Superradiance in molecular H aggregates

Direct evidence of superradiance from an organic semiconductor (quaterthiophene) whose molecules are arranged in a H aggregate fashion, is reported. Time resolved photoluminescence measurements show a linear correlation between the radiative lifetime (tau(rad)) of the purely electronic exciton recombination and the inverse of the number (N(C)) of the coherently emitting dipoles, i.e., tau(rad) proportional, variant 1/N(C). These data support the recently developed theoretical models describing the optical properties of H aggregates of rodlike molecules with a nonvanishing component of the perpendicular molecular transition dipole moment.     

Cubic phases of amphiphilic molecular aggregates

Stability and geometry of the lyotropic periodic cubic mesophases are considered in the framework of a general symmetry based phenomenological approach. A limited number of cubic structural types is shown to be formed by amphiphilic molecular aggregates due to the specific nature of self-organizing units. The related thermodynamic models predict topology of phase diagrams and specific features of transitions between isotropic, lamellar, cubic bicontinuous and cubic micellar phases. Received 25 February 1999 and Received in final form 29 June 1999     

温度对光系统Ⅱ中色素分子取向的影响

利用类囊体溶液的激发光谱和偏振荧光光谱,研究了温度对光系统Ⅱ(photosystemⅡ, PSⅡ)中色素分子取向的影响。激发光谱表明在15～45 ℃范围内,随着温度的升高,叶绿素a对应的吸收峰发生红移,激发谱强度在35 ℃达到最大,65和75 ℃时大大减弱。类囊体溶液的偏振荧光光谱中,荧光峰位在15～45 ℃范围内始终保持不变,计算得到的荧光偏振度随着温度的升高而增加。分析表明温度通过影响光系统Ⅱ内色素之间以及色素蛋白之间的相互作用,改变色素排列方向,调节光合作用效率。结果可为研究光合过程能量吸收与传递、光合保护以及太阳能电池材料等方面提供参考。     

Excitons in molecular J-aggregates of cyanine dyes: Simulation of trapping and energy transfer

A theoretical model is provided to simulate the energy transfer and trapping of excitons in cyanine J-aggregates for various geometrical configurations. Intermolecular interactions are calculated using the extended dipole method. Frenkel exciton states are obtained by a numerical diagonalization of the aggregate Hamiltonian taking into account the static disorder. A model of exciton–phonon coupling is used to describe the trapping and the energy transfer processes among the exciton states. Scattering rates are calculated and used in a Master Equation to obtain the time evolution of the excitonic populations after initial excitation. Configurationally averaged absorption lineshapes and time-resolved fluorescence decays are obtained. Our simulation model is applied to describe the excitation energy transfer between two closely spaced linear chains of pseudoisocyanine (PIC) molecules and to a two-dimensional monolayer composed of a mixing of oxacyanine and thiacyanine molecules.     

Excitons in silicon nanocrystallites

Recombination and binding energies of excitons in nanocrystalline silicon quantum dots are calculated within the effective mass approximation including the effects of the induced electrostatic polarization. The calculated exciton recombination energies compare well with other calculations and with the results from photoluminescence measurements in porous silicon. The calculated exciton binding energies are far larger than the bulk exciton binding energy and show substantial dependence on the matrix that surrounds the nanocrystallites. A model is proposed that explains the main orange-red, blue and infrared luminescence peaks of porous silicon within a simple unified framework.     

Excitons in Si nanocrystals

The states of electron-hole pairs in spherical silicon nanocrystals are theoretically studied using the “multiband” effective-mass approximation in the limit of an infinitely high potential barrier at the boundary. The degeneracy of the states at the top of the valence band is taken into account in the spherical approximation, and the ellipsoidal character of the electronic spectrum in the conduction band is allowed for. Coulomb interaction-induced corrections to the energy of an electron-hole pair are found.     

Excitons in organic semiconductors

In this article, excitonic effects in organic semiconductors investigated within the framework of many-body perturbation theory are reviewed. As an example for this technologically relevant class of materials the oligoacene series is studied. The electron–hole interaction is included by solving the Bethe–Salpeter equation for the electron–hole Green's function. This approach allows for the evaluation of the exciton binding energies, which are of major interest concerning the application in organic opto-electronic devices. We start the discussion with a comparison of the Kohn–Sham band structure with recent angular resolved photo-emission data. Starting from this one-electron band structure we focus on the impact of the electron–hole interactions on the optical properties by solving the Bethe–Salpeter equation. We demonstrate the dependence of the exciton binding energy on the molecular size and emphasize the effect of the intermolecular interaction on the exciton binding energies by means of pressure investigations. To cite this article: P. Puschnig, C. Ambrosch-Draxl, C. R. Physique 10 (2009).     

