二苯胺取代吖啶衍生物发光材料的合成、表征及电致发光性能

设计合成了2个苯胺取代吖啶衍生物N3,N3,N6,N6-四苯基吖啶基-3,6-二胺(1)和N3,N3,N6,N6-四对甲苯基吖啶基-3,6-二胺(2),通过化学修饰在吖啶核的两端引入二苯胺取代基可以调节化合物的能级和堆积结构等性质,从而使这些吖啶衍生物具有良好的发光性能,可用于制备电致发光器件.基于吖啶衍生物为掺杂发光材料制备的电致发光器件均呈现绿光发射,器件开启电压较低(2.4 V),以化合物1和2制备的器件最高功率效率分别为4.9和8.2 lm/W.考察了其光物理、电化学、热学和荧光量子效率等性能.结果表明,化合物1和2具有较高的量子效率及匹配的能级结构,这是获得较高电致发光效率的基础.     

Single‐Molecule Methods to Study Membrane Receptor Oligomerization

Membrane receptors control fundamental cellular processes. Binding of a specific ligand to a receptor initiates communication through the membrane and activation of signaling cascades. This activation process often leads to a spatial rearrangement of receptors in the membrane at the molecular level. Single‐molecule techniques contributed significantly to the understanding of receptor organization and rearrangement in membranes. Here, we review four prominent single‐molecule techniques that have been applied to membrane receptors, namely, stepwise photobleaching, Förster resonance energy transfer, sub‐diffraction localization microscopy and co‐tracking. We discuss the requirements, benefits and limitations of each technique, discuss target labeling, present a selection of applications and results and compare the different methodologies.     

Forced Folding of a Disordered Protein Accesses an Alternative Folding Landscape

Intrinsically disordered proteins (IDPs) are involved in diverse cellular functions. Many IDPs can interact with multiple binding partners, resulting in their folding into alternative ligand‐specific functional structures. For such multi‐structural IDPs, a key question is whether these multiple structures are fully encoded in the protein sequence, as is the case in many globular proteins. To answer this question, here we employed a combination of single‐molecule and ensemble techniques to compare ligand‐induced and osmolyte‐forced folding of α‐synuclein. Our results reveal context‐dependent modulation of the protein′s folding landscape, suggesting that the codes for the protein′s native folds are partially encoded in its primary sequence, and are completed only upon interaction with binding partners. Our findings suggest a critical role for cellular interactions in expanding the repertoire of folds and functions available to disordered proteins.     

Dissecting Cooperative Communications in a Protein with a High‐Throughput Single‐Molecule Scalpel

Miscued communication often leads to misfolding and aggregation of the proteins involved in many diseases. Owing to the ensemble average property of conventional techniques, detailed communication diagrams are difficult to obtain. Mechanical unfolding affords an unprecedented perspective on cooperative transitions by observing a protein along a trajectory defined by two mutated cysteine residues. Nevertheless, this approach requires tedious sample preparation at the risk of altering native protein conformations. To address these issues, we applied click chemistry to tether a protein to the two dsDNA handles through primary amines in lysine residues as well as at the N terminus. As a proof of concept, we used laser tweezers to mechanically unfold and refold calmodulin along 36 trajectories, maximally allowed by this strategy in a single batch of protein preparation. Without a priori knowledge of the particular residues to which the double‐stranded DNA handles attach, we used hierarchical cluster analysis to identify 20 major trajectories, according to the size and the pattern of unfolding transitions. We dissected the cooperativity into all‐or‐none and partially cooperative events, which represent strong and weak high‐order interactions in proteins, respectively. Although the overall cooperativity is higher within the N or C lobe than that between the lobes, the all‐or‐none cooperativity is anisotropic among different the unfolding trajectories and becomes relatively more predominant when the size of the protein segments increases. The average cooperativity for all‐or‐none transitions falls within the expected range observed by ensemble techniques, which supports the hypothesis that unfolding of a free protein can be reconstituted from individual trajectories.     

Dark‐Field‐Based Observation of Single‐Nanoparticle Dynamics on a Supported Lipid Bilayer for In Situ Analysis of Interacting Molecules and Nanoparticles

Observation of single plasmonic nanoparticles in reconstituted biological systems allows us to obtain snapshots of dynamic processes between molecules and nanoparticles with unprecedented spatiotemporal resolution and single‐molecule/single‐particle‐level data acquisition. This Concept is intended to introduce nanoparticle‐tethered supported lipid bilayer platforms that allow for the dynamic confinement of nanoparticles on a two‐dimensional fluidic surface. The dark‐field‐based long‐term, stable, real‐time observation of freely diffusing plasmonic nanoparticles on a lipid bilayer enables one to extract a broad range of information about interparticle and molecular interactions throughout the entire reaction period. Herein, we highlight important developments in this context to provide ideas on how molecular interactions can be interpreted by monitoring dynamic behaviors and optical signals of laterally mobile nanoparticles.     

