斯塔克调制—电旋转激光光谱技术及其应用

采用斯塔克调制电旋转激光光谱技术将由偶然简并能级跃迁产生的电旋转信号从非简并能级跃迁中分离出来，因而简化了转动量子态的跃迁谱线，减少了谱线重叠现象，反映了分子能级受偶然简并斯塔克相互作用以及电四极相互作用的特性，非常适合那些转动谱线密集，微扰严重的多原子分子的光谱测量与分析。本文既给出了这种光谱技术的半经典理论模型，又运用微扰理论解释了用该技术所测的ＮＯ２分子的转动光谱的形成原因和它们的主要特征。     

Cu_2O和Ge的基本反射光谱——两种不同性质的反射带结构

本文在室温下测量了Cu_2O和Ge的基本反射光谱(0.22—1.00μ);研究了区分激子反射带结构和带际跃迁反射带结构的实验方法。光学抛光处理晶体表面对反射光谱中激子结构的影响极大,但对带际跃迁结构的影响不大。确定了Cu_2O紫外反射带的带际跃迁性质。讨论了Cu_2O和Ge的基本反射光谱和能带结构的联系。特别注意了Ge的反射光谱中的一些弱结构和能带结构的联系。工作中也涉及了晶格的有序度和能带结构的联系和吸收气氛影响短波反射带“下塌”的现象。     

Cu2O和Ge的基本反射光谱——两种不同性质的反射带结构

本文在室温下测量了Cu₂O和Ge的基本反射光谱(0.22—1.00μ);研究了区分激子反射带结构和带际跃迁反射带结构的实验方法。光学抛光处理晶体表面对反射光谱中激子结构的影响极大,但对带际跃迁结构的影响不大。确定了Cu₂O紫外反射带的带际跃迁性质。讨论了Cu₂O和Ge的基本反射光谱和能带结构的联系。特别注意了Ge的反射光谱中的一些弱结构和能带结构的联系。工作中也涉及了晶格的有序度和能带结构的联系和吸收气氛影响短波反射带“下塌”的现象。     

半导体超晶格和量子阱中量子态的光谱研究

本文讨论半导体超晶格及量子阱导带和价带的量子化亚带或子能级之间的带间光跃迁过程。所讨论的光跃迁过程或光谱研究方法有吸收光谱、光电流谱、光荧光和荧光激发谱、调制光谱以及喇曼散射光谱。关于亚带能量状态将着重讨论量子阱中的激子效应和价带亚带混和及其对带间光跃迁的影响。     

半导体超晶格和量子阱中量子态的光谱研究

本文讨论半导体超晶格及量子阱导带和价带的量子化亚带或子能级之间的带间光跃迁过程。所讨论的光跃迁过程或光谱研究方法有吸收光谱、光电流谱、光荧光和荧光激发谱、调制光谱以及喇曼散射光谱。关于亚带能量状态将着重讨论量子阱中的激子效应和价带亚带混和及其对带间光跃迁的影响。     

玻璃中CuCl微晶的尺寸量子化激子

通过对尺寸分布非均匀加宽的激子吸收带选择激发的方法,研究了玻璃中几个nm量级的CuCl微晶的激子发光光谱.发现尺寸量子化的激子态劈裂形成多个分量.通过对尺寸量子化所产生的球形微晶中激光跃迁能级劈裂的分析,得到CuCl的z_(1.2)激子跃迁质量,Luttinger参数以及x线性项系数等数据.     

分子聚集体中激子-激子湮灭过程

分子的激发能量转移和电荷转移是提高光伏电池和发光二极管效率的关键问题,其中分子聚集体中的激子-激子湮灭过程是影响分子激发能量转移的重要方面,细致研究激子-激子湮灭的动力学过程并与相关的瞬间吸收谱信号对比对相关的理论和实验都有重要意义.本文在分子间弱耦合近似下,用经典的率方程,应用方酸分子的基本参数对激子-激子湮灭过程做了微观描述,通过改变相关参数,研究了外场激发强度、聚集体的偶极矩位形、分子内的衰变率等因素对激子-激子湮灭过程的影响,分析了激子在第一激发态和高阶激发态的驰豫时间、电荷转移相干时间、激子融合和湮灭时间之间的关系,得到的结论适用于高阶激发态能级能量约为第一激发态能级能量的2倍的分子组成的分子聚集体.研究发现,J型聚集体由于相干能量转移时间较短,比H型聚集体有更高的湮灭率.激发场强越强,激子-激子湮灭的效率越高.分子高阶激发态的衰变率是激子-激子湮灭过程的关键因素.     

