Excitation energy transfer in chromophore aggregates within a dissipative medium

The Redfield theory-based model of excitation energy transfer in chromophore ensembles within dissipative environment is proposed. Application of the multipole expansion to an operator of interaction between the chromophore molecules and the environment together with some assumptions about the latter led to the closed-form expressions for the elements of the dissipation tensor. These expressions relate the rates of transition between eigenstates of a chromophore ensemble with the spectral and electronic properties of an environment and the chromophore molecules. For several model cases the exact solution of the Redfield equations was obtained.     

Influence of the redox state of QA on phycobilisome mobility in the cyanobacterium Synechocystis sp. strain PCC 6803

In a unicellular cyanobacterium, the mobile fraction of phycobilisome (PBS) was found to be maximum at a particular redox value of Q_A (i.e., 0.52). An upward or downward shift in the redox value leads to a decrease in this mobile fraction of PBS. Furthermore, the regulatory effect of the redox state of Q_A on PBS mobility was found to be independent of the effect exerted by the plastoquinone pool. These findings indicate for the first time that PBS mobility is regulated by the Q_A redox state in cyanobacteria. A possible working mechanism underlying this control is discussed.     

氢分子振动态与铯分子基态碰撞中转动-振动能量转移

利用受激拉曼泵浦将H2激发到v=1,J=3态,研究了H2(1, 3)态与Cs2分子碰撞(1, 3)态的弛豫及Cs2(X1+g)振动态的激发过程。利用相干反斯托克斯拉曼散射(CARS)检测H2的振转态分布,由CARS峰值得到密度比[H2(1, 3)]/[H2(0, 3)]和[H2(1, 1)]/[H2(1, 3)],由H2(v=0)振转态的Boltzmann分布确定H2(0, 3)的密度,由此得到[H2(1, 3)]和[H2(1, 1)]态的密度。激光诱导荧光光谱(LIF)确定被碰撞激发的Cs2(X1+g, v=11-15)各态。利用单模半导体激光作瞬时光吸收,对于v= 11, 12, 13, 14和15,积分吸收系数(单位：106cm-1s-1)分别是6.5,7.9,7.0,6.1和4.7,结合H2(1, 3)的密度,得到H2(1, 3)Cs2(X1+g, v)的转移速率系数,对于v=11-15,分别是(单位：10-13cm-1s-1)1. 40. 6,1.70. 7,1.50. 6,1.30.5和1.00. 4。利用吸收线Doppler增宽测量分别得到了Cs2(X1+g, v=11-15)的平动能。     

氢分子振动态与铯分子基态碰撞中转动-振动能量转移

利用受激拉曼泵浦将H2激发到v=1,J=3态,研究了H2(1, 3)态与Cs2分子碰撞(1, 3)态的弛豫及Cs2(X1+g)振动态的激发过程。利用相干反斯托克斯拉曼散射(CARS)检测H2的振转态分布,由CARS峰值得到密度比[H2(1, 3)]/[H2(0, 3)]和[H2(1, 1)]/[H2(1, 3)],由H2(v=0)振转态的Boltzmann分布确定H2(0, 3)的密度,由此得到[H2(1, 3)]和[H2(1, 1)]态的密度。激光诱导荧光光谱(LIF)确定被碰撞激发的Cs2(X1+g, v=11-15)各态。利用单模半导体激光作瞬时光吸收,对于v= 11, 12, 13, 14和15,积分吸收系数(单位：106cm-1s-1)分别是6.5,7.9,7.0,6.1和4.7,结合H2(1, 3)的密度,得到H2(1, 3)Cs2(X1+g, v)的转移速率系数,对于v=11-15,分别是(单位：10-13cm-1s-1)1. 40. 6,1.70. 7,1.50. 6,1.30.5和1.00. 4。利用吸收线Doppler增宽测量分别得到了Cs2(X1+g, v=11-15)的平动能。     

Efficient wireless non-radiative mid-range energy transfer

We investigate whether, and to what extent, the physical phenomenon of long-lifetime resonant electromagnetic states with localized slowly-evanescent field patterns can be used to transfer energy efficiently over non-negligible distances, even in the presence of extraneous environmental objects. Via detailed theoretical and numerical analyses of typical real-world model-situations and realistic material parameters, we establish that such a non-radiative scheme can lead to “strong coupling” between two medium-range distant such states and thus could indeed be practical for efficient medium-range wireless energy transfer.     

