiCoRuMo, due to the underlying Cr-Fe synergistic effects on tuning the electronic structures at active surface sites, as revealed by the first-principles density functional theory calculations of the authors. The eight-component HEO also demonstrates excellent stability under continuous electrochemical working conditions, suitable for a wide range of applications such as metal-air batteries.

Highly Strengthened and Toughened Zn-Li-Mn Alloys as Long-Cycling Life and Dendrite-Free Zn Anode for Aqueous Zinc-Ion Batteries.

Zn-ion batteries (ZIBs) using aqueous electrolyte, recently, have been a hot topic owing to the high safety, low cost, and high specific energy capacity. However, the formation of dendrite and side reactions on the Zn anode during cycling inhibit the application of ZIBs. An advanced Zn anode by alloying a small amount of Li and Mn with Zn is hereby reported. It is found that Li and Mn can form cationic ions which restrain lateral diffusion of Zn ions and regulate zinc electrodeposition through the electrostatic shield mechanism. As a result, the formation of Zn dendrite is greatly inhibited. This process also mitigates the formation of Zn-based byproduct and Zn passivation. Consequently, the symmetric ZnLiMn/ZnLiMn cell presents a small overpotential of 30 mV at 1 mA cm-2 , greatly enhanced cycling durability (1000 h at a current density of 1 mA cm-2 ), and a dendrite-free morphology after cycles. Moreover, the authors find that the ZnLiMn alloy has greatly enhanced mechanical properties. The assembled ZnLiMn/MnO2 full cell can retain 96% capacity after 400 cycles at 1 C. Thus, the alloying low-cost Li/Mn strategy is very promising for large-scale production of dendrite-free Zn electrode in rechargeable ZIBs.

Red-diode-clad-pumped CW and mode-locked Er:ZBLAN fiber laser at 3.5†µm.

We report on a red-diode-clad-pumped continuous-wave (CW) and mode-locked Er:ZBLAN fiber laser at 3.5 µm for the first time. Numerical simulation shows that a heavily-doped Er:ZBLAN fiber is favorable for effective generation of 3.5 µm laser through 658 nm laser diode pumping. Using a 7.0 mol.% Er:ZBLAN fiber, CW output power of 203 mW was experimentally obtained at 3462 nm. By incorporating a home-made semiconductor saturable absorber mirror into the cavity, diode-pumped CW mode-locked 3.5 µm Er:ZBLAN fiber laser was first demonstrated with an average power of 19 mW, a pulse duration of 18.1 ps, and a repetition rate of 46 MHz. The research results show that red-diode-clad-pumping provides a simple and potential scheme for 3.5 µm CW and mode-locked Er:ZBLAN fiber laser.

Efficient generation of mid-infrared few-cycle pulses by the intrapulse difference-frequency generation in YCOB.

Yttrium calcium oxyborate (YCOB) crystals have been widely applied for generating intense near-infrared laser pulses by optical parametric amplification. Here, we show that the YCOB crystals oriented in both the XZ and XY principal planes possess broadband phase-matching property of intrapulse difference-frequency generation in the mid-infrared region. Few-cycle pulses tunable from 2 to 4 µm are experimentally produced by using a 7.5-fs pump laser at 800 nm, in which the conversion efficiency can be as high as 2.5%. With a large-size crystal and high-power pump laser, intrapulse difference-frequency generation based on YCOB may provide a new route for directly producing intense few-cycle mid-infrared pulses.

Semiconductor saturable absorber mirror in the 3-5†µm mid-infrared region.

Semiconductor saturable absorber mirrors (SESAMs) have been regarded as a revolutionary technology for ultrafast mode-locked lasers, producing numerous landmark laser breakthroughs. However, the operating wavelength of existing SESAMs is limited to less than 3 µm. In this study, we create a 3-5 µm mid-infrared (MIR) SESAM by engineering an InAs/GaSb type-II superlattice. Bandgap engineering and the strong coupling between potential wells in a superlattice enable a broadband response of saturable absorption in the 3-5 µm spectral range. Using the fabricated SESAM, we realize a SESAM mode-locked Er:ZBLAN fiber laser at 3.5 µm, which delivers MIR ultrashort pulses with high long-term stability. The breakthrough of SESAM fabrication in the MIR will promote the development of MIR ultrafast coherent sources and related application fields.

Hydrogen-assisted synthesis of Ni-ZIF-derived nickel nanoparticle chains coated with nitrogen-doped graphitic carbon layers as efficient electrocatalysts for non-enzymatic glucose detection.

