Amorphous High-Entropy Hydroxides of Tunable Wide Solar Absorption for Solar Water Evaporation

The high-entropy materials have raised much attention in recent years due to their extraordinary performances in mechanical, catalysis, energy storage fields. Herein, a new type of high-entropy hydroxides (e.g., NiFeCoMnAl(OH)_x) that are amorphous and capable of broad solar absorption is reported. A facile one-pot co-precipitation method is employed to synthesize these amorphous high-entropy hydroxides (a-HEHOs) under ambient conditions. The a-HEHOs thus obtained display widely tunable bandgap (e.g., from 2.6 to 1.1 eV) due to their high-entropy and amorphous characteristics, enabling efficient light absorbance and photothermal conversion in the solar regime. Further solar water evaporation measurements show that the a-HEHOs delivered a considerable energy conversion efficiency of 55%, comparable to black titanium oxides that are synthesized using more complex and expensive methods.     

基于碳化硅衬底的宽禁带半导体外延

宽禁带半导体具备禁带宽度大、电子饱和飘移速度高、击穿场强大等优势,是制备高功率密度、高频率、低损耗电子器件的理想材料。碳化硅(SiC)材料具有热导率高、化学稳定性好、耐高温等优点,在SiC衬底上外延宽禁带半导体材料,对充分发挥宽禁带半导体材料的优势,并提升宽禁带半导体电子器件的性能具有重要意义。得益于SiC衬底质量持续提升及成本不断降低,基于SiC衬底的宽禁带半导体电子市场占比呈现逐年增加的态势。在SiC衬底上外延生长高质量的宽禁带半导体材料是提高宽禁带半导体电子器件性能及可靠性的关键瓶颈。本文综述了近年来国内外研究者们在SiC衬底上外延SiC、氮化镓(GaN)、氧化镓(Ga₂O₃)所取得的研究进展,并展望了SiC衬底上宽禁带半导体外延的发展及应用前景。     

Tuning the electronic properties of hydrogen passivated C3N nanoribbons through van der Waals stacking

The two-dimensional (2D) C₃N has emerged as a material with promising applications in high performance device owing to its intrinsic bandgap and tunable electronic properties. Although there are several reports about the bandgap tuning of C₃N via stacking or forming nanoribbon, bandgap modulation of bilayer C₃N nanoribbons (C₃NNRs) with various edge structures is still far from well understood. Here, based on extensive first-principles calculations, we demonstrated the effective bandgap engineering of C₃N by cutting it into hydrogen passivated C₃NNRs and stacking them into bilayer heterostructures. It was found that armchair (AC) C₃NNRs with three types of edge structures are all semiconductors, while only zigzag (ZZ) C₃NNRs with edges composed of both C and N atoms (ZZCN/ CN) are semiconductors. The bandgaps of all semiconducting C₃NNRs are larger than that of C₃N nanosheet. More interestingly, AC-C₃NNRs with CN/CN edges (AC-CN/CN) possess direct bandgap while ZZ-CN/CN have indirect bandgap. Compared with the monolayer C₃NNR, the bandgaps of bilayer C₃NNRs can be greatly modulated via different stacking orders and edge structures, varying from 0.43 eV for ZZ-CN/CN with AB′-stacking to 0.04 eV for AC-CN/CN with AA-stacking. Particularly, transition from direct to indirect bandgap was observed in the bilayer AC-CN/CN heterostructure with AA′-stacking, and the indirect-to-direct transition was found in the bilayer ZZ-CN/CN with ABstacking. This work provides insights into the effective bandgap engineering of C₃N and offers a new opportunity for its applications in nano-electronics and optoelectronic devices.     

Mixed Fano-SP resonant absorption of THz electromagnetic waves in a photonic resonator contacting with a metal film

In terahertz frequency region, we have investigated theoretically the correlation between spectra of a free photonic structure and that deposited on a metal for several models of metal. It was found that for quasi-normal incidence of p-polarized electromagnetic field the presence of metal generates narrow spectral wells in the middle of reflection windows existing in a free photonic crystal. Quite another manifestation of metal-resonator inter-influence takes place at incident angles exceeding the Brewster angle when reflection spikes coincide with modes of photonic crystal resonator and they are absent throughout the stopband areas. The effects are strongly depended on polarization, number of periods and angle of incidence.     

Anisotropic phononic crystal structure with low-frequency bandgap and heat flux manipulation

This study presents a two-dimensional phononic crystal with heat flux manipulation and wide bandgaps of out-of-plane modes within the low-frequency range. The anisotropic matrix made of spiral-multilayered materials with different thermal conductivities, and the coating layer inserted with metal are designed for heat flux manipulation. Rubber-coated metal cylinders are periodically embedded in the anisotropic matrix to obtain the low-frequency bandgaps of out-of-plane modes. Numerical simulation is carried out to validate the heat and elastic characteristics of the spiral-multilayered anisotropic structure and reveal the effects of the laying angle and temperature on the bandgaps. Subsequently, a spiral-multilayered plate with periodic structures is studied, which shows an obvious vibration attenuation in the frequency ranges of the bandgaps and a deflected heat flux from the initial propagation direction. In the experimental investigation, the multi-phase spiral-multilayered anisotropic plate is simplified to a single-phase anisotropic plate made of aluminum. The characteristics of this type of anisotropic phononic crystal structure may pave the way for the design of a new kind of thermo-acoustic metamaterial serving in combined thermal and acoustic environments.     