基于Metglas/PFC磁电层状复合材料的电能无线传输系统

本文完整推导了无直流偏磁条件下, 磁致伸缩材料和压电材料黏接而得的磁电层状复合材料输出电压、电流、磁电系数表达式, 制备了多个样品并实现了电能无线传输系统. 对样品的测试结果验证了理论分析的正确性. 进一步试验结果表明: 磁电层状复合材料的输出具有倍频特性, 材料长度与谐振频率成反比, 谐振状态下样品可在20 Oe的磁场中输出接近100 V (有效值)开路电压, 样品最大传输功率为520 mW (此为该传输方式下公开报道的最大功率), 功率密度为1.21 W/cm³, 样品最大传输效率达35%, 30°以内的偏转角度对材料的输出无显著影响. 试验结果表明, 基于Metglas/PFC磁电层状复合材料是小体积、 小功率、 对传输效率不甚敏感的电能无线传输应用的一种非常有前景的实现方式. 关键词： 磁电复合材料 无线能量传输     

Phonon-assisted excitation energy transfer in photosynthetic systems

The phonon-assisted process of energy transfer aiming at exploring the newly emerging frontier between biology and physics is an issue of central interest.This article shows the important role of the intramolecular vibrational modes for excitation energy transfer in the photosynthetic systems.Based on a dimer system consisting of a donor and an acceptor modeled by two two-level systems,in which one of them is coupled to a high-energy vibrational mode,we derive an effective Hamiltonian describing the vibration-assisted coherent energy transfer process in the polaron frame.The effective Hamiltonian reveals in the case that the vibrational mode dynamically matches the energy detuning between the donor and the acceptor,the original detuned energy transfer becomes resonant energy transfer.In addition,the population dynamics and coherence dynamics of the dimer system with and without vibration-assistance are investigated numerically.It is found that,the energy transfer efficiency and the transfer time depend heavily on the interaction strength of the donor and the high-energy vibrational mode,as well as the vibrational frequency.The numerical results also indicate that the initial state and dissipation rate of the vibrational mode have little influence on the dynamics of the dimer system.Results obtained in this article are not only helpful to understand the natural photosynthesis,but also offer an optimal design principle for artificial photosynthesis.     

双模腔场中纠缠转移时纠缠与能量关系的研究

在初态为Bell态的两个二能级原子与双模腔场的耦合系统中,我们研究了其子系统纠缠转移时两原子的能量与其纠缠演化之间的关系。结果表明：两者的关系是密不可分的。而且,我们还讨论了原子间的偶极-偶极相互作用和腔场中的光子数对这种关系的影响。     

侧链结构对PPV/C_(60)组合体系的激发传递和电荷转移过程的影响

本文考察不同的侧链长度对聚对苯乙炔 (PPV)衍生物的光学性质等的影响 ,以及PPV/C60 的组合薄膜中的激发传递和电荷转移过程。结果表明随着连接在PPV的侧链长度的增长 ,其π π 跃迁带隙变窄 ,使得吸收和发射峰的位置逐渐红移 ;同时观测到PPV/C60 间存在着极有效的激发传递过程 ,从而使得PPV衍生物的荧光在很大程度上被C60 分子所猝灭 ;MD PPV/C60 组合膜中观测到了C-60 的吸收峰 ,这表明该体系存在着基态电荷转移过程 ,同时也表明PPV衍生物与C60 分子间的相互作用和PPV的侧链长短密切相关。     

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.     

