Identification of vacancies in electron irradiated GaSb by coincidence Doppler broadening spectroscopy

In this paper we present the results of coincidence Doppler broadening (CDB) measurements and positron lifetime spectroscopy (PLS) on the semiconductor material GaSb. Gallium vacancy with positron lifetime of about 283 ps (V_{Ga, 283 ps}) was identified in as-grown sample by CDB technique and PAS technique. For electron irradiated samples with dosages of 10¹⁷ cm^− 2 and 10¹⁸ cm^− 2, the PAS showed almost the same defect-related positron lifetime of about 285 ps. CDB experiments indicated that defects in irradiated samples were related to Ga vacancies.     

A π-Conjugated Van der Waals Heterostructure Between Single-Atom Ni-Anchored Salphen-Based Covalent Organic Framework and Polymeric Carbon Nitride for High-Efficiency Interfacial Charge Separation

Semiconductor-based heterostructures have exhibited great promise as a photocatalyst to convert solar energy into sustainable chemical fuels, however, their solar-to-fuel efficiency is largely restricted by insufficient interfacial charge separation and limited catalytically active sites. Here the integration of high-efficiency interfacial charge separation and sufficient single-atom metal active sites in a 2D van der Waals (vdW) heterostructure between ultrathin polymeric carbon nitride (p-CN) and Ni-containing Salphen-based covalent organic framework (Ni-COF) nanosheets is illustrated. The results reveal a Ni N₂ O₂ chemical bonding in NiCOF nanosheets, leading to a highly separated single-atom Ni sites, which will function as the catalytically active sites to boost solar fuel production, as confirmed by X-ray absorption spectra and density functional theory calculations. Using ultrafast femtosecond transient adsorption (fs-TA) spectra, it shows that the vdW p-CN/Ni-COF heterostructure exhibits a faster decay lifetime of the exciton annihilation (τ = 18.3 ps) compared to that of neat p-CN (32.6 ps), illustrating an efficiently accelerated electron transfer across the vdW heterointerface from p-CN to Ni-COF, which thus allows more active electrons available to participate in the subsequent reduction reactions. The photocatalytic results offer a chemical fuel generation rate of 2.29 mmol g⁻¹ h⁻¹ for H₂ and 6.2 µmol g⁻¹ h⁻¹ for CO, ≈127 and three times higher than that of neat p-CN, respectively. This work provides new insights into the construction of a π-conjugated vdW heterostructure on promoting interfacial charge separation for high-efficiency photocatalysis.     

Hierarchical Nanoarchitectonics of Ultrathin 2D Organic Nanosheets for Aqueous Processed Electroluminescent Devices

Ultrathin 2D organic nanosheets (2DONs) with high mobility have received tremendous attention due to thickness of few molecular layers. However, ultrathin 2DONs with high luminescence efficiency and flexibility simultaneously are rarely reported. Here, the ultrathin 2DONs (thickness: 19 nm) through the modulation of tighter molecular packing (distance: ≈3.31 Å) achievable from the incorporation of methoxyl and dipenylamine (DPA) groups into 3D spirofluorenexanthene (SFX) building blocks is successfully prepared. Even with closer molecular stacking, ultrathin 2DONs still enable the suppression of aggregation quenching to exhibit higher quantum yields of blue emission (Φ_F = 48%) than that on amorphous film (Φ_F = 20%), and show amplified spontaneous emission (ASE) with a mediate threshold (332 mW cm⁻²). Further, through drop-casting method, the ultrathin 2DONs are self-organized into large-scale flexible 2DONs films (1.5 × 1.5 cm) with the low hardness (H: 0.008 Gpa) and low Young's modulus (E_r: 0.63 Gpa). Impressively, the large-scale 2DONs film can realize electroluminescence performances with a maximum luminance (445 cd m⁻²) and low turn on voltage (3.7 V). These ultrathin 2DONs provide a new avenue for the realization of flexible electrically pumping lasers and intelligent quantum tunneling systems.     

