InAs 单量子点中级联辐射光子的关联测量

利用分子束外延生长InAs单量子点样品,温度为5 K时,测量了单量子点中单、双激子自发辐射的荧光(PL)光谱.研究了单、双激子发光强度随激发功率的变化及对应发光峰的偏振特性和精细结构劈裂.基于Hanbury-Brown Twiss(HBT) 实验,测量了单、双激子间发光光谱的关联函数,证实了其发光过程为级联发射过程. 关键词： InAs 单量子点 单、双激子 荧光光谱 级联辐射     

Total syntheses of (+)- and (−)-1,3,4,5-tetragalloylapiitol and revision of absolute configuration of naturally occurring (−)-1,3,4,5-tetragalloylapiitol

The total syntheses of (+)- and (−)-1,3,4,5-tetragalloylapiitol were achieved in seven steps from d- and l-ribose, respectively. By comparing the optical rotations of both enantiomers with those of the natural product, the absolute configuration at C-3 in the naturally occurring 1,3,4,5-tetragalloylapiitol has been revised to R. The absolute configurations at C-3 in the synthetic (+)- and (−)-1,3,4,5-tetragalloylapiitol were further confirmed by the circular dichroism exciton chirality method.     

Assessment of TD-DFT- and TD-HF-based approaches for the prediction of exciton coupling parameters, potential energy curves, and electronic characters of electronically excited aggregates

The reliability of linear response approaches such as time-dependent Hartree-Fock (TD-HF) and time-dependent density functional theory (TD-DFT) for the prediction of the excited state properties of 3,4;9,10-tetracarboxylic-perylene-bisimide (PBI) aggregates is investigated. A dimer model of PBI is investigated as a function of a torsional motion of the monomers, which was shown before to be an important intermolecular coordinate in these aggregates. The potential energy curves of the ground state and the two energetically lowest neutral excited and charge-transfer (CT) states were obtained with the spin-component scaling modification of the approximate coupled-cluster singles-and-doubles (SCS-CC2) method as a benchmark for dispersion corrected TD-HF and a range of TD-DFT approaches. The highly accurate SCS-CC2 results are used to assess the other, computationally less demanding methods. TD-HF predicts similar potential energy curves and transition dipole moments as SCS-CC2, as well as the correct order of neutral and CT states. This supports an exciton trapping mechanism, which was found on the basis of TD-HF data. However, the investigated TD-DFT methods provide generally the opposite character for the excited states. As a consequence, these TD-DFT results have unacceptably large errors for optical properties of these dye aggregates.     

Exciton luminescence and many-body effect of monolayer WS2 at room temperature

Monolayer transition metal dichalcogenides favor the formation of a variety of excitonic quasiparticles, and can serve as an ideal material for exploring room-temperature many-body effects in two-dimensional systems. Here, using mechanically exfoliated monolayer WS₂ and photoluminescence (PL) spectroscopy, exciton emission peaks are confirmed through temperature-dependent and electric-field-tuned PL spectroscopy. The dependence of exciton concentration on the excitation power density at room temperature is quantitatively analyzed. Exciton concentrations covering four orders of magnitude are divided into three stages. Within the low carrier concentration stage, the system is dominated by excitons, with a small fraction of trions and localized excitons. At the high carrier concentration stage, the localized exciton emission from defects coincides with the emission peak position of trions, resulting in broad spectral characteristics at room temperature.     

Comparison of the electronic structure of different perylene‐based dye‐aggregates

