应变层超晶格（ZnSe）n／（ZnS）m的激子结合能

在双量子阱近似下,用变分法计算了（ＺｎＳｅ）ｎ／（ＺｎＳ）ｍ应变层超晶格的激子结合能,为光致发光谱和光致发光振荡谱的分析提供了依据和参考数据。     

Simultaneous fluorescence and Raman scattering from single carbon nanotubes

Single-molecule fluorescence spectroscopy was used to determine the electronic properties of individual single-walled carbon nanotubes. Carbon nanotube structure was determined simultaneously from Raman spectroscopy. Fluorescence spectra from individual nanotubes with identical structures have different emission energies and linewidths that likely arise from defects or the local environment. Unlike most other molecules studied to date, the fluorescence intensity or spectrum from a single nanotube unexpectedly did not fluctuate.     

Observing the multiexciton state in singlet fission and ensuing ultrafast multielectron transfer

Multiple exciton generation (MEG) refers to the creation of two or more electron-hole pairs from the absorption of one photon. Although MEG holds great promise, it has proven challenging to implement, and questions remain about the underlying photo-physical dynamics in nanocrystalline as well as molecular media. Using the model system of pentacene/fullerene bilayers and femtosecond nonlinear spectroscopies, we directly observed the multiexciton (ME) state ensuing from singlet fission (a molecular manifestation of MEG) in pentacene. The data suggest that the state exists in coherent superposition with the singlet populated by optical excitation. We also found that multiple electron transfer from the ME state to the fullerene occurs on a subpicosecond time scale, which is one order of magnitude faster than that from the triplet exciton state.     

Optical signatures of coupled quantum dots

An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.     

Control of exciton fluxes in an excitonic integrated circuit

Efficient signal communication uses photons. Signal processing, however, uses an optically inactive medium, electrons. Therefore, an interconnection between electronic signal processing and optical communication is required at the integrated circuit level. We demonstrated control of exciton fluxes in an excitonic integrated circuit. The circuit consists of three exciton optoelectronic transistors and performs operations with exciton fluxes, such as directional switching and merging. Photons transform into excitons at the circuit input, and the excitons transform into photons at the circuit output. The exciton flux from the input to the output is controlled by a pattern of the electrode voltages. The direct coupling of photons, used in communication, to excitons, used as the device-operation medium, may lead to the development of efficient exciton-based optoelectronic devices.     

Unmasking electronic energy transfer of conjugated polymers by suppression of O(2) quenching

The photochemistry of poly[2-methoxy, 5-(2'-ethyl-hexyloxy)-p-phenylene-vinylene] (MEH-PPV) has been found to be highly dependent on the presence of O(2), which increases singlet exciton quenching dramatically. Spectroscopy on isolated single molecules of MEH-PPV in polycarbonate films that exclude O(2) reveals two distinct polymer conformations with fluorescence maxima near 555 and 580 nanometers wavelength, respectively. Time-resolved single-molecule data demonstrate that the 580-nanometer conformation exhibits a "landscape" for intramolecular electronic energy relaxation with a "funnel" that contains a 580-nanometer singlet exciton trap at the bottom. The exciton traps can be converted to exciton quenchers by reaction with O(2). Conformationally induced, directed-energy transfer is arguably a critical dynamical process that is responsible for many of the distinctive photophysical properties of conjugated polymers.     

缙云山四川大头茶年轮生长的功率谱分析

在重庆缙云山采集了２００多个四川大头茶（Ｇｏｒｄｏｎｉａａｃｕｍｉｎａｔａ）年轮样品，建立了该树木的年轮指数年表，并对照有关气象资料应用功率谱方法对其年轮生长动态进行了分析研究。结果表明，四川大头茶年轮年表与重庆地区年降水量密切相关。其年轮的功率谱密度值随波数分布不均匀。年轮宽度生长变异的周期为２年、１１年、２２年左右。分析四川大头茶年轮生长变异的功率谱，可以探讨、揭示其环境降雨量的变化趋势     

Ultralong-range polaron-induced quenching of excitons in isolated conjugated polymers

In conjugated polymers, radiative recombination of excitons (electron-hole pairs) competes with nonradiative thermal relaxation pathways. We visualized exciton quenching induced by hole polarons in single-polymer chains in a device geometry. The distance-scale for quenching was measured by means of a new subdiffraction, single-molecule technique--bias-modulated intensity centroid spectroscopy--which allowed the extraction of a mean centroid shift of 14 nanometers for highly ordered, single-polymer nanodomains. This shift requires energy transfer over distances an order of magnitude greater than previously reported for bulk conjugated polymers and far greater than predicted by the standard mechanism for exciton quenching, the unbiased diffusion of free excitons to quenching sites. Instead, multistep "energy funneling" to trapped, localized polarons is the probable mechanism for polaron-induced exciton quenching.     