Excitons in the polyenes

The excited electronic states of an infinite, all-trans, polyene are calculated using a Wannier function expansion. The relationship between these states and the excited electronic states of the finite polyenes, as found in molecular orbital configuration interaction studies, is explored.     

Excitons in quantum wires

This paper deals with excitons in quantum wires. We first study these excitons as the limit of excitons in D dimensions when . In order to do it, we have had to find a new resolution of the hydrogen atom Schrödinger equation: besides the fact that the usual resolution found in textbooks is not valid for D exactly equal to 1, it is, surprisingly enough, inconsistent since it relies on two hypergeometric functions which are not independent for the parameters of physical interest! In a second part, we write down the exact potential felt by the exciton relative motion along the wire in terms of the wire confinement. This allows a quite precise determination of the effective Coulomb potential for this 1D motion, which is of crucial importance to obtain a meaningfull finite value for the exciton ground state energy. In a last part, we study the dependence of the exciton energies on the wire area and anisotropy. While the quantitative results are here given for cylindrica l and rectangular wires with infinite barriers, we show how they can easily be extended to any particular wire shape and barrier height.Received: 5 August 2002, Published online: 23 July 2003PACS: 71.35.-y Excitons and related phenomena - 73.21.Hb Quantum wires     

Light scattering by aggregates of varying porosity and the opposition phenomena observed in the low-albedo particulate media

The rule that the opposition phenomena in brightness and linear polarization observed in many regolith surfaces usually accompany each other is violated in the cases of very dark asteroids and particulate samples: practically no nonlinear surge of brightness to opposition is observed while the branch of negative polarization at small phase angles exists. To explain this fact, we model the light scattering by particulate media with ensembles of spherical particles (with size comparable to the wavelength) of varying packing density and refractive index. The superposition T-matrix method is used. The increase in the absorption and/or packing density diminishes the amplitude of the brightness opposition peak, and its profile becomes wider. The influence on the branch of negative polarization is more complex and depends on the relation between the size parameters of the constituents, the refractive index, and the porosity. However, the feature common to all considered cases is that the negative branch changes its shape and the polarization minimum moves to the inversion point. This behavior radically differs from that observed in nonabsorbing ensembles of particles and reflects the fact that the efficiency of the coherent backscattering, which mainly determines these characteristics in nonabsorbing ensembles (to the packing density of about 30%), decreases. Moreover, since the angular profiles are not simply damped, but the polarization minimum changes its angular position, we may conclude that the near-field interaction of the constituents becomes important: the shielding of particles by each other eliminates many constituents from the scattering and the near-field effects promote the negative polarization and smooth the backscattering brightness surge. Due to this, when the packing density exceeds 10-20%, the opposition phenomena in absorbing ensembles are caused not only by the coherent backscattering, and situations, when the opposition brightness surge is practically suppressed, but the negative branch of polarization still survives, are possible. This may explain the fact that the dark regolith surfaces show no brightness opposition effect, but produce the branch of negative polarization with the minimum shifted from opposition.     

Single-molecule spectroscopy of molecular aggregates at low temperature

We have conducted single-molecule spectroscopy of a fluorescent polyphenylene dendrimer consisting of four peripheral perylenemonoimides which serve as energy donors and a central terrylenediimide which is the energy acceptor. After selective excitation of the donors the low-temperature emission spectra of single dendrimers show the purely electronic zero-phonon line as the most prominent feature of the acceptor. These sharp emission lines are subjected to appreciable spectral shifts. Fluorescence excitation spectroscopy of individual dendrimers in the spectral region of the donor absorption allows to extract energy transfer rates for single donors within the dendrimer. Although the energy transfer from perylenemonoimide to terrylenediimide is quite efficient, energy transfer between two proximate perylenemonoimides might be a competing process. This is shown by experiments with molecular dimers, in which two perylenemonoimides are held at a short distance by a benzil spacer.     

Excitons in GaAs quantum wells

This paper attempts to summarize some of the salient properties of excitons in GaAs quantum wells and in doing so it will emphasize work at AT&T Bell Labs with which the authors have been associated. Although the text relies heavily on published material, an effort has been made to stress new material, and where feasible, unpublished aspects, e.g., figures, related to earlier work. Topics discussed on the quasi-2D excitons in GaAs quantum well include: their inherent tendency for intrinsic free-exciton emission, exciton binding energies, bound and localized excitons including biexcitons and excitons bound to neutral impurities, effects of n- and p-type modulation and antimodulation doping, and the developments leading to a proposed set of quantum well parameters that results in acceptable fits to the observed exciton transitions for GaAs quantum wells with both square and parabolic potential profiles.     