Construction of Nitronyl Nitroxide‐Based 3d–4f Clusters: Structure and Magnetism

Three unprecedented nitronyl nitroxide radical‐bridged 3d–4f clusters, [Ln₂Cu₂(hfac)₁₀(NIT‐3py)₂(H₂O)₂](Ln^III=Y, Gd, Dy), have been obtained from the self‐assembly of Ln(hfac)₃, Cu(hfac)₂, and the radical ligand. The Dy complex shows a slow relaxation of magnetization, representing the first nitronyl nitroxide radical‐based 3d–4f cluster with single‐molecule magnet behavior.     

Investigating S-wave bound states composed of two pseudoscalar mesons

In this study, we systematically investigated two-pseudoscalar meson systems with the Bethe-Salpeter equation in the ladder and instantaneous approximations. By solving the Bethe-Salpeter equation numerically with the kernel containing the one-particle exchange diagrams, we found that the \begin{document}$ K\bar{K} $\end{document}, \begin{document}$ DK $\end{document}, \begin{document}$ B\bar{K} $\end{document}, \begin{document}$ D\bar{D} $\end{document}, \begin{document}$ B\bar{B} $\end{document}, \begin{document}$ BD $\end{document}, \begin{document}$ D\bar{K} $\end{document}, \begin{document}$ BK $\end{document}, and \begin{document}$ B\bar{D} $\end{document} systems with \begin{document}$ I=0 $\end{document} can exist as bound states. We also studied the contributions from heavy meson (\begin{document}$ J/\psi $\end{document} and \begin{document}$\Upsilon $\end{document}) exchanges and found that the contributions from heavy meson exchanges cannot be ignored.     

基于吡嗪空穴传输层的合成及在p-i-n型钙钛矿太阳能电池中的应用

钙钛矿太阳能电池由于具有高的光电转换效率,简单的溶液加工工艺,较低的成本等优势因而拥有广阔的应用前景。有机小分子空穴传输层材料在钙钛矿太阳能电池中扮演着极其重要的角色。在本工作中,我们设计和合成了基于吡嗪为分子中心核,三苯胺为分枝的X型空穴传输层材料PT-TPA。与Si-OMeTPA对比,吡嗪的引入不仅不会影响其结晶性,并且能够改善其电荷转移特性和分子中心共平面性,从而显著提升了PT-TPA的空穴迁移率。在非掺杂的情况之下,基于PT-TPA空穴传输层的p-i-n型钙钛矿太阳能电池展现出17.52%的光电转换效率,与相同条件下基于Si-OMeTPA空穴传输层的器件相比,效率提高了近15%。     

Development of bioorthogonal SERS imaging probe in biological and biomedical applications

Living-cell imaging demands high specificity,sensitivity,and minimal background interference to the targets of interest.However,developing a desirable imaging probe that can possess all the above features is still challenging.The bioorthogonal surface-enhanced Raman scattering(SERS) imaging has been recently emerged through utilizing Raman reporters with characteristic peaks in Raman-silent region of cells(1800-2800 cm~(-1)),which opens a revolutionary avenue for living-cell imaging with multiplexing capability.In this review,we focus on the recent advances in the technology development and the biological and biomedical applications of the living-cell bioorthogonal SERS imaging technique.After introduction of fundamental principles for bioorthogonal tag or label,we present applications for visualization of various intracellular components and environment including proteins,nucleic acids,lipids,pH and hypoxia,even for cancer diagnosis in tissue samples.Then,various bioorthogonal SERS imaging-guided thera py strategies have been discussed such as photothera py and surge ry.In conclusion,this strategy has great potential to be a flexible and robust tool for visualization detection and diseases diagnosis.     

17O-核磁共振法研究不同处理方法对液态水缔合结构的影响

水作为人类重要的生产要素,参与了卷烟生产的多个环节。水在自然条件下以分子簇的形式存在,多种处理方式可以改变水分子团簇的大小。本文以¹⁷O-核磁共振法为水分子团簇的表征手段,以自来水为水源,考察了氢气、远红外辐射陶瓷球、反渗透、磁场四种处理方法对水分子簇的影响。结果表明:四种处理方式均能使一定量水分子由氢键结合态变为自由态,从而使水分子簇变小。不同处理方法对液态水缔合结构的影响大小排序为氢气处理>远红外陶瓷球处理>反渗透处理>磁场处理。同时,对氢气处理效果的时效性进行了考察,随着放置时间增加,部分自由态水分子再次转变为氢键结合态,水分子簇尺寸变大,但三天后仍保留了一定处理效果。本研究表明氢气处理为四种处理方式中最优的水处理方式,具有提升烟草行业生产用水品质的潜在应用价值。