Condensation of semiconductor microcavity exciton polaritons

A phase transition from a classical thermal mixed state to a quantum-mechanical pure state of exciton polaritons is observed in a GaAs multiple quantum-well microcavity from the decrease of the second-order coherence function. Supporting evidence is obtained from the observation of a nonlinear threshold behavior in the pump-intensity dependence of the emission, a polariton-like dispersion relation above threshold, and a decrease of the relaxation time into the lower polariton state. The condensation of microcavity exciton polaritons is confirmed.     

Measuring picosecond isomerization kinetics via broadband microwave spectroscopy

The rotational spectrum of a highly excited molecule is qualitatively different from its pure rotational spectrum and contains information about the intramolecular dynamics. We have developed a broadband Fourier transform microwave spectrometer that uses chirped-pulse excitation to measure a rotational spectrum in the 7.5- to 18.5-gigahertz range in a single shot and thereby reduces acquisition time sufficiently to couple molecular rotational spectroscopy with tunable laser excitation. After vibrationally exciting a single molecular conformation of cyclopropane carboxaldehyde above the barrier to C-C single-bond isomerization, we applied line-shape analysis of the dynamic rotational spectrum to reveal a product yield and picosecond reaction rate that were significantly different from statistical predictions. The technique should be widely applicable to dynamical studies of radical intermediates, molecular complexes, and conformationally flexible molecules with biological interest.     

Coupling and entangling of quantum states in quantum dot molecules

We demonstrate coupling and entangling of quantum states in a pair of vertically aligned, self-assembled quantum dots by studying the emission of an interacting electron-hole pair (exciton) in a single dot molecule as a function of the separation between the dots. An interaction-induced energy splitting of the exciton is observed that exceeds 30 millielectron volts for a dot layer separation of 4 nanometers. The results are interpreted by mapping the tunneling of a particle in a double dot to the problem of a single spin. The electron-hole complex is shown to be equivalent to entangled states of two interacting spins.     

利用瞬态荧光技术研究单重态激子裂变的电荷转移模型

有机材料中单重态激子的裂变过程,由于其在有机光伏器件中的潜在应用而成为一个科学研究的热点.传统的观点采用电荷转移模型来解释激子裂变过程,即认为2个参与裂变的分子之间通过两次的电荷转移来实现分子状态的改变.而在电荷转移的物理图像中,又包括双空穴转移方式和双电子转移方式两种可能性.为了检验电荷转移模型的合理性,将能够发生激子裂变过程的红荧烯分子分别混合于其他4种有机分子中,这4种有机分子被当作间隔分子,用来分离混合膜中掺杂的红荧烯分子.对红荧烯分子与间隔分子,二者间HOMO能级的能量差构成空穴转移的隧穿势垒,而二者间LUMO能级的能量差构成电子转移的隧穿势垒.对4个样品发光衰减曲线的测量与分析表明,激子裂变的速率与电子隧穿势垒的高度具有明显的关联,这从实验角度首次印证了双电子转移模型而否定了双空穴转移模型.     

Conformational equilibria in spin-labeled hemoglobin

A component characteristic of deoxyhemoglobin appears in the paramagnetic resonance spectrum of spin-labeled oxyhemoglobin, and vice versa, under conditions of pH and ionic strength consistent with the interpretation that the spectrum is sensitive to the conformational equilibrium of the carboxy-terminal histidines. The oxygenation-induced change in the resonance spectrum is discussed in terms of shifts in this equilibrium.     