Facile preparation of Gd3+ doped carbon quantum dots: Photoluminescence materials with magnetic resonance response as magnetic resonance/fluorescence bimodal probes

There are a few bimodal molecular imaging probes constructed by gadolinium (3+) ions in combination with carbon quantum dots (CQDs), and the reported ones show such obvious drawbacks as low luminous efficiency and weak MRI contrast. In the paper, a kind of CQDs photoluminescence materials with magnetic resonance response was prepared by hydrothermal method and employing gadopentetate monomeglumine (GdPM) as a precusor. Here, the GdPM plays a role of not only carbon source, but also gadolinium (3+) sources. When the GdPM aqueous solution with a concentration of 4 mg mL⁻¹ was pyrolyzed under 220 °C and 2.0 MPa for 8 h, an optimal CQDs was obtained which are doped with gadolinium (3+) ions in both chelates and Gd₂O₃ (named as Gd³⁺-CQDs). The average diameter of the Gd³⁺-CQDs is about 1.6 nm, which show a high photoluminescence quantum yield of 7.1%, as well as high longitudinal relaxivity (r₁) of 9.87 mM⁻¹ s⁻¹. And owing to the unconspicuous cell toxicity, the Gd³⁺-CQDs show big possibility for clinical application in magnetic resonance/fluorescence bimodal molecular imaging.     

Promoting CO2 Dynamic Activation via Micro-Engineering Technology for Enhancing Electrochemical CO2 Reduction

Optimizing the coordination structure and microscopic reaction environment of isolated metal sites is promising for boosting catalytic activity for electrocatalytic CO₂ reduction reaction (CO₂RR) but is still challenging to achieve. Herein, a newly electrostatic induced self-assembly strategy for encapsulating isolated Ni-C₃N₁ moiety into hollow nano-reactor as I-Ni SA/NHCRs is developed, which achieves FE_CO of 94.91% at −0.80 V, the CO partial current density of ≈−15.35 mA cm⁻², superior to that with outer Ni-C₂N₂ moiety (94.47%, ≈−12.06 mA cm⁻²), or without hollow structure (92.30%, ≈−5.39 mA cm⁻²), and high FE_CO of ≈98.41% at 100 mA cm⁻² in flow cell. COMSOL multiphysics finite-element method and density functional theory (DFT) calculation illustrate that the excellent activity for I-Ni SA/NHCRs should be attributed to the structure-enhanced kinetics process caused by its hollow nano-reactor structure and unique Ni-C₃N₁ moiety, which can enrich electron on Ni sites and positively shift d-band center to the Fermi level to accelerate the adsorption and activation of CO₂ molecule and *COOH formation. Meanwhile, this strategy also successfully steers the design of encapsulating isolated iron and cobalt sites into nano-reactor, while I-Ni SA/NHCRs-based zinc-CO₂ battery assembled with a peak power density of 2.54 mW cm−⁻² is achieved.     

ZnO ultra-fine powders and films: hydrothermal synthesis,luminescence and UV lasing at room temperature

Zinc oxide ultra-fine crystalline powders and polycrystalline films of high optical quality were synthesized under soft hydrothermal conditions. The phase composition, crystal morphology, and luminescent properties of submicron ZnO powders and films were studied depending on synthesis conditions (system composition, precursor kind, solvent type and concentration, temperature). For the systems containing metallic zinc, the ZnO growth mechanism was suggested. The most intensive UV luminescence and the highest values of I_UV/I_VIS were observed for polycrystalline films grown on Zn substrates. Low-threshold UV lasing at room temperature was found for ZnO-films, grown in hydrothermal systems with hydroxide or halide solutions as solvents, E _th = 1–5 MW/cm². The lowest threshold was observed on the ZnO films grown using LiOH as a solvent and zinc nitrate as ZnO-precursor. Clear mode structures with line-width 0.3 nm are characteristic of the lasing spectra.     