Aggregates of functionalized polycyclic aromatic molecules like perylene derivatives differ in important optoelectronic properties such as absorption and emission spectra or exciton diffusion lengths. Although those differences are well known, it is not fully understood if they are caused by variations in the geometrical orientation of the molecules within the aggregates, variations in the electronic structures of the dye aggregates or interplay of both. As this knowledge is of interest for the development of materials with optimized functionalities, we investigate this question by comparing the electronic structures of dimer systems of representative perylene‐based chromophores. The study comprises dimers of perylene, 3,4,9,10‐perylene tetracarboxylic acid bisimide (PBI), 3,4,9,10‐perylene tetracarboxylic acid dianhydride (PTCDA), and diindeno perylene (DIP). Potential energy curves (PECs) and characters of those electronic states are investigated which determine the optoelectronic properties. The computations use the spin‐component‐scaled approximate coupled‐cluster second‐order method (SCS‐CC2), which describes electronic states of predominately neutral excited (NE) and charge transfer (CT) character equally well. Our results show that the characters of the excited states change significantly with the intermolecular orientation and often represent significant mixtures of NE and CT characters. However, PECs and electronic structures of the investigated perylene derivatives are almost independent of the substitution patterns of the perylene core indicating that the observed differences in the optoelectronic properties mainly result from the geometrical structure of the dye aggregate. It also hints at the fact that optical properties can be computed from less‐substituted model compounds if a proper aggregate geometry is chosen. © 2012 Wiley Periodicals, Inc.     

有机高分子链内的场致激子解离

基于SSH(Su-Schrieffer-Heeger)模型,采用静态及动力学自洽算法模拟了有机高分子链内激子在光激发及外电场作用下的形成与解离过程。结果表明,受光激发后,有机高分子链内激子的生成与解离密切依赖于施加外电场的时机,当外电场与光激发同时发生时,激子能否生成完全取决于电场强度的大小;而当外电场在光激发后的一段时间(通常为皮秒量级)之后被引入,则在有机高分子链内能够形成稳定的激子,且该激子只有在强外电场(超过1MV/cm)的作用下,才会发生解离,临界场强量级与实验结果相符合。     

闪锌矿GaN/AlGaN量子点中激子态及光学性质的研究

在有效质量近似的框架下,运用变分方法研究闪锌矿GaN/AlGaN量子点中的激子态及相关光学性质,探讨电子与空穴在量子点中的三维空间受限和有限势效应.数值计算结果显示,当量子点的尺寸增加时, 量子尺寸效应对电子和空穴的影响减弱,基态激子结合能和带间光跃迁能也都降低;而当该量子点中垒层AlGaN中 Al含量增加时,提高了量子点对电子和空穴的束缚作用, 同时基态激子结合能和带间光跃迁能都增加.数值的理论结果与相关实验测量结果一致.     

Modifying optical properties of ZnO nanowires via strain-gradient

We conduct systematical cathodolumiuescence study on red-shift of near-band-edge emission energy in elastic bent ZnO nanowires with diameters within the exciton diffusion length （- 200 nm） in liquid nitrogen temperature （81 K）. By charactering the emission spectra of the nanowires with different; local curvatures, we find a linear relationship between strain-gradient and the red-shift of near-band-edge emission photon energy, an elastic strain-gradient effect in semiconductor similar to the famous flexoelectric effect in liquid crystals. Our results provide a new route to understand the inhomogeneous strain effect on the energy bands and optical properties of semiconductors and should be useful for designing advanced nano-optoelectronic devices.     

异质结界面修饰对TiO2/P3HT杂化太阳电池光电性能的增强作用

采用水热法在F-SnO₂(FTO)导电玻璃上制备了一维TiO₂纳米棒阵列, 将一种两亲有机三苯胺染料M分子吸附在其表面, 进而旋涂有机聚合物聚3-己基噻吩P3HT, 构建结构为FTO/TiO₂/M/P3HT/PEDOT:PSS/Au的杂化太阳电池. 瞬态光电流谱反映在杂化电极中存在pn异质结. 接触角测试表明TiO₂表面吸附有机M分子后, 亲水性表面转变为疏水性表面, 利于与聚合物P3HT的进一步接触; 稳态荧光发射光谱表明经修饰的杂化电极的荧光发射强度降低, 由荧光衰减曲线拟合得到的荧光寿命降低, 说明在TiO₂与P3HT之间存在有效的电荷转移, 电荷复合被抑制. 电化学阻抗分析表明界面修饰后电子复合电阻和电子寿命增大. 电池的特性参数均比界面修饰前有所提高, 光电转换效率为1.61%. 另外, 对该电池的工作机理、电荷传输过程进行了初步探讨.