Laser-induced quadrupole-quadrupole collisional energy transfer in Xe-Kr

By considering the relative velocity distribution function and multipole expansion interaction Hamiltonian, a three-state model for calculating the cross section of laser-induced quadrupole-quadrupole collisional energy transfer is presented. Calculated results in Xe-Kr system show that in the present system, the laser-induced collision process occurs for ～4 ps, which is much shorter than the dipole-dipole laser-induced collisional energy transfer (LICET) process. The spectrum of laser-induced quadrupole-quadrupole collisional energy transfer in Xe-Kr system has wider tunable range in an order of magnitude than the dipole-dipole LICET spectra. The peak cross section decreases and moves to the quasi-static wing with increasing temperature and the full width at half peak of the profile becomes larger as the system temperature increases.     

Laser induced collisional energy transfer in Sr—Li system

A four-state model considering the relative velocity distribution function for calculating the cross section of laserinduced collisional energy transfer in a Sr-Li system is presented and profiles of laser-induced collision cross section are obtained.The resulting spectra obtained from different intermediate states are strongly asymmetrical in an opposite asymmetry.Both of the two intermediate states have contributions to the final state,and none of the intermediate states should be neglected.The peak of the laser-induced collisional energy transfer(LICET) profile shifts toward the red and the FWHM becomes narrower obviously with laser field intensity increasing.A cross section of 1.2 × 10-12 cm 2 at a laser field intensity of 2.17 × 10 7 V/m is obtained,which indicates that this collision process can be an effective way to transfer energy selectively from a storage state to a target state.The existence of saturation for cross section with the increase of the laser intensity shows that the high-intensity redistribution of transition probabilities is an important feature of this process,which is not accounted for in a two-state treatment.     

Interaction and energy transfer between carbon dots and serum human transferrin

Human serum transferrin has been used as a potential drug carrier to transport anticancer drugs to tumor cells, where transferrin receptors are overexpressed on the surface. Carbon dots are biocompatible, and have potential application to drug delivery. The interaction mechanism of human serum transferrin with carbon dots was investigated by fluorescence spectra, ultraviolet–visible absorption spectroscopy, circular dichroism, at extracellular pH 7.4 and endosomal pH 4.8, at varying temperatures. We observed a quenching of fluorescence of human serum transferrin in the presence of carbon dots by a static quenching mechanism and also analyzed the quenching results using the Stern–Volmer equation and obtained high-affinity binding to human serum transferrin dominated by hydrogen bonds or van der Waals forces. An isoemissive point was seen, indicating that quenching of human serum transferrin depends on the formation of human serum transferrin–carbon dots complex. Binding distance between carbon dots and human serum transferrin substantiated that the photoinduced electron transfer and Föster nonradiative resonance energy transfer mechanism were also involved in the quenching of protein. Furthermore, the circular dichroism also showed that carbon dots changed the secondary structure of human serum transferrin to some extent with decreased α-helix content or peak wavelength red-shifted. This study provides some theoretical foundation for carbon dots as a promising probe to monitor the process of delivering drugs to human serum transferrin in the future.     

Vibration-assisted coherent excitation energy transfer in a detuned dimer

The important role of high-energy intramolecular vibrational modes for excitation energy transfer in the detuned photosynthetic systems is studied. Based on a basic dimer model which consists of two two-level systems(pigments)coupled to high-energy vibrational modes, we find that the high-energy intramolecular vibrational modes can enhance the energy transfer with new coherent transfer channels being opened when the phonon energy matches the detuning between the two pigments. As a result, the energy can be effectively transferred into the acceptor. The effective Hamiltonian is obtained to reveal the strong coherent energy exchange among the donor, the acceptor, and the high-energy intramolecular.A semi-classical explanation of the phonon-assisted mechanism is also shown.     