Emissive characteristics of mesa-stripe lasers (λ=3.0–3.6 μm) made from InGaAsSb/InAsSbP double heterostructures

The directional patterns, current-voltage characteristics, and spectral characteristics of mesastripe lasers with InGaAsSb active layers, emitting at λ=3.0–3.6 μm (77 K) and having threshold currents ≥15 mA (j _th≥200 A/cm²), are investigated. The maximum output power is 1.4 mW (λ∼3.3 μm), the differential quantum efficiency ∼3%(τ=5–30 μs, f=500 Hz) for lasing in a longitudinal mode with beam divergences ΔΘ∥∼15° and ΔΘ ⊥ ∼30°. The relationship of the differential quantum efficiency to the order of the spatial mode of the lasing is demonstrated. A single-mode, current-tunable (−30 cm⁻¹/A) laser is used to measure the transmission of methane in the region of the ν ₃ absorption band. Pis’ma Zh. Tekh. Fiz. 24, 40–45 (June 26, 1998)     

Scanning Kerr Microscopy of the Spin Hall Effect in <Emphasis Type="Italic">n</Emphasis>-Doped GaAs with Various Doping Concentration

We investigated the doping concentration (N _D) dependence of the extrinsic spin Hall effect (SHE) in n-doped GaAs with N _D raging from 3×10¹⁶ cm⁻³ to 5×10¹⁷ cm⁻³. By using scanning Kerr microscopy (SKM) measurements, we observed the Kerr rotation signal due to the spin accumulation near the channel edges in all the samples with different N _D. Moreover, the position and in-plane magnetic field dependence of the Kerr rotation signal are found to vary with N _D. We analyzed the N _D dependence of the spin Hall conductivity by taking account of the N _D-dependent spin lifetime based on the typical drift-diffusion model.     

High cycle fatigue behaviour of microsphere Al2O3–Al particulate metal matrix composites

The high-cycle stress-life (S–N) curve and fatigue crack growth threshold (ΔK_th) behaviour of COMRAL-85^TM, a 6061 aluminium–magnesium–silicon alloy reinforced with 20 vol.% Al₂O₃-based polycrystalline ceramic microspheres, and manufactured by a liquid metallurgy route, have been investigated for a stress ratio of R = −1 (fully reversed loading). Fatigue testing was conducted on both smooth round bar (S–N) specimens and notched round bar (fatigue threshold) specimens. Unreinforced Al 6061-T6 also processed by a liquid metallurgy route and six powder metallurgy processed composites with particle volume fractions ranging between 5% and 30% were also studied. S–N data revealed that the powder metallurgy processed composites generally gave longer fatigue lives than the matrix alloy, whereas COMRAL-85^TM exhibited a reduced fatigue life. The fatigue threshold results were very similar for all the composites, being lower than for Al 6061-T6. Fatigue failure mechanisms were determined from examination of the fracture surfaces and the crack profiles.     

Highly-Directional,Highly-Efficient Solution-Processed Light-Emitting Diodes of All-Face-Down Oriented Colloidal Quantum Well Self-Assembly

Semiconductor colloidal quantum wells (CQWs) provide anisotropic emission behavior originating from their anisotropic optical transition dipole moments (TDMs). Here, solution-processed colloidal quantum well light-emitting diodes (CQW-LEDs) of a single all-face-down oriented self-assembled monolayer (SAM) film of CQWs that collectively enable a supreme level of IP TDMs at 92% in the ensemble emission are shown. This significantly enhances the outcoupling efficiency from 22% (of standard randomly-oriented emitters) to 34% (of face-down oriented emitters) in the LED. As a result, the external quantum efficiency reaches a record high level of 18.1% for the solution-processed type of CQW-LEDs, putting their efficiency performance on par with the hybrid organic-inorganic evaporation-based CQW-LEDs and all other best solution-processed LEDs. This SAM-CQW-LED architecture allows for a high maximum brightness of 19,800 cd m⁻² with a long operational lifetime of 247 h at 100 cd m⁻² as well as a stable saturated deep-red emission (651 nm) with a low turn-on voltage of 1.7 eV at a current density of 1 mA cm⁻² and a high J₉₀ of 99.58 mA cm⁻². These findings indicate the effectiveness of oriented self-assembly of CQWs as an electrically-driven emissive layer in improving outcoupling and external quantum efficiencies in the CQW-LEDs.     