4氢-吡喃-4-硫酮1(n-π*),1Ag-(π→π*)和1Bu+(π→π*)等的激发态特征

理论上4氢-吡喃-4-硫酮的激发态特征用量子化学方法以及二维实空间分析法和三维立体实空间分析法加以研究.理论上的结果揭示1(n→π*)和1Ag-(π→π*)激发态是分子内电荷转移(ICT)激发态,而1Bu (π→π*)激发态是离域激发态.它们的跃迁偶极矩的强度和方向用三维密度跃迁(TD)加以解释,用三维电荷密度差(CDD)观察分子间电荷转移(ICT)的激发态特征或局部激发态特征.用二维实空间分析法研究电子.空穴相关性,离域化和激子的尺寸.     

Zno纳米晶的室温紫外受激发射特征

ZnO的激子特性对制备氧化锌基的光电子器件至关霞要,因此对ZnO量子点中激子的发光性质及其跃迁过程进行研究显得十分必要.采用溶胶-凝胶法制备了ZnO纳米晶,X射线衍射(XRD)结果表明样品具有六角纤锌矿多晶结构.研究了在不同泵浦功率激发下ZnO纳米晶的紫外发射的时间积分光谱和时间分辨光谱,观察到自南激子发光,激子-激子碰撞和电子-空穴等离子体引起的受激发射,研究了在不同泵浦功率激发下自由激子及激子-激子碰撞随泵浦功率依赖的动力学过程.研究结果对理解激子带边发射有一定帮助,对ZnO材料在短波长半导体光电器件方面有潜在的应用价值.     

高组分稀磁半导体Cd1-xMnxTe/CdTe超晶格的荧光谱研究

报道用分子束外延(MBE)技术生长的x=0.4,0.8的高组分稀磁半导体Cd1-xMnxTe/CdTe超晶格低温和室温荧光谱研究结果.基态激子跃迁能级荧光谱实验结果显示高组分超晶格中具有高量子效率和高质量光发射.对激子能级随温度的变化进行了详细研究,给出激子跃迁能量的温度系数.激子能级线型的展宽随温度变化关系可用激子-纵向光学声子耦合模型解释.与光调制反射谱实验结果进行了比较.     

Coverage dependent organic–metal interaction studied by high-resolution core level spectroscopy: SnPc (sub)monolayers on Ag(1 1 1)

We study the electronic structure of tin-phthalocyanine (SnPc) molecules adsorbed on a Ag(1 1 1) surface by high-resolution photoelectron spectroscopy. We particularly address the effect of different SnPc coverages on the interaction and charge transfer at the interface. The results give evidence for a covalent molecule–substrate interaction, which is temperature and coverage dependent. The valence and core level spectra as well as the work function measurements allow us monitoring subtle differences in the strength of the interface interaction, thus demonstrating the sensitivity of the methods. The results consistently show the effect of charge exchange between substrate and molecules which obviously leads to a net charge transfer into the SnPc molecules, and which is increased with decreasing coverage. Surprisingly, the Sn3d core levels are neither effected by variations of charge transfer and interaction strength, nor by a possible “Sn-up” or “Sn-down” orientation, which have been observed for sub-monolayers.     

Optical absorption of triplet molecular excitons in alkali cyanides

The optical absorption spectra of alkali cyanides in the UV region present a set of weak absorption bands which are identified as triplet a'³Σ⁺ molecular excitons. The nature of the molecular exciton transitions in the ionic-molecular crystals is discussed and the existence of an admixture between molecular exciton and charge transfer exciton states is suggested.     

基于电荷转移过程的PAN-C60共聚物薄膜的时间分辨荧光研究

利用吸收光谱和皮秒时间分辨荧光研究PAN－C60星状共聚物的电荷转移过程。PAN－C60共聚物的吸收和荧光光谱结果显示共聚物中存在着电荷转移过程。时间分辨荧光结果表明PAN的荧光衰减遵循双指数衰减规律（一快过程160ps和一慢过程1500ps)，快衰减过程主要来源于聚合物中主链间相互作用产生的空间间接极化子对的影响，慢变过程主要来源于单重态激子的辐射跃迁弛豫。在共聚物中，C60分子的存在除导致PAN激发态寿命缩短外，还影响聚合物链间的相互作用，C60分子对PAN荧光猝 灭作用主要通过慢变过程影响的，而对PAN的空间极化子对的影响主要与其快衰减过程有关。     