多振子声子晶体的低频特性研究

本文设计了一种由硅橡胶包覆层包裹4个钨振子的新型声子晶体结构,通过有限元法计算该结构的色散曲线、振动模态和传输损失谱。结果表明,该结构的带隙范围为18.85~225.28 Hz,与传输损失谱频率衰减范围相吻合,能够有效抑制20~200 Hz的弹性波在声子晶体中传播。通过分析色散曲线上点的振动模态,说明带隙产生的原因。本文讨论了声子晶体板的缺口角度和振子之间的纵向和横向间距对带隙的影响,结果表明:当缺口角度减小时,带隙下边界几乎保持不变,带隙上边界升高从而增加了带隙的宽度;振子之间横向或纵向间距增大时,带隙下边界和上边界均上升,带隙变宽,进而优化了声子晶体模型的带隙。同时声子晶体板的缺口设计能够节省材料,从而减轻结构的质量。     

Interlayer interaction mechanism and its regulation on optical properties of bilayer SiCNSs

Silicon carbide nanosheets (SiCNSs) have a very broad application prospect in the field of new two-dimensional (2D) materials. In this paper, the interlayer interaction mechanism of bilayer SiCNSs (BL-SiCNSs) and its effect on optical properties are studied by first principles. Taking the charge and dipole moment of the layers as parameters, an interlayer coupling model is constructed which is more convenient to control the photoelectric properties. The results show that the stronger the interlayer coupling, the smaller the band gap of BL-SiCNSs. The interlayer coupling also changes the number of absorption peaks and causes the red or blue shift of absorption peaks. The strong interlayer coupling can produce obvious dispersion and regulate the optical transmission properties. The larger the interlayer distance, the smaller the permittivity in the vertical direction. However, the permittivity of the parallel direction is negative in the range of 150-300 nm, showing obvious metallicity. It is expected that the results will provide a meaningful theoretical basis for further study of SiCNSs optoelectronic devices.     

Superb thermal stability purple-blue phosphor through synergistic effect of emission compensation and nonradiative transition restriction of Eu2+

Phosphors with outstanding luminescence thermal stability are desirable for high-power phosphor-converted light-emitting diode (pc-LED) lightings. High structural rigidity and large bandgap of phosphor hosts are helpful to suppress nonradiative relaxation of optical centers and realize excellent thermal stability. Unfortunately, few host materials simultaneously possess aforementioned structural features. Herein, we confirm that Sr₃(PO₄)₂ (SPO) phosphate possesses high structural rigidity (Debye temperature, Θ_D = 559 K) and large bandgap (E_g = 8.313 eV) by density functional theory calculations. As expected, Eu²⁺-doped SPO purple-blue phosphors show extraordinary thermal stability. At 150/300 °C, SPO:5%Eu²⁺ presents emission loss of only 4%/8% and a predicated ultrahigh thermal quenching temperature of 973 °C. The most strikingly discoveries here are that thermal-induced emission compensation appears within two distinct Eu²⁺ sites of SPO host. The outstanding thermal stability, on one hand, is attributed to rigid structure and large bandgap of host that inhibits nonradiative relaxation of Eu²⁺ and on the other hand, the emission self-compensation of Eu²⁺. Benefiting from synergistic effect of emission compensation and nonradiative transition restriction of Eu²⁺, as-prepared SPO:5%Eu²⁺ purple-blue phosphor not only presents superior thermal stability but also high internal quantum efficiency of 95.1% and excellent hydrolysis resistant. Some advanced applications are explored including white LED lighting and wide-color-gamut display. Our work provides in-deep insights into structure-property relationships of thermally stable phosphors.     

Changes in the physical properties of low bandgap polymer after interaction with ionic liquids

Over the past few years, polymers shown comprehensive utilization in optical devices, solar cells, sensors, and other such devices. However, the efficiency of these devices remains a problem. We have synthesized new thiophene based, lowband gap polymer, poly(2-heptadecyl-4-vinylthieno[3,4-d] [1,3] selenazole) (PHVTS) and investigated the interactions between the PHVTS and ionic liquids (ILs), in this study. We have used imidazolium- and ammonium-family ILs, and studied the interactions using various spectroscopic techniques such UV–visible, FTIR, and confocal Raman spectroscopies. Additionally, we studied surface morphology of the polymer-IL film. Spectroscopic studies show that both families of ILs can interact with the newly synthesized polymer poly(2-heptadecyl-4-vinylthieno[3,4-d] [1,3] selenazole). However, the imidazolium-family Ionic Liquid-polymer (IL-polymer) mixture films show higher conductivities than ammonium-family IL–polymer mixture films.     

Beyond Donor–Acceptor (D–A) Approach: Structure–Optoelectronic Properties—Organic Photovoltaic Performance Correlation in New D–A1–D–A2 Low‐Bandgap Conjugated Polymers

Low‐bandgap near‐infrared polymers are usually synthesized using the common donor–acceptor (D–A) approach. However, recently polymer chemists are introducing more complex chemical concepts for better fine tuning of their optoelectronic properties. Usually these studies are limited to one or two polymer examples in each case study so far, though. In this study, the dependence of optoelectronic and macroscopic (device performance) properties in a series of six new D–A₁–D–A₂ low bandgap semiconducting polymers is reported for the first time. Correlation between the chemical structure of single‐component polymer films and their optoelectronic properties has been achieved in terms of absorption maxima, optical bandgap, ionization potential, and electron affinity. Preliminary organic photovoltaic results based on blends of the D–A₁–D–A₂ polymers as the electron donor mixed with the fullerene derivative [6,6]‐phenyl‐C₇₁‐butyric acid methyl ester demonstrate power conversion efficiencies close to 4% with short‐circuit current densities (J _sc) of around 11 mA cm⁻², high fill factors up to 0.70, and high open‐circuit voltages (V _ocs) of 0.70 V. All the devices are fabricated in an inverted architecture with the photoactive layer processed in air with doctor blade technique, showing the compatibility with roll‐to‐roll large‐scale manufacturing processes.