Infrared-to-green up-conversion in Er3+, Yb3+-doped monoclinic KGd(WO4)2 single crystals

Optical spectroscopy of the green emission of erbium in KGd(WO₄)₂ (KGW) single crystals codoped with ytterbium ions is investigated. To do this, we firstly grew good-optical-quality KGW single crystals doped with Er³⁺ and Yb³⁺ at several dopant concentrations by the Top-seeded-solution-growth slow-cooling method (TSSG). Green photoluminescence of Er³⁺ in KGW host was studied at room temperature (RT) and low temperature (10 K) by means of Yb³⁺ sensitization after infrared excitation at 981 nm (10194 cm⁻¹). We calculated the emission and gain cross-sections and compared these with those of other known Er³⁺-doped laser materials like LiYF₄ :Er (YLF:Er) and Y₃Al₅O₁₂:Er (YAG:Er) at RT. Our study also focused on determining the optimal concentration of ions for generating the most intense green emission. We measured the lifetime of the green emission after infrared pump at several Yb³⁺ concentrations. From the low-temperature emission experiments, we determined the energy position of the sublevels of the ground state of erbium.     

Single-Crystal Nanowire Cesium Tin Triiodide Perovskite Solar Cell

This work reports for the first time a highly efficient single-crystal cesium tin triiodide (CsSnI₃) perovskite nanowire solar cell. With a perfect lattice structure, low carrier trap density (≈5 × 10¹⁰ cm⁻³), long carrier lifetime (46.7 ns), and excellent carrier mobility (>600 cm² V⁻¹ s⁻¹), single-crystal CsSnI₃ perovskite nanowires enable a very attractive feature for flexible perovskite photovoltaics to power active micro-scale electronic devices. Using CsSnI₃ single-crystal nanowire in conjunction with highly conductive wide bandgap semiconductors as front-surface-field layers, an unprecedented efficiency of 11.7% under AM 1.5G illumination is achieved. This work demonstrates the feasibility of all-inorganic tin-based perovskite solar cells via crystallinity and device-structure improvement for the high-performance, and thus paves the way for the energy supply to flexible wearable devices in the future.     

Hydrogenation of nanocrystalline Si thin film transistors employing inductively coupled plasma chemical vapor deposition for flexible electronics

We have investigated the plasma hydrogenation effect on a nanocrystalline silicon (nc-Si) thin film transistor (TFT) fabricated by inductively coupled plasma chemical vapor deposition (ICP-CVD) at 150 °C. The top-gate nc-Si TFT showed a mobility of ∼ 6 cm²/Vs and V_th of 8 V. The hydrogenation employing ICP-CVD was performed at 100 °C for 4 min in order to improve the characteristics of nc-Si TFT. The mobility was increased from ∼ 6 cm²/Vs to 11 cm²/Vs. The V_th of the nc-Si TFTs was decreased to about 6.8 V from 8.1 V. The on-current at the saturation regime also increased by 66% while the off current was increased slightly. The improvement of mobility, threshold voltage and on-current can be attributed to the hydrogen passivation of the Si dangling bonds in the nc-Si film. The experimental results showed that the 100 °C ICP-CVD hydrogenation is effective to improve the 150 °C nc-Si TFT.     

