阻尼最小二乘算法CARS光谱温度拟合

为了解决相干反斯托克斯喇曼散射（CARS）光谱CARSFT计算程序在温度拟合过程中,对初值依赖大、测量光谱信噪比差、不易收敛的问题,通过分析非线性迭代算法,采用了阻尼最小二乘算法对氮气CARS光谱进行温度拟合。针对CARS理论光谱计算公式较为复杂的特点,采用数值差分的方式来获得迭代计算时所需要的设计矩阵。分析了横向偏移、纵向偏移和温度三个主要参量对拟合残差的影响,发现纵向偏移的初值设置对温度拟合影响较大。拟合温度2000 K时的标准理论CARS光谱,设置偏离较大的初始值,采用阻尼最小二乘法获得了较好的结果。迭代计算167步后,温度拟合为2 005.6 K,残差为0.027 463。拟合光谱信噪比较差的CARS光谱,阻尼最小二乘法也能稳定收敛。结果验证了阻尼最小二乘法对初值的依赖不大,并且当拟合谱信噪比较差时也能收敛,可用于在恶劣环境下CARS测量光谱的拟合。     

0.4 THz回旋行波管的设计与模拟

利用三维粒子模拟仿真软件,对共焦波导结构的0.4 THz回旋行波管进行了注波互作用的模拟研究。以共焦波导的冷腔色散以及衍射损耗入手,最终选定HE06模作为互作用工作模式。为了对寄生振荡进行抑制,在互作用结构中引入了截断。在模拟过程中,通过调节束压、束流、工作磁场、电子束横纵速度比,得到了最优的工作参数。最终,在束压34 kV、磁场14.25、束流2 A、横纵速度比0.75的工作参数下,当输入信号为1 W时,得到了最高2.76 kW的功率输出,增益超过34 dB,3 dB带宽为8 GHz,效率达到4%。     

超薄前投激光显示系统研制

为了解决光学系统投影厚度过大问题,采用自由曲反射面结合非球面设计方法设计出超短距离、超广角投影显示系统,其屏幕投影距离小于20 cm。为解决激光色域系统转换,建立了激光三基色与荧光粉三基色色域变换与扩展的理论模型并搭建了基于DSP高速图像处理芯片为核心的颜色变化实时硬件处理试验开发系统。通过该系统可以调试不同颜色系统转换算法,验证转换模型的正确性,并为实现专用颜色转模块提供了开发平台。     

基于天文观测的相机标定及姿态测量技术研究

为利用相机进行天文观测以实现高精度的相机姿态测量,必须先对相机参数进行精确标定。针对传统相机标定方法工作距离有限的问题,提出了以恒星为控制点的相机标定方法,根据球面天文学方法计算观测时刻控制点的世界坐标,利用摄像测量原理建立了恒星观测模型,求解相机的内外参数并分析了误差因素。实验结果表明,该标定方法在不依赖于精密、复杂的外部设备情况下可达到较高精度,并具有较强的抗噪声能力。将标定结果用于天文观测并求解相机姿态,航向角和俯仰角的解算重复性优于10″,能够满足高精度姿态测量的需求。该方法可进一步推广应用于星敏感器的标定。     

Unveiling the Layer‐Dependent Catalytic Activity of PtSe2 Atomic Crystals for the Hydrogen Evolution Reaction

Two‐dimensional (2D) PtSe₂ shows the most prominent layer‐dependent electrical properties among various 2D materials and high catalytic activity for hydrogen evolution reaction (HER), and therefore, it is an ideal material for exploring the structure–activity correlations in 2D systems. Here, starting with the synthesis of single‐crystalline 2D PtSe₂ with a controlled number of layers and probing the HER catalytic activity of individual flakes in micro electrochemical cells, we investigated the layer‐dependent HER catalytic activity of 2D PtSe₂ from both theoretical and experimental perspectives. We clearly demonstrated how the number of layers affects the number of active sites, the electronic structures, and electrical properties of 2D PtSe₂ flakes and thus alters their catalytic performance for HER. Our results also highlight the importance of efficient electron transfer in achieving optimum activity for ultrathin electrocatalysts. Our studies greatly enrich our understanding of the structure–activity correlations for 2D catalysts and provide new insight for the design and synthesis of ultrathin catalysts with high activity.     

Enantioselective Total Synthesis of Pseudopteroxazole and Ileabethoxazole

Enantioselective total syntheses of pseudopteroxazole ( 1 ) and ileabethoxazole ( 2 ) are presented. The two original stereocenters were constructed in excellent enantioselectivity and good diastereoselectivity through Carreira's asymmetric dual catalytic allylation, which shows potential for accessing diastereoisomers at C2 and C3 of 1 and 2 . Cationic cyclizations of 13 and 24 demonstrated an effective pathway for the construction of the opposite configurations at C1 in 1 and 2 . Additionally, an approach for the introduction of methyl at C4 is a feasible solution for structural modifications at C4 in 1 and 2 .     

High Uptake of ReO4− and CO2 Conversion by a Radiation‐Resistant Thorium–Nickle [Th48Ni6] Nanocage‐Based Metal–Organic Framework

Assembled from [Th₄₈Ni₆] nanocages, the first transition‐metal (TM)‐thorium metal–organic framework (MOF, 1 ) has been synthesized and structurally characterized. 1 exhibits high solvent and acid/base stability, and resistance to 400 kGy β irradiation. Notably, 1 captures ReO₄^? (an analogue of radioactive ⁹⁹TcO₄^?, a key species in nuclear wastes) with a maximum capacity of 807 mg g^?1, falling among the largest values known to date. Furthermore, 1 can enrich methylene blue (MB) and can also serve as an effective and recyclable catalyst for CO₂ fixation with epoxides; there is no significant loss of catalytic activity after 10 cycles. Theoretical studies with nucleus‐independent chemical shifts and natural bond orbital analysis reveal that the [Th₆O₈] clusters in 1 have a unique stable electronic structure with (d–p)π aromaticity, partially rationalising 1 ′s stability.     

Stereoselective Synthesis of Trisubstituted Vinylboronates from Ketone Enolates Triggered by 1,3‐Metalate Rearrangement of Lithium Enolates

An unprecedented stereoselective synthesis of trisubstituted vinylboronates is reported to proceed by direct borylation of lithium ketone enolates under transition‐metal‐free conditions. The stereospecific C?O borylation of lithium enolates was triggered by a carbonyl‐induced 1,3‐metalate rearrangement via a C‐bound boron enolate. DFT calculations and control experiments revealed that the stereoselectivity is controlled by sterics. A variety of stereospecific trisubstituted vinylboronates, together with several tetrasubstituted vinylboronates, were conveniently synthesized with the newly developed methodology. Based on the transformation of stereospecific vinylboronate, a single isomer of Dienestrol was efficiently obtained.     

One-step synthesis of magnetic composite UiO-66/Fe3O4/GO for the removal of radioactive cesium ions

Journal of Radioanalytical and Nuclear Chemistry - In this study, the UiO-66/Fe3O4/GO composite was prepared by one step method for removal of cesium ions (Cs+) in water and exhibited excellent...