CdTe量子点-铜酞菁复合体系荧光共振能量转移的研究

以波长为780 nm、重复频率为76 MHz、脉宽为130 fs的飞秒激光作为激发光源, 采用超快时间分辨光谱技术研究了CdTe量子点-铜酞菁复合体系的荧光共振能量转移. 实验结果表明, 在780 nm的双光子激发条件下, 复合体系中CdTe量子点的荧光寿命随着铜酞菁溶液浓度的增加而减少, 荧光共振能量转移效率增加. 同时也研究了激发功率对荧光共振能量转移效率的影响. 结果表明, 随着激发光功率的增加, 复合体系溶液中CdTe量子点的荧光寿命增加, 荧光共振能量转移效率减小, 其物理机理是因为高激发功率下的热效应和由双光子诱导的高阶激发态的跃迁. 当激发光功率为200 mW时, 双光子荧光共振能量转移效率为43.8%. 研究表明CdTe量子点-铜酞菁复合体系是非常有潜力的第三代光敏剂.     

Spectral characteristics of luminescence of solutions of complex molecules under conditions of electronic excitation transfer to a saturable acceptor in the case of inhomogeneous broadening of electronic energy levels

Spectral characteristics of solutions of complex molecules under conditions of inhomogeneous broadening of energy levels are considered in the case when the nonlinear dependence of the population of molecular states on the excitation intensity is determined not by saturation of molecular levels but by exchange of the electronic excitation energy with the environment. Calculations have shown that the dependence of the position of the fluorescence spectrum on the excitation frequency is nonmonotonic in solutions of the type and varies substantially with the excitation intensity. Belarusian State University, 4, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 64, No. 2, pp. 164–168, March–April, 1997.     

Electronic States and Photoprocesses in Bichromophore Systems

We present the results of quantumchemical investigation of energy transfer in organic molecules and systems and the inferences drawn. The Förster theory has been subjected to a critical analysis in order that the energy transfer could be described in the context of the current theory of nonradiative transitions and the incorrectness of the basic premises of the Förster theory has been demonstrated. A new variant of the mechanism of electronic energy transfer on the basis of the theory of electron transitions and of the quantum mechanics of molecules has been suggested. It is shown that the interaction of the molecules of the donor and acceptor perturbs the electronic states of isolated molecules even before the excitation of the donor molecule. A characteristic feature of the manifestation of intermolecular interaction is the spatial delocalization of the wave functions of the electronic states of interacting molecules, leading to the possibility of occurrence of conventional photophysical processes with participation of the electronic states of various molecules of the bimolecular system. In experimental investigations, the result of the intermolecular nonradiative transition is recorded as evidence of the spatial transfer of the energy of electronic excitation from the donor molecule to the acceptor molecule.     

Quantum Dynamics of Entanglement and Single Excitation Transfer in LH1-RC-Type Trimer

In this paper,we study quantum dynamics of entanglement and single excitation transfer(SET) in an LH1-RC-type trimer which can describe a basic unit cell in the LH1-RC complex in the photosynthetic process.It is shown that there exists a sudden change of entanglement at the critic point of quantum phase transition(QPT) of the system at low temperatures,the entanglement sudden change caused by the QPT is suppressed at higher temperatures.We investigate the influence of environment on entanglement and SET.We show the generation of the dephasing-assisted entanglement between a donor and an acceptor and the existence of the steady-state entanglement,and demonstrate the entanglement transfer from donor-donor entanglement to donor-acceptor entanglement in the dynamic evolution.We reveal the close relation between the SET probability and donor-acceptor entanglement.Especially,we find that the SET probability is proportional to the amount of donor-acceptor entanglement under certain conditions.     

有机多层量子阱的能量转移

采用多源有机分子气相沉积系统制备了不同类型的有机多量子阱结构,利用电化学循环伏安法和吸收光谱、荧光光谱研究了量子阱的类型、光致发光的特性.电化学循环伏安法和吸收光谱的测量结果表明,PBD/8-羟基喹啉铝(Alq₃)有机量子阱为Ⅰ型量子阱结构,NPB/Alq₃和BCP/Alq₃有机量子阱为Ⅱ型量子阱结构.荧光光谱的研究结果表明,PBD/Alq₃和BCP/Alq₃量子阱结构可以实现PBD,BCP向Alq₃能量完全转移,而NPB/Alq₃量子阱结构,NPB和Alq₃之间只是部分能量转移.文中对影响能量转移的因素进行了讨论.关键词：有机量子阱能量转移     

产生二步混合激发受激辐射的光延时效应研究

本文对双光束二步混合激发气体样品产生受激辐射的光延时效应进行了研究.通过三能级模型计算了激发能级上粒子数布居随时间的变化,并以实验进行验证.计算得到与实验值符合较好.     

