Suppressing Strong Exciton–Phonon Coupling in Blue Perovskite Nanoplatelet Solids by Binary Systems

Quasi-two-dimensional (2D) perovskites are promising candidates for light generation owing to their high radiative rates. However, strong exciton–phonon interactions caused by mechanical softening of the surface act as a bottleneck in improving their suitability for a wide range of lighting and display applications. Moreover, it is not easily available to tune the phonon interactions in bulk films. Here, we adopt bottom-up fabricated blue emissive perovskite nanoplatelets (NPLs) as model systems to elucidate and as well as tune the phonon interactions via engineering of binary NPL solids. By optimizing component domains, the phonon coupling strength can be reduced by a factor of 2 driven by the delocalization of 2D excitons in out-of-plane orientations. It shows the picosecond energy transfer originated from the Förster resonance energy transfer (FRET) efficiently competes with the exciton–phonon interactions in the binary system.     

Redox Communication within Multinuclear Iron–Sulfur Complexes Related to Electronic Interplay in the Active Site of [FeFe]Hydrogenase

The one‐electron oxidations of a Fe₂ complex lead to the formation of a persistent metal‐stabilized thiyl radical Fe₂ species, mixed‐valent Fe₄, and Fe₈ complexes. The unpaired spin in the Fe₂ radical species delocalizes over the Fe₂ and the aromatic dithiolate, mostly on the terminal sulfur. The subsequent dimerization of the singly oxidized Fe₂ to the Fe₄ retains the partial thiyl radical character. For an analogue with less steric hindrance, the π–π stacking interaction between the dithiolato aromatic rings induces generation of the Fe₈, in which process electronic structures of the species are modulated through reducing the thiyl radical to the thiolate. Electronic reorganization repeats when the Fe₈ is converted to Fe₄. Electronic interplay in the complexes decreases the energy gap of frontier MOs and buffers electronic impacts upon redox events. Easier accessible redox potentials and increased stability of the species are facilitated. The results demonstrate that electronic versatility of the benzenedithiolate exerts pronounced influences on electronic and coordination structure of the metal complexes.     

Stereodivergent Desymmetrization of Simple Dicarboxylates via Branch-Selective Pd/Cu Catalyzed Allylic Substitution

Asymmetric desymmetrization has been demonstrated to be a powerful strategy for building stereocenters in asymmetric synthesis. Herein, a Pd/Cu catalyzed asymmetric desymmetrization reaction with a simple geminal dicarboxylate is reported. A wide scope of imino esters bearing an aryl or heteroaromatic group were compatible with this bimetallic catalytic system. The reactions proceeded smoothly, giving the desired products in good yields with high to excellent regio-, diastereo-, and enantioselectivity (up to 20 : 1 branched:linear, >20 : 1 dr, >99 % ee). Notably, the reaction favored branched selectivity, which is unusual for the Pd-catalyzed allylic alkylation reaction. In addition, the standard product could be easily transformed to other valuable molecules such as chiral allylic alcohols, carbamates, and organic boron compounds. Furthermore, DFT calculations were conducted to explain the origin of the branched selectivity.     

Extracellular Matrix Proteins Involved in Alzheimer's Disease

Alzheimer's disease (AD) is one of the most common neurodegenerative diseases and characterized by cognitive and memory impairments. Emerging evidence suggests that the extracellular matrix (ECM) in the brain plays an important role in the etiology of AD. It has been detected that the levels of ECM proteins have changed in the brains of AD patients and animal models. Some ECM components, for example, elastin and heparan sulfate proteoglycans, are considered to promote the upregulation of extracellular amyloid-beta (Aβ) proteins. In addition, collagen VI and laminin are shown to have interactions with Aβ peptides, which might lead to the clearance of those peptides. Thus, ECM proteins are involved in both amyloidosis and neuroprotection in the AD process. However, the molecular mechanism of neuronal ECM proteins on the pathophysiology of AD remains elusive. More investigation of ECM proteins with AD pathogenesis is needed, and this may lead to novel therapeutic strategies and biomarkers for AD.     

材料化学课程线上教学初探

2020新年伊始,新冠肺炎突然来袭,为了防止聚集性感染,教育部提出了"停课不停教、停课不停学"的要求。地方普通高校学生的自律性、自觉性及能动性差别十分明显,这样的学情对如何有效开展化学专业的线上教学工作提出了更大的挑战。本文以材料化学课程线上教学为例,介绍地方普通高校化学专业线上教学工作的开展情况。针对教学过程中遇到的各种问题和采用的应对方案,探讨线上教学过程中的注意事项。希望本文能为地方普通高校化学专业线上教学工作提供有益的参考。     

Non-perturbative positive Lyapunov exponent of Schrödinger equations and its applications to skew-shift mapping

We first study the discrete Schrödinger equations with analytic potentials given by a class of transformations. It is shown that if the coupling number is large, then the Lyapunov exponent equals approximately to the logarithm of this coupling number. When the transformation becomes the skew-shift mapping, we prove that the Lyapunov exponent is weak Hölder continuous, and the spectrum satisfies Anderson Localization and contains large intervals. Moreover, all of these conclusions are non-perturbative.     

基于特征正交分解的一类瞬态非线性热传导问题的新型快速分析方法

提出了一种基于特征正交分解(POD)和有限元法的瞬态非线性热传导问题的模型降阶快速分析方法, 建立了导热系数随温度变化的一类瞬态非线性热传导问题有限元格式的POD降阶模型. 在隐式时间推进方法的基础上有效结合单元预转换方法和多级线性化方法发展了一种加速求解瞬态非线性热传导降阶模型的新型计算方法,并通过二维和三维算例验证了该方法的准确性和高效性. 研究结果表明: (1)降阶模型解的均方根误差在经过初始时段轻微的脉动后稳定于0.01%以下, 而其计算效率比有限元全阶模型提高2$\sim $3个数量级, 并且自由度数量(DOFs)愈大提高的幅度也愈加显著; (2)新型算法解决了常规算法在计算非线性降阶模型时加速性能差的问题, 即使是在DOFs比较小的时候也能够明显提高计算效率; (3)常数边界条件下得到的POD模态可以用来建立相同求解域在各种复杂时变边界条件下的瞬态非线性热传导降阶模型, 并对其传热过程和温度场进行快速准确的分析与预测, 具有很好的工程应用价值.      

金属导体电阻温度系数实验数据处理方法的比较

基于金属导体电阻温度系数实验数据的特点,我们采用三种不同的数据处理方法:逐差法、最小二乘法和Origin绘图,对实验数据进行了分析处理,并且将三种方法在处理实验数据时的特点做了对比分析。根据我们的分析发现,将Origin应用到大学物理实验教学的数据处理中,不仅能够简单、快捷地完成数据的统计、分析和曲线拟合,而且有利于帮助学生掌握物理规律,更好地提高物理实验教学的效果。