Chains of nickel nanoparticles coated with few nitrogen-doped graphitic carbon layers (Ni@NC) are synthesized by hydrogen-assisted pyrolysis of Ni-ZIF. Hydrogen and temperature can play key roles in the formation of oriented Ni@NC nanoparticle chains, and carbon shells can protect Ni nanoparticles from external oxidation and aggregations. Under the optimized potential (0.60 V vs. Ag/AgCl), the Ni@NC7H nanoparticle chains obtained at 700 °C under H2/Ar atmosphere (Ni@NC7H) demonstrate outstanding performances, such as high sensitivity of 1.44 mA mM-1 cm-2 (RSD = 1.0%), low detection limit of 0.34 µM (S/N = 3), broad linear range from 1 µM to 1.81 mM, and excellent application potential in artificial sweat and human serum. Therefore, the findings above indicate that this study will provide a general methodology for the synthesis of chains-like core-shell nanoparticle electrocatalysts for non-enzymatic glucose detection.

Comparison of multiple tractography methods for reconstruction of the retinogeniculate visual pathway using diffusion MRI.

The retinogeniculate visual pathway (RGVP) conveys visual information from the retina to the lateral geniculate nucleus. The RGVP has four subdivisions, including two decussating and two nondecussating pathways that cannot be identified on conventional structural magnetic resonance imaging (MRI). Diffusion MRI tractography has the potential to trace these subdivisions and is increasingly used to study the RGVP. However, it is not yet known which fiber tracking strategy is most suitable for RGVP reconstruction. In this study, four tractography methods are compared, including constrained spherical deconvolution (CSD) based probabilistic (iFOD1) and deterministic (SD-Stream) methods, and multi-fiber (UKF-2T) and single-fiber (UKF-1T) unscented Kalman filter (UKF) methods. Experiments use diffusion MRI data from 57 subjects in the Human Connectome Project. The RGVP is identified using regions of interest created by two clinical experts. Quantitative anatomical measurements and expert anatomical judgment are used to assess the advantages and limitations of the four tractography methods. Overall, we conclude that UKF-2T and iFOD1 produce the best RGVP reconstruction results. The iFOD1 method can better quantitatively estimate the percentage of decussating fibers, while the UKF-2T method produces reconstructed RGVPs that are judged to better correspond to the known anatomy and have the highest spatial overlap across subjects. Overall, we find that it is challenging for current tractography methods to both accurately track RGVP fibers that correspond to known anatomy and produce an approximately correct percentage of decussating fibers. We suggest that future algorithm development for RGVP tractography should take consideration of both of these two points.

MOF Structure Engineering to Synthesize CoNC Catalyst with Richer Accessible Active Sites for Enhanced Oxygen Reduction.

Single-atom cobalt-based CoNC are promising low-cost electrocatalysts for oxygen reduction reaction (ORR). However, further increasing the single cobalt-based active sites and the ORR activity remain a major challenge. Herein, an acetate (OAc) assisted metal-organic framework (MOF) structure-engineering strategy is developed to synthesize hierarchical accordion-like MOF with higher loading amount and better spatial isolation of Co and much higher yield when compared with widely reported polyhedron MOF. After pyrolysis, the accordion-structured CoNC (CoNC (A)) is loaded with denser CoN4 active sites (Co: 2.88 wt%), approximately twice that of Co in the CoNC reported. The presence of OAc in MOF also induces the generation of big pores (5-50 nm) for improving the accessibility of active sites and mass transfer during catalytic reactions. Consequently, the CoNC (A) catalyst shows an admirable ORR activity with a E1/2 of 0.89 V (40 mV better than Pt/C) in alkaline electrolytes, outstanding durability, and absolute tolerance to methanol in both alkaline and acidic media. The CoNC-based Zn-air battery exhibits a high specific capacity (976 mAh g-1 Zn ), power density (158 mW cm-2 ), rate capability, and long-term stability. This work demonstrates a reliable approach to construct single atom doped carbon catalysts with denser accessible active sites through MOF structure engineering.

2-MW peak-power pulses from a dispersion-managed fluoride fiber amplifier at 2.8 µm.

We report on a scheme of pulse amplification and simultaneous self-compression in fluoride fiber for generating a high-peak-power pulse at 2.8-µm wavelength. We find dispersion management plays a key role for the amplification and self-compression process. Through dispersion management with a Ge rod, pulse amplification and simultaneous pulse self-compression were realized in the small anomalous dispersion region. A 2-MW peak-power pulse was achieved through amplification and self-compression in Er:ZBLAN fiber, with pulse energy of 101 nJ and pulse duration of 49 fs. To the best of our knowledge, this is the highest peak power obtained from fluoride fiber at 2.8 µm, and will benefit a series of applications.

Creation of a novel trigeminal tractography atlas for automated trigeminal nerve identification.

