Investigation of photoelectron temporal characteristics in silver halide microcrystals using the microwave absorption technique

The free photoelectron lifetime reflects to a large extent the latent image formation efficiency and sensitivity of silver halide material. The microwave absorption dielectric-spectrum technique enables measurement of the photoelectron decay process of silver halide emulsion exposed to 35ps laser pulse. For T-grain AgBr emulsion, the relationship between exciting energy and photoelectron action has been obtained, and the influence of iodide dopants on photoelectron lifetime was measured and analysed. The photoelectron lifetime of dye-sensitized AgBr emulsion with tabular grains is shorter than that with cubic grains, and the latent image formation efficiency of the former is higher than the latter.     

超快非均质电子转移的优化控制研究(Ⅱ)

本文用优化控制理论,以分子的基态作为目标态,考虑了在不同条件下,从二萘嵌苯到TiO2超快电子转移的动力学过程.发现在此目标态的作用下,电子经过一个电子激发-回落的过程从分子的基态激发到与半导体导带耦合的第一电子激发态,然后在给定目标态的作用下回落至电子基态,从而实现了较高的目标态产生率.由于二萘嵌苯的电子激发态与半导体导带能级间的强电子转移耦合,这一控制任务较电子激发态为目标态而言,更适合于实验研究.     

Investigation of the photoelectron decay of silver halide microcrystal

The microwave absorption dielectric spectrum can be used to study the decay process of free photoelectrons and shallow-trapped electrons in semiconductor crystals. The decay curve of free photoelectrons and shallow-trapped electrons of silver halide grains is measured using this technique. The influence of iodide and K_4Fe(CN)_6 shallow electron trap dopants on the photoelectron lifetime of silver halide grains is studied. For the unsensitized cubic AgCl crystals, when the free photoelectron lifetime (FLT) reaches a maximum, the photographic efficiency is optimal. From our analysis, we conclude that FLT is the longest for the cubic AgCl crystals doped with 0.5% iodide at 80% doping position and 1×10^{-6} mol K_4Fe(CN)_6/molAg, whereas, for the highly photosensitized cubic AgBrCl crystals doped with K_4Fe(CN)_6, the photographic efficiency is optimal when the FLT reaches its minimum. The free photoelectron lifetime reaches minimum and the sensitivity of AgBrCl emulsion reaches maximum when the doping position is 30%Ag at K_4Fe(CN)_6 content of 10^{-6}mol/molAg.     

光合作用原初过程能量和电荷超快传递过程原理浅析

文章侧重于从物理的角度,介绍光合作用原初过程中能量和电荷超快传递过程的相关物理化学原理,如费米黄金规则,Frster及Dexter传能机制,Marcus电荷转移理论及激子理论.辨析相关原理的适用范围、共性及差异,并力图在上述相关原理的基础上阐述光合膜蛋结构与功能的关系,勾画出该研究方向的基本脉络.     

界面电子转移对量子点荧光闪烁行为的影响

利用激光扫描共聚焦显微系统分别测量了CdSe/ZnS量子点在SiO2玻片表面、铟锡氧化物(ITO)纳米粒子表面和聚甲基丙烯酸甲酯(PMMA)薄膜表面上的荧光闪烁行为.研究发现,不同界面环境中量子点的亮态发光持续时间的概率密度都服从指数修正的幂律分布P(t)∝t-αexp(-t/μ).与处于SiO2玻片表面的情况相比,在ITO表面上的单量子点具有非常短暂的亮态发光持续时间,而在PMMA表面的单量子点亮态发光持续时间最长.这种荧光闪烁行为的不同主要归因于量子点与三种材料之间的界面电子转移特性.     

超快非均质电子转移的优化控制研究(Ⅰ)

本文用三能级的单振动模型,模拟了从二萘嵌苯到TiO2超快电子转移的动力学过程,发现在弱电子转移耦合下,电子在激光场的作用下激发至分子激发态转移然后到半导体导带,在强电子转移耦合下,电子直接由基态转移到半导体导带。在优化控制的理论模拟中以电子激发态的振动基态为目标态,考虑了不同注入位置条件下的电子转移的动力学过程,研究了优化激光场在给定时间内实现目标态的过程,由于从分子激发态到半导体的超快电子转移,只有当分子激发态能级与半导体导带底能级简并时,才能实现较高的目标态产生率。     

The influence of trapping centres on the photoelectron decay in silver halide

Photoelectron is the foundation of latent image formation, the decay process of photoelectrons is influenced by all kinds of trapping centres in silver halide. By analysing the mechanism of latent image formation it is found that electron trap, hole trap, and one kind of recombination centre where free electron and trapped hole recombine are the main trapping centres in silver halide. Different trapping centres have different influences on the photoelectron behaviour. The effects of all kinds of typical trapping centres on the decay of photoelectrons are systematically investigated by solving the photoelectron decay kinetic equations. The results are in agreement with those obtained in the microwave absorption dielectric spectrum experiment.     