一类有机发色团分子电子吸收跃迁能的计算研究

利用MINDO/3、MNDO、AM1以及PM3四种通用半经验量子化学计算方法和限制性多电子组态相互作用方法(MECI)并根据Onsager方程计算溶剂效应,成功地对9-氨基吖啶(AMAR)、9,10-二甲氧基-2-甲基蒽(DMAN)、9-甲基蒽(AN)、α-萘甲酸乙酯(NAAC)四种有机发色团分子的吸收跃迁能进行了理论计算,吸收跃迁能理论计算值与光谱实验测定值相关分析表明,它们具有相当好的相关系数,显示半经验量子化学方法可以作为预测有机发色团光谱性质的有效计算方法.     

LiYF4:Nd3+中脉冲光泵浦的上转换蓝光

本文报道利用578.4nm的脉冲光泵浦,在室温和77K下,观察到LiYF4:Nd3+单晶中的上转换蓝光。由发光强度与泵浦光强度平方的直线关系,确定此上转换过程是双光子过程.通过对吸收谱和激发谱以及衰减曲线的研究,确定其上转换激发机制为两步激发和能量传递上转换。     

利用信息流方法优化多激发自旋链中的量子态传输

研究了量子态在一条均匀耦合的反铁磁自旋链中传输时, 信道中自旋激发数变化对其传输性质的影响. 利用信息流方法分析输出端粒子的算符演化动力学, 获得了量子态传输的平均保真度与信道自旋初态之间的关系. 结果表明, 平均保真度的大小只依赖于信道中自旋激发数的奇偶性. 通过比较在奇偶激发信道中获得的最大平均保真度, 构建了优化信道来提升量子态在自旋链中的传输质量. 进一步分析了纠缠在激发信道中的传输情况, 发现纠缠的传输质量不仅和信道中自旋激发的具体个数有关, 还取决于激发自旋的初始排列. 特别地, 当信道中自旋无激发或全部激发时, 纠缠传输的大小和持续时间都优于其他的激发信道. 上述研究结果有助于在实际系统中搭建适合量子态和纠缠传输的量子信道.     

Assessment of a composite CC2/DFT procedure for calculating 0–0 excitation energies of organic molecules

The task to assess the performance of quantum chemical methods in describing electronically excited states has in recent years started to shift from calculation of vertical (ΔE_ve) to calculation of 0–0 excitation energies (ΔE₀₀). Here, based on a set of 66 excited states of organic molecules for which high-resolution experimental ΔE₀₀ energies are available and for which the approximate coupled-cluster singles and doubles (CC2) method performs particularly well, we explore the possibility to simplify the calculation of CC2-quality ΔE₀₀ energies using composite procedures that partly replace CC2 with more economical methods. Specifically, we consider procedures that employ CC2 only for the ΔE_ve part and density functional theory methods for the cumbersome excited-state geometry optimisations and frequency calculations required to obtain ΔE₀₀ energies from ΔE_ve ones. The results demonstrate that it is indeed possible to both closely (to within 0.06–0.08 eV) and consistently approximate ‘true’ CC2 ΔE₀₀ energies in this way, especially when CC2 is combined with hybrid density functionals. Overall, the study highlights the unexploited potential of composite procedures, which hitherto have found widespread use mostly in ground-state chemistry, to also play an important role in facilitating accurate studies of excited states.     

Tb3+、Yb3+共掺BaGd2ZnO5荧光粉的制备及其近红外量子剪裁研究

采用高温固相法合成了Tb3+、Yb3+共掺杂的BaGd2ZnO5荧光粉。XRD测量数据表明合成的样品为纯相。在Tb3+特征激发(297 nm)下得到了Yb3+的特征发射(977 nm),并且对Tb3+与Yb3+能级图进行分析,证明Tb3+到Yb3+为合作能量传递。测量了不同Yb3+浓度下Tb3+的5D4能级(544 nm)的发光寿命曲线,计算得到Tb3+与Yb3+的能量传递效率和量子效率,最高量子效率为125.5%。Yb3+的发射与硅太阳能电池的吸收匹配,该材料有可能应用于硅太阳能电池以提高其转换效率。