Excitons in hybrid organic-inorganic nanostructures

In two-dimensional heterostructures made of semiconductor and organic layers, when resonance between the Wannier and Frenkel excitons is realized, the dipole-dipole interaction coupling them leads to novel effects. First, we discuss the pronounced nonlinear optical properties of the hybrid Frenkel-Wannier excitons appearing when the energy splitting of the excitonic spectrum is large compared to the exciton linewidths (the case of strong resonant coupling). Next, we consider the case of weak resonant coupling for which the Förster mechanism of energy transfer from an inorganic quantum well to an organic overlayer is of great interest: the electrical pumping of excitons in the semiconductor quantum well could be employed to turn on efficiently the organic material luminescence.     

光合作用体系捕光复合物线性和非线性光谱的理论研究：修正的Redfield方法的验证

使用数值精确的级联方程方法对其计算可靠性进行了验证．目前已知,修正的Redfield方法所用的微扰和马尔科夫近似,在中间耦合区对激发态能量转移会给出不正确的描述．因此研究其在计算各 种光谱信号时是否仍然有效有重要意义．利用不同参数下的二聚体模型和Fenna-Matthews-Olson复合物模型,使用级联方程方法和修正的Redfield方法,计算并比较了它们的吸收谱、发射谱和二维电子相干光谱．研究发现在较大的参数范围内两种方法给出一致的结果,这两种方法的对比也增进了对光合作用捕光复合物的2D光谱中量子拍频信号来源的认识．     

Spectral study on the molecular orientation of a tetracationic porphyrin dye on the surface of layered silicates

Tetracationic porphyrin dyes TMPyP and ZnPyP were intercalated into hydrophobized layered silicate films of three smectites. The smectites represented the layered silicate specimens of high (Fluorohectorite, Corning; FHT), medium (Kunipia F montmorillonite; KF) and low layer charge (Laponite, Laporte; LAP). The molecular orientations of the dye cations were studied by means of linearly-polarized ultraviolet-visible (UV-VIS) spectroscopy. The spectral analysis and consequent calculations of tilting angles of the transition moments at the wavelengths of Soret band transitions were in the range of 25°-35°. The determined angles indicated molecular orientation of the dye cations being almost parallel to the surface of the silicates. Slightly higher values (above 35°), determined for a FHT film, indicated either a slightly tilted orientation of the dye cations or the change of molecular comformation after the intercalation of the dye. Presented at 5-th International Conference Solid State Surfaces and Interfaces, November 19–24, 2006, Smolenice Castle, Slovakia     

Excitons in coupled quantum dots

Properties of excitons in vertically coupled GaAs/AlGaAs quantum dots were investigated using the variational method within the envelope function and effective mass approximations. It was found that when the thickness of the spacer layer becomes less than about one exciton Bohr radius, both the exciton binding energy and the fundamental optical transition energy are reduced compared to those in isolated quantum dots. This is a result of increased space extension of exciton due to the penetration of carrier wave functions into the spacer layer and corresponding reduction in confinement energy which dominates over the Coulomb interaction between the electron and the hole.     

Probability density function of the intensity scattered by Rayleigh-particle aggregates. Evolution with optical properties

We study the probability density function of the statistical fluctuations of the intensity scattered by an aggregate freely floating in space and constituted by Rayleigh particles under the dipole approximation. Its evolution as a function of the optical properties of the particles (polarizability) and their separation distance is analyzed. Aggregate geometries with two and three particles will be considered. The influence of the multiple scattering effect on the statistics of the scattered intensity is especially studied.     

Excitons in ZnO Quantum Wells

Physics of the Solid State - Reflectance and photoluminescence spectra of the ZnO/Zn0.78Mg0.22O structures with ZnO quantum wells and thick ZnO and Zn0.78Mg0.22O layers have been thoroughly...     

Excitons in quantum—dot quantum—well nanoparticles

A variational calculation is presented for the ground-state properties of excitons confined in spherical core-shell quantum-dot quantum-well (QDQW) nanoparticles. The relationship between the exciton states and structure parameters of QDQW nanoparticles is investigated, in which both the heavy-hole and the light-hole exciton states are considered. The results show that the confinement energies of the electron and hole states and the exciton binding energies depend sensitively on the well width and core radius of the QDQW structure. A detailed comparison between the heavy-hole and light-hole exciton states is given. Excellent agreement is found between experimental results and our calculated 1s_e－1s_h transition energies.