Response of photosensitive silver halide micro-crystals to multiple-charged particles

Temperature dependence of sensitivity of silver halide micro-crystals is theoretically examined for a wide range of momenta and charges of ionising particles. Our earlier results on the ionisation theory have now been extended for the interaction of multiple-charged particles with AgBr emulsion grains.     

银层超透镜光学传递函数的研究

银层超透镜对基于表面等离子体激元的超分辨光刻、 成像和生物传感有着重要作用.利用银层超透镜的光学传递函数详 细研究了银板的表面等离子体激元共振和成像特性, 并利用时域有限差分法计算模拟了银层超透镜的成像过程, 得到与理论推导公式相符合的结果, 证明了光学传递函数的可靠性, 为基于表面等离子体激元的传感器件、 超分辨成像以及辅助增强干涉光刻提供了快速参数优化方法.     

Laser pulse control of ultrafast electron transfer reactions

The optimal control (OC) scheme for molecular dynamics is applied to the study of ultrafast bridge mediated electron transfer (ET). Utilizing the methods of dissipative quantum dynamics in combination with the OC approach the guided charge motion in a donor-bridge-acceptor system including a single active vibrational coordinate is studied. The control field drives the optical transition from the electronic ground-state of the ET system into the donor-level and can be used to prepare special electronic and vibrational states. In particular, it is demonstrated that charge localization becomes possible at the acceptor or bridge molecule as well as in the electronic ground-state of the ET system. Received 30 August 2000 and Received in final form 25 October 2000     

Deterministic and replaceable transfer of silver flakes for microcavities

How to fabricate high-quality microcavities simply and at low cost without causing damage to environmentally sensitive active layers such as perovskites are crucial for the studies of exciton−polaritons, however, it remains challenging in the field of microcavity fabrication. Usually, once the top mirror is deposited, the detuning of the microcavity is fixed and there is no easy way to tune it. Here, we have developed a method for deterministically transferring silver mirrors, which is relatively simple and guarantees the active layer from damaging of high temperature, particle bombardment, etc., during the deposition of the top mirror. Furthermore, with the help of a glass probe, we demonstrate a replaceable silver transfer method to tune the detuning of the microcavity, thereby changing the coupling of photons and excitons therein. The developed deterministic and replaceable silver mirror transfer methods will provide the capability to fabricate high-quality and tunable microcavities and play an active role in the development of the exciton−polariton field.     

一种普适型国产银盐感光胶的全息特性实验研究

实验研究了一种普适型国产HR_1型卤化银乳胶的主要全息特性;论述了其曝光量对衍射效率的影响;比较了两种化学后处理方法对衍射效率和信噪比的影响。实验结果表明,HR_1型卤化银乳胶是一种适合于记录透射和反射型合成全息图的记录介质,可以获得较高的衍射效率和信噪比。     

异质结线性吸收谱中的等离激元效应

将染料分子与半导体表面所组成的异质结与金属纳米粒子的耦合系统作为研究对象,考虑分子的振动态,在偶极-偶极近似下研究其线性吸收谱及相关的电荷转移动力学过程. 对金属纳米粒子作用下吸收谱变宽及相关的电子转移增强过程作了仔细的分析和讨论,理论分析了金属钠米粒子的表面等离激元对异质结中超快电子转移的影响. 关键词： 金属纳米粒子 等离激元 异质结电荷转移     

Accurate analysis of electron transfer from quantum dots to metal oxides in quantum dot sensitized solar cells

Electron transfer rate from quantum dot (QD) to metal oxide (MO) in quantum dot sensitized solar cells (QDSSCs) has an important role in the efficiency. In this work, we analyse the electron transfer rate from CdSe, CdS and CdTe QDs to TiO₂, ZnO and SnO₂ MOs by extending the related equations with considering various effects, based on the Marcus theory. In this regard, the effects of QD diameter, QD–MO spacing, the crystalline defects, temperature, and the reorganizational energy, on the electron transfer rate are investigated. The results show that, the maximum electron transfer rate is achieved for CdTe QD with the mentioned three MOs. Moreover, in order to direct the designer to reach the appropriate QDs–MOs combinations for obtaining the maximum electron transfer rate, the average electron transfer rate for various combinations is calculated. For the verification of simulation method, a part of work has been compared with the previous experimental and theoretical results, which indicates the correctness of our simulation algorithm.     