Interaction of Wannier–Stark levels in a wide well superlattice

We have investigated the energy spectrum of a superlattice with wide quantum wells under the bias of an electric field perpendicular to the superlattice layers. By using photocurrent spectroscopy, transitions of Wannier–Stark levels for the various electron and hole states are observed, and at low fields, further structures corresponding to miniband edge transitions are found. Various anticrossings could be observed at higher and lower electric fields. The anticrossings at high electric fields are due to energy alignment of different electronic sublevels in adjacent wells. The anticrossing structures at low fields could be interpreted as resonances between intrawell and interwell excitonic Wannier–Stark states with equal sublevel states, where the anticrossing is caused by differences in exciton binding energy. Fitting of transitions and anticrossings was done by using a semi-empirical model and we have extracted relevant fitting parameters like the quantum-confined Stark coefficient, binding energies for the excitonic Wannier–Stark levels and the resonant coupling strength for states involved in the various anticrossing transitions. Finally, insight into the excitonic influences on the coupling of the WS states could be obtained by comparing the fitted parameters for the various transitions.     

CdSe/ZnS纳晶中相干电声耦合效应的二维电子光谱研究

Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy (2DES) measurements. Benefiting from the ability of 2DES to dissect assembles in nanocrystal films, we have clearly identified experimental evidences of coherent coupling between exciton and phonon in CdSe/ZnS nanocrystals. In time domain, 2DES signals of excitonic transitions beat at a frequency resonant to a longitudinal optical phonon mode; in energy domain, phonon side bands are distinct at both Stokes and anti-Stokes sides. When temperature increases, phonon-induced exciton dephasing is observed with dramatic broadening of homogeneous linewidth. The results suggest exciton-phonon coupling is essential in elucidating the quantum dynamics of excitonic transitions in semiconductor nanocrystals.     

New directions in modulation spectroscopy

Since its inception in 1964, modulation spectroscopy has achieved a high level of maturity as applied to the study of interband critical point transitions in “perfect” crystals. Several papers at this conference describe applications of the physical principles and experimental techniques of modulation spectroscopy in ways that were completely unforeseen eight years ago. In this paper we review and discuss additional new directions not explicitly covered elsewhere in this volume, with emphasis on electric field modulation of optical properties in systems where the initial and/or final states are not Bloch (band) states. These include molecular spectroscopy (determination of excited state dipole moments by electric field modulated luminescence; electroabsorption in charge transfer complexes), impurity and defect spectroscopy (Stark effect of impurities; piezospectroscopy of deep defect levels), and applications in materials science (phase separation in III–V alloy thin films, and surface reactions on IV–VI epitaxial films).     

Competing periodicities in fractionally filled one-dimensional bands

We present a variable temperature scanning tunneling microscopy and spectroscopy study of the Si(553)-Au atomic chain reconstruction. This quasi-one-dimensional system undergoes at least two charge density wave (CDW) transitions, which can be attributed to electronic instabilities in the fractionally filled 1D bands of the high-symmetry phase. Upon cooling, Si(553)-Au first undergoes a single-band Peierls distortion, resulting in period doubling along the chains. This Peierls state is ultimately overcome by a competing x3 CDW, which is accompanied by a x2 periodicity in between the chains. These locked-in periodicities indicate small charge transfer between the nearly 1/2-filled and 1/4-filled bands. The presence and the mobility of atomic-scale dislocations in the x3 CDW state indicates the possibility of manipulating phase solitons carrying a (spin, charge) of (1/2, +/- e/3) or (0, +/-2e/3).     

Characterization of ultra-thin organic hetero-interfaces — SnPc/PTCDA/Ag(111)

Ultra-thin organic hetero-layers consisting of tin-phthalocyanine (SnPc) and 1,3,4,8-perylen-tetracarboxylicacid dianhydride (PTCDA) adsorbed on a Ag(111) surface are characterized with photoelectron spectroscopy (PES) and near edge X-ray absorption fine structure (NEXAFS) spectroscopy. If SnPc is deposited on the Ag(111) substrate, which is precovered with one monolayer of PTCDA, a well defined interface is formed with a closed SnPc wetting layer as can be derived from angle dependent core level and from valence photoelectron spectra. Moreover, X-ray absorption data show that the molecules are lying flat and that the bonding at the SnPc/PTCDA interface is weak.     

A DFT/TD‐DFT study for the ground and excited states of peramine and some pyrrolopyrazinone compounds

Peramine, a heterocyclic natural molecule, reveals two main, different in nature, electronic absorption bands. Theoretical calculations at the TD‐B3LYP/6–311++G(d,p) level of theory show that the electronic excitations are connected predominantly with π → π^* and charge‐transfer (CT) transitions. Excitation of electrons from the pyrrolopyrazinone ring to the side chain plays a role in creating the CT transition. The character and energy of the first 30 singlet–singlet electronic transitions have also been investigated for the most stable conformation of peramine. Copyright © 2009 John Wiley & Sons, Ltd.