转动传能中的量子干涉--干涉角和转动量子数的关系

沙国河等人在CO(A1∏(v=0)~e3∑-(v=1))体系与He,Ne和Ar碰撞诱导转动传能中首次观测到了量子干涉效应,并测量了干涉度。从理论上进一步研究原子-双原子分子体系碰撞诱导转动传能中量子干涉效应与转动量子数以及能量间隔的关系是十分必要的。我们考虑长程相互作用势,应用一级玻恩近似和直线轨迹近似,分别计算了CO(A1∏(v=0)~e3∑-(v=1))体系和He,Ne,Ar碰撞诱导转动传能中不同转动量子数以及不同能量间隔下的干涉角,得到了干涉角随转动量子数和能量间隔的变化趋势。这些结果对设计、分析这种类型的实验有一定的指导意义。     

Laser-induced quadrupoleben quadrupole collisional energy transfer in Xe-Kr

By considering the relative velocity distribution function and multipole expansion interaction Hamiltonian, a three-state model for calculating the cross section of laser-induced quadrupole-quadrupole collisional energy transfer is presented. Calculated results in Xe-Kr system show that in the present system, the laser-induced collision process occurs for ~4 ps, which is much shorter than the dipole-dipole laser-induced collisional energy transfer (LICET) process. The spectrum of laser-induced quadrupole-quadrupole collisional energy transfer in Xe-Kr system has wider tunable range in an order of magnitude than the dipole-dipole LICET spectra. The peak cross section decreases and moves to the quasi-static wing with increasing temperature and the full width at half peak of the profile becomes larger as the system temperature increases.     

Tuning energy transfer efficiency in quantum dots mixture by controling donor/acceptor ratio

Improving the emission performance of colloidal quantum dots (QDs) is of paramount importance for their applications on light-emitting diodes (LEDs), displays and lasers. A highly promising approach is to tune the carrier recombination channels and lifetime by exploiting the energy transfer process. However, to achieve this precise emission optimization, quantitative modulation on energy transfer efficiency is highly desirable but still challenging. Here, we demonstrate a convenient approach to realize tunable energy transfer efficiency by forming QDs mixture with controllable donor/acceptor (D/A) ratio. With the mixing ratio ranging from 16/1 to 1/16, the energy transfer efficiency could be effectively tuned from near zero to ~70%. For the high mixing ratio of 16/1, acceptors obtain adequate energy supplied by closely surrounding donors, leading to~2.4-fold PL enhancement. While for the low mixing ratio, the ultrafast and efficient energy extraction process directly suppresses the multi-exciton and Auger recombination in the donor, bringing about a higher threshold. The facile modulation of emission performance by controllably designed mixing ratio and quantitatively tunable energy transfer efficiency will facilitate QD-based optoelectronic and photovoltaic applications.     

关于理想平行板电容器充电过程的能量传输问题

通过对基于简单RC电路的理想平行板电容器缓慢充电过程的研究,得到了相关的电磁场分布以及能量分布,并讨论了其中的电磁场能量传输问题．     

水平变化波导中的简正波耦合与能量转移

针对海底地形水平变化对声场能量传播和声场干涉结构的影响,对简正波之间的耦合和能量转移进行了研究.建立了一种二维大步长格式的耦合简正波模型和三维楔形波导耦合简正波模型,以便快速有效地分析简正波之间的耦合和能量转移.基于耦合简正波模型,阐述了前向声场能量在水平变化波导中传播时的转移过程.并根据射线简正波理论,解释了海底地形变化对声场能量分布的影响机理.水平变化波导中声场的仿真计算表明,当本征值虚部发生剧烈变化时声场存在着较强的简正波耦合和能量转移,且海底地形变化将导致声场能量的水平传播方向偏转至海水深度增加的方向.在声场能量转移和传播方向变化中,声场的能量趋于保留在波导中而不向海底泄漏.同时,声场能量分布受到类似于压缩或稀疏的作用,从而形成椭圆状的干涉结构.     

Calculation of laser induced collisional energy transfer in the Sr-Ca system

Based on the four-state model of laser-induced collisional energy transfer,the cross section of the collisional energy transfer in the Sr-Ca system is obtained.Various factors,including field intensity,relative speed,and temperature,which influence the collisional cross section,are discussed for illustrating the features of the Sr-Ca laser-induced collisional energy transfer(LICET) process.The calculated results show that the LICET spectral profiles obviously become narrower when the laser field intensity i...