Defective TiO2−x for High-Performance Electrocatalytic NO Reduction toward Ambient NH3 Production

Synthesis of green ammonia (NH₃) via electrolysis of nitric oxide (NO) is extraordinarily sustainable, but multielectron/proton-involved hydrogenation steps as well as low concentrations of NO can lead to poor activities and selectivities of electrocatalysts. Herein, it is reported that oxygen-defective TiO₂ nanoarray supported on Ti plate (TiO_2−x/TP) behaves as an efficient catalyst for NO reduction to NH₃. In 0.2 m phosphate-buffered electrolyte, such TiO_2−x/TP shows competitive electrocatalytic NH₃ synthesis activity with a maximum NH₃ yield of 1233.2 µg h⁻¹ cm⁻² and Faradaic efficiency of 92.5%. Density functional theory calculations further thermodynamically faster NO deoxygenation and protonation processes on TiO_2−x (101) compared to perfect TiO₂ (101). And the low energy barrier of 0.7 eV on TiO_2−x (101) for the potential-determining step further highlights the greatly improved intrinsic activity. In addition, a Zn-NO battery is fabricated with TiO_2−x/TP and Zn plate to obtain an NH₃ yield of 241.7 µg h⁻¹ cm⁻² while providing a peak power density of 0.84 mW cm⁻².     

Photoluminescence and electrochemistry behavior of well-dispersible poly-N-[5-(8-quinolinol)ylmethyl]aniline/nano-TiO2 composite

Well-dispersible poly-N-[5-(8-quinolinol)ylmethyl]aniline/nano-TiO₂ composite was synthesized by the surface modification of nano-TiO₂ particles using poly-N-[5-(8-quinolinol)ylmethyl] (PANQ), and it was characterized by Fourier-transform infrared spectroscopy, photoluminescence spectroscopy, thermogravimetric analysis and scanning electron microscope, as well as conductivity and cyclic voltammogram were given. The conductivity of this composite was 2.1 × 10⁻² S cm⁻¹ at 25 °C, and showed good redox reversibility. It was easy to cast a transparent conducting film with photoluminescent property.     

Superior Energy Storage Properties and Optical Transparency in K0.5Na0.5NbO3-Based Dielectric Ceramics via Multiple Synergistic Strategies

Eco-friendly transparent dielectric ceramics with superior energy storage properties are highly desirable in various transparent energy-storage electronic devices, ranging from advanced transparent pulse capacitors to electro-optical multifunctional devices. However, the collaborative improvement of energy storage properties and optical transparency in KNN-based ceramics still remains challenging. To address this issue, multiple synergistic strategies are proposed, such as refining the grain size, introducing polar nanoregions, and inducing a high-symmetry phase structure. Accordingly, outstanding energy storage density (W_total ≈7.5 J cm⁻³, W_rec ≈5.3 J cm⁻³) and optical transmittance (≈76% at 1600 nm, ≈62% at 780 nm) are simultaneously realized in the 0.94(K_0.5Na_0.5)NbO₃-0.06Sr_0.7La_0.2ZrO₃ ceramic, together with satisfactory charge-discharge performances (discharge energy density: ≈2.7 J cm⁻³, power density: ≈243 MW cm⁻³, discharge rate: ≈76 ns), surpassing previously reported KNN-based transparent ceramics. Piezoresponse force microscopy and transmission electron microscopy revealed that this excellent performance can be attributed to the nanoscale domain and submicron-scale grain size. The significant improvement in the optical transparency and energy storage properties of the materials resulted in the widening of the application prospects of the materials.     

RF diode reactive sputtering of n- and p-type zinc oxide thin films

We present the relationship between parameters of reactive RF diode sputtering from a zinc oxide (ZnO) target and the crystalline, electrical and optical properties of n-/p-type ZnO thin films. The properties of the ZnO thin films depended on RF power, substrate temperature and, particularly, on working gas mixtures of Ar/O₂ and of Ar/N₂. Sputtering in Ar+O₂ working gas (up to 75% of O₂) improved the structure of an n-type ZnO thin film, from fibrous ZnO grains to columnar crystallites, both preferentially oriented along the c-axis normally to the substrate (〈0 0 2〉 direction). These films had good piezoelectric properties but also high resistivity (ρ≈10³ Ω cm). ZnO:N p-type films exhibited nanograin structure with preferential 〈0 0 2〉 orientation at 25% N₂ and 〈1 0 0〉 orientation for higher N₂ content. The presence of nitrogen N_O at O-sites forming N_O-O acceptor complexes in ZnO was proven by SIMS and Raman spectroscopy. A minimum value of resistivity of 790 Ω cm, a p-type carrier concentration of 3.6×10¹⁴ cm⁻³ and a Hall mobility of 22 cm² V⁻¹ s⁻¹ were obtained at 75% N₂.     