A switch in the electron transfer from heme a to binuclear centre of cytochrome c oxidase

New experimental evidence that a switch controls the reduction of the heme a₃－Cu_B binuclear centre has been observed in the N₂-dried thin film of purified cytochrome oxidase. When immersing the enzyme film into the acid phosphate buffer with extremely low concentration of dithionite, a spectrum was given to show a reduction of heme a with no electrons resting on Cu_A. By increasing dithionite, electrons could be accumulated gradually on Cu_A, but the binuclear centre still remains in the oxidized state. When the accumulation of electrons on Cu_A and/or heme a exceeded a threshold, a turnover of reduction of the binuclear centre and oxidation of heme a occurred abruptly. This switch-like action is pH-dependent.     

Study on time-resolved fluorescence dynamics of cyanine dye sensitizing AgBr

The fluorescence spectra of three different dyes adsorbed on the tabular and cubic AgBr microcrystals are obtained by the picosecond time-resolved streak camera technique. The dependence of the ultrafast electron transferring from dye-aggregates to the conduction band of AgBr and the efficiency of spectral sensitization on different kinds of dyes with different concentrations is analyzed. Further more, the microcosmic mechanism of the sensitization process is discussed. It is found that the fluorescence decay curves are fitted very well by the double exponential function, consisting of a slow component and a fast one with large amplitude. We consider this fast one mainly attributable to the electron transfer from dye J-aggregates to the conduction band of AgBr. Supported by the National Natural Science Foundation of China (Grant No. 60478033), the Doctoral Foundation of Hebei Province of China (Grant No. B2003119), and the Science and Technology Project of Hebei Province of China (Grant No. 05215102)     

Efficiency of energy transfer by resonance in quenching of protein fluorescence by dyes

Considering the quenching of tryptophan fluorescence of bovine serum albumin by various dyes as an example, it is shown that overlap of radiation and absorption spectra does not necessarily lead to energy transfer by resonance. No correlation is revealed between the limiting quenching and the Forster overlap integral. Quenching can occur even in the absence of overlap. The magnitude of energy transfer is markedly lower than that of quenching owing to competing processes, namely, excitation deactivation by the dye and, probably, by the protein itself which undergoes conformation upon sorption of the dye. Negatively charged and neutral dyes posses, on the average, a higher quenching activity relative to albumin than do positively charged dyes. Institute of the Biophysics of Cells of the Russian Academy of Sciences, Pushchino, 142292, Moscow Region, Russia. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 65, No. 2, pp. 290–293, March–April, 1998.     

Vibrational control of molecular electron transfer reactions

ABSTRACT

Vibrational motions promote molecular electron transfer (ET) reactions by bringing electron donor and electron acceptor electronic states to fleeting resonance, and by modulating the donor-to-acceptor electronic coupling. The main experimental signature of molecular motion effects on the ET rate is the temperature dependence of the rate, which gives information about the overall free energy activation barrier for the ET reaction. Another approach to probing the vibrational control of ET reactions is to excite specific electron-transfer-active vibrational motions by external infrared (IR) fields. This type of experimental probe is potentially more specific than thermal excitation and recent experiments have shown that molecular ET rates can be perturbed by mode-specific IR driving. We review the theory and experiments of vibrational control of ET rates, and discuss future challenges that need to be tackled in order to achieve the mode-specific tuning of rates.     

Model for primary electron transfer and coupling of electronic states at reaction centers of purple bacteria

A detailed derivation is presented for relations making it possible to describe the effect of temperature on the halfwidth of the P960 and P870 absorption bands and also on the electron transfer (ET) rate at reaction centers (RCs) of the purple bacteria Rps. viridis and Rb. sphaeroides. Primary electron transfer is considered as a resonant nonradiative transition between P* and P⁺B _L ⁻ states (where P is a special pair, B_L is an additional bacteriochlorophyll in the L branch of the reaction center). It has been shown that the vibrational h_α mode with frequency 130–150 cm⁻¹ controls primary electron transfer. It has been found that the matrix element of the electronic transition between the states P* and P⁺B _L ⁻ is equal to 12.7 ± 0.9 and 12.0 ± 1.2 cm⁻¹ for Rps. viridis and Rb. sphaeroides respectively. The mechanism is discussed for electron transport from P* and B_L and then to bacteriopheophytin H_L. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 73, No. 3, pp. 294–303, May–June, 2006.     

Bunch evolution study in optimization of MeV ultrafast electron diffraction

Megaelectronvolt ultrafast electron diffraction (UED) is a promising detection tool for ultrafast processes. The quality of diffraction image is determined by the transverse evolution of the probe bunch. In this paper, we study the contributing terms of the emittance and space charge effects to the bunch evolution in the MeV UED scheme, employing a mean-field model with an ellipsoidal distribution as well as particle tracking simulation. The small transverse dimension of the drive laser is found to be critical to improve the reciprocal resolution, exploiting both smaller emittance and larger transverse bunch size before the solenoid. The degradation of the reciprocal spatial resolution caused by the space charge effects should be carefully controlled.