水溶性壳聚糖的制备及结构表征

探讨了如何控制反应的均相条件来制备水溶性壳聚糖 ,并对水溶性壳聚糖进行了红外光谱分析和元素分析。研究发现随着乙酸酐的用量的增加 ,壳聚糖的脱乙酰度随之降低 ,而反应时间对脱乙酰度没有影响。元素分析和红外光谱分析表明 ,5 0 %脱乙酰度的水溶性壳聚糖与 90 %脱乙酰度的壳聚糖在分子结构上并没有什么不同 ,5 0 %脱乙酰度的壳聚糖的水溶性的提高可能是部分脱乙酰化对晶体的破坏作用而造成的     

Phase diagram of degenerate exciton systems

Degenerate exciton systems have been produced in quasi-two-dimensional confined areas in semiconductor coupled quantum well structures. We observed contractions of clouds containing tens of thousands of excitons within areas as small as (10 micron)2 near 10 kelvin. The spatial and energy distributions of optically active excitons were determined by measuring photoluminescence as a function of temperature and laser excitation and were used as thermodynamic quantities to construct the phase diagram of the exciton system, which demonstrates the existence of distinct phases. Understanding the formation mechanisms of these degenerate exciton systems can open new opportunities for the realization of Bose-Einstein condensation in the solid state.     

风险模型的破产概率的计算及其相关问题

本文主要研究了在Sparre Andersen风险过程中时间间隔过程为Erlang(n)的破产概率及其相关问题。在此基础上,特别考虑了理赔量为possion理赔过程时候满足的破产概率的显示表达形式,同时计算出了最大盈余量未到达b时的带有边际条件的同类积分—微分方程破产概率的表达形式方程的通解问题和当n=2时的生存概率的显示表达形式。     

Polar solvent dynamics and electron-transfer reactions

Polar solvents often exert a dramatic influence on reactions in solution. Equilibrium aspects of this influence involve differential solvation of reactants compared to the transition state that lead to alteration of the free-energy barrier to reaction. Such effects are well known, and often give rise changes in reaction rates of many orders of magnitude. Less well understood are effects arising from non-equilibrium, dynamical aspects of solvation. During the course of reaction, charge is rapidly redistributed among reactants. How the reaction couples to its solvent environment depends critically on how fast the solvent can respond to these changes in reactant charge distribution. In this article the dynamics of solvation in polar liquids and the influence of this dynamics on electron-transfer reactions are discussed. A molecular picture suggests that polar solvation occurs on multiple time scales as a result of the involvement of different types of solvent motion. A hierarchy of models from a homogeneous continuum model to one incorporating molecular aspects of solvation, combined with computer simulations, gives insight into the underlying dynamics. Experimental measures of solvation dynamics from picosecond and subpicosecond time-dependent Stokes shift studies are compared with the predictions of theoretical models. The implication of these results for electron-transfer reactions in solution are then briefly considered.     

香菇子实体蛋白多糖Le-Ⅲ的分离、纯化及其性质研究

香菇子实体经热水提取,乙醇沉淀,脱蛋白,ＤＥＡＥ纤维素柱及纤维素凝胶柱层析得到淡黄色纤维状疏松固体Ｌｅ－Ⅲ,Ｌｅ－Ⅲ经聚丙烯酰胺凝胶电泳和Ｓｅｐｈａｒｏｓｅ ＣＬ－６Ｂ柱层分析,证明了分子量分布均一的多糖－蛋白质复合物。Ｌｅ－Ⅲ红外扫描有典型的多糖吸收峰,气相色谱测单糖组成为阿拉伯糖、木糖、甘露糖、半乳糖、葡萄糖,摩尔比０．３１：０．４７：１．００：１．１５：８．９２。     

Examining nanoenvironments in solids on the scale of a single, isolated impurity molecule

Optical spectroscopy of single impurity molecules in solids can be used as an exquisitely sensitive probe of the structure and dynamics of the specific local environment around the single molecule (the "nanoenvironment"). Recently observed effects such as spectral diffusion, perturbations by external fields, changes in molecular photophysics, shifts in vibrational modes, optical modification of the absorption spectrum, dynamics due to amorphous system physics, and magnetic resonance of a single molecular spin attest to the vitality of and growing interest in this new field, which may lead to optical storage on the single-molecule level.     

Quantum deconstruction of the infrared spectrum of CH5+

We present two quantum calculations of the infrared spectrum of protonated methane (CH5+) using full-dimensional, ab initio-based potential energy and dipole moment surfaces. The calculated spectra compare well with a low-resolution experimental spectrum except below 1000 cm(-1), where the experimental spectrum shows no absorption. The present calculations find substantial absorption features below 1000 cm(-1), in qualitative agreement with earlier classical calculations of the spectrum. The major spectral bands are analyzed in terms of the molecular motions. Of particular interest is an intense feature at 200 cm(-1), which is due to an isomerization mode that connects two equivalent minima. Very recent high-resolution jet-cooled spectra in the CH stretch region (2825 to 3050 cm(-1)) are also reported, and assignments of the band origins are made, based on the present quantum calculations.