Diffusion MRI (dMRI) tractography has been successfully used to study the trigeminal nerves (TGNs) in many clinical and research applications. Currently, identification of the TGN in tractography data requires expert nerve selection using manually drawn regions of interest (ROIs), which is prone to inter-observer variability, time-consuming and carries high clinical and labor costs. To overcome these issues, we propose to create a novel anatomically curated TGN tractography atlas that enables automated identification of the TGN from dMRI tractography. In this paper, we first illustrate the creation of a trigeminal tractography atlas. Leveraging a well-established computational pipeline and expert neuroanatomical knowledge, we generate a data-driven TGN fiber clustering atlas using tractography data from 50 subjects from the Human Connectome Project. Then, we demonstrate the application of the proposed atlas for automated TGN identification in new subjects, without relying on expert ROI placement. Quantitative and visual experiments are performed with comparison to expert TGN identification using dMRI data from two different acquisition sites. We show highly comparable results between the automatically and manually identified TGNs in terms of spatial overlap and visualization, while our proposed method has several advantages. First, our method performs automated TGN identification, and thus it provides an efficient tool to reduce expert labor costs and inter-operator bias relative to expert manual selection. Second, our method is robust to potential imaging artifacts and/or noise that can prevent successful manual ROI placement for TGN selection and hence yields a higher successful TGN identification rate.

Large magnitude, sign controllable, ultrafast group-velocity control via resonant cascaded nonlinearity in tandem.

Resonant cascaded nonlinearity (RCN) induced by optical parametric amplification (OPA) in a chirped quasi-phase-matching chip can be applied to control the group velocity of ultrafast lasers. However, the group delay produced in a single-stage OPA is limited to the pulse duration, and its sign cannot be altered. In this study, we propose a tandem RCN configuration with multiple OPA stages that can produce large-magnitude and sign-controllable group delays. The group delay produced in the multi-stage configuration is shown to be a linear superposition of each single-stage group delay. By virtue of the byproduct idler in the OPA process, the signal-group delay can be altered from positive to negative (and vice versa) with the same chip structure and pump condition. In the numerical simulation with two OPA stages, both a positive and negative group delay of six-fold pulse duration were achieved for 100-fs pulses at 1550 nm. A much larger group delay can be achieved by increasing the number of OPA stages.

Generation of a mid-infrared femtosecond vortex beam from an optical parametric oscillator.

Mid-infrared femtosecond vortex beams generated by optical parametric oscillators (OPO) are reported for the first time, to the best of our knowledge. Order-tunable femtosecond Hermite-Gauss beams from the first to sixth order are produced from a synchronously pumped OPO and then converted into the corresponding first through sixth-order femtosecond vortex beams by a cylindrical lens mode converter. By slightly tuning the cavity length, the wavelength of the vortex beam can be continuously tunable in the range from 2323 to 2382 nm, and the pulse duration can be changeable from ${\sim}{400}\;{\rm fs}$∼400fs to ${\sim}{1.1}\;{\rm ps}$∼1.1ps. The work provides a flexible and reliable way to generate mid-infrared femtosecond vortex beams, and is of special significance for expanding the wavelength range of femtosecond vortex beams and their application fields.

Few-cycle pulses tunable from 3 to 7 µm via intrapulse difference-frequency generation in oxide LGN crystals.

An ultrashort mid-infrared (IR) source beyond 5 µm is crucial for a plethora of existing and emerging applications in spectroscopy, medical diagnostics, and high-field physics. Nonlinear generation of such sources from well-developed near-IR lasers, however, remains a challenge due to the limitation of mid-IR crystals. Based on oxide La3Ga5.5Nb0.5O14 (LGN) crystals, here we report the generation of femtosecond pulses tunable from 3 to 7 µm by intrapulse difference-frequency generation of 7.5 fs, 800 nm pulses. The efficiency and bandwidth dependences on pump polarization and crystal length are studied for both Type-I and Type-II phase-matching configurations. Maximum pulse energy of ∼10nJ is generated at 5.2 µm with a conversion efficiency of ∼0.14%. Because of the few-cycle pump pulse duration, the generated mid-IR pulses are as short as about three cycles. These results, to the best of our knowledge, represent the first experimental demonstration of LGN in generating mid-IR ultrashort pulses.

Nanoporous Al-Ni-Co-Ir-Mo High-Entropy Alloy for Record-High Water Splitting Activity in Acidic Environments.

Ir-based binary and ternary alloys are effective catalysts for the electrochemical oxygen evolution reaction (OER) in acidic solutions. Nevertheless, decreasing the Ir content to less than 50 at% while maintaining or even enhancing the overall electrocatalytic activity and durability remains a grand challenge. Herein, by dealloying predesigned Al-based precursor alloys, it is possible to controllably incorporate Ir with another four metal elements into one single nanostructured phase with merely ≈20 at% Ir. The obtained nanoporous quinary alloys, i.e., nanoporous high-entropy alloys (np-HEAs) provide infinite possibilities for tuning alloy's electronic properties and maximizing catalytic activities owing to the endless element combinations. Particularly, a record-high OER activity is found for a quinary AlNiCoIrMo np-HEA. Forming HEAs also greatly enhances the structural and catalytic durability regardless of the alloy compositions. With the advantages of low Ir loading and high activity, these np-HEA catalysts are very promising and suitable for activity tailoring/maximization.