Engineering Interfacial Built-in Electric Field in Polymetallic Phosphide Heterostructures for Superior Supercapacitors and Electrocatalytic Hydrogen Evolution

Herein, a patterned rod-like CoP@NiCoP core-shell heterostructure is designed to consist of CoP nanowires cross-linked with NiCoP nanosheets in tight strings. The interfacial interaction within the heterojunction between the two components generates a built-in electric field that adjusts the interfacial charge state and create more active sites, accelerating the charge transfer and improving supercapacitor and electrocatalytic performance. The unique core-shell structure suppresses the volume expansion during charging and discharging, achieving excellent stability. As a result, CoP@NiCoP exhibits a high specific capacitance of 2.9 F cm⁻² at a current density of 3 mA cm⁻² and a high ion diffusion rate (D_ion is 2.95 × 10⁻¹⁴ cm² s⁻¹) during charging/discharging. The assembled asymmetric supercapacitor CoP@NiCoP//AC exhibits a high energy density of 42.2 Wh kg⁻¹ at a power density of 126.5 W kg⁻¹ and excellent stability with a capacitance retention rate of 83.8% after 10 000 cycles. Furthermore, the modulated effect induced by the interfacial interaction also endows the self-supported electrode with excellent electrocatalytic HER performance with an overpotential of 71 mV at 10 mA cm⁻². This research may provide a new perspective on the generation of built-in electric field through the rational design of heterogeneous structures for improving the electrochemical and electrocatalytical performance.     

Vapor growth of CdSe:Cr and CdS:Cr single crystals for mid-infrared lasers

Single crystals of CdSe:Cr and CdS:Cr with the doping level up to 10¹⁹ cm⁻³ were grown by a vapor phase contact-free technique. An efficient room-temperature pulsed and continuous wave (CW) lasing with the CdSe:Cr crystal was achieved. First a pulsed lasing with the CdS:Cr crystal was also demonstrated. The slope efficiency on the absorbed energy was as high as 46.5% for Cr²⁺:CdSe and 39% for Cr²⁺:CdS lasers. Using an intra-cavity prism, the Cr²⁺:CdSe laser wavelength was continuously tuned from 2.26 to 3.61 μm while the Cr²⁺:CdS laser from 2.2 to 3.3 μm. For the laser wavelength, the crystal passive loss coefficient was estimated to be smaller than 0.045 cm⁻¹ for CdSe:Cr crystals and 0.039 cm⁻¹ for CdS:Cr crystals. For the Cr²⁺:CdSe laser, the CW output power up to 1.07 W was achieved.     

Ultrafast excitation relaxation in titanylphthalocyanine thin film

Ultrafast excitation relaxation in the whole Q band of titanylphthalocyanine amorphous thin film fabricated by physical jet deposition was investigated by femtosecond time-resolved pump–probe technique. The measured relaxation dynamics was found to be strongly dependent on the wavelength of the laser beam and consists of three quite different processes: an ultrafast process with a lifetime of 0.5–5 ps, a fast and a long-lived processes with lifetimes of about 5–10 ps and longer than 100 ps, respectively. The initial ultrafast decay appearing to be excitation intensity dependent is suggested to represent a bimolecular exciton–exciton annihilation process with a t^−1/2 time dependence of the excited-state population, assigned to a one-dimensional exciton diffusion. The exciton–exciton annihilation is observed in the pump intensity as low as 0.27 GW/cm².