Specific features of the hybridization of Frenkel and Wannier–Mott excitons in a microcavity

Polariton states have been investigated in a microcavity, where the energy of the Frenkel exciton in an organic quantum well and the energy of the semiconductor Wannier–Mott exciton in an inorganic quantum well are close to the microcavity optical mode. It has been shown that the interaction of each of these excitons with the microcavity optical mode leads to their interaction with each other and to the formation of mutually coupled hybrid excitations. The influence of the location of the quantum wells in a microcavity on the spectra of hybrid states with different polarizations has been analyzed.     

Wilson chains are not thermal reservoirs

The effects of transverse electric field on the electronic structures, exciton states and excitonic absorption spectra in a cylindrical quantum wire are theoretically investigated in detail. The quantum wire is assumed to GaAs material surrounded by the infinite potential barrier. The results show that the external electric field removes the degeneracy of the electron or hole states. The energy levels of electron and hole, exciton binding energy, excitonic absorption coefficient and absorption energy decrease with increasing the strength of the electric field or the wire radius. The effects of the electric field become more significant for wide wires. The phenomena can be explained by the reduced spatial overlap of ground electron and hole states.     

Assessment of the coherent potential approximation for the absorption spectra of a one-dimensional Frenkel exciton system with a Gaussian distribution of fluctuations in the optical transition frequency

We investigate the accuracy of the coherent potential approximation (CPA) for the optical absorption spectra of a one-dimensional Frenkel exciton system with nearest-neighbor interactions and a Gaussian distribution of fluctuations in the optical transition frequency (diagonal Gaussian disorder). Our earlier studies have established that the CPA gives highly accurate results for the integral of the density of states of this system. In this paper we compare the CPA results for the normalized optical absorption with the finite-array calculations of Schreiber and Toyozawa and Schreiber for the same model. It is found that the CPA results for the absorption are in good agreement with their findings. It is pointed out that an expansion of the density of states in terms of the eigenstates of the ideal (no disorder) array contains a term proportional to the normalized absorption. Since the density of states is accurately approximated by the CPA, the presence of this term explains the success of the CPA in reproducing the absorption spectra. Our findings support the use of the Gaussian disorder model to interpret the absorption spectra of one and quasi-one dimensional exciton systems.     

用斯塔克光谱技术研究酞菁锡薄膜中的激子跃迁和电荷转移

采用斯塔克光谱技术研究了酞菁锡多晶薄膜中的激子跃迁和电荷转移。观察到一系列分子间电荷转移所形成的双分子激子谱带，显示了斯塔克光谱技术在探测淹没于弗伦克尔激子带下面的微弱电荷转移跃迁方面具有独特的优点和很高的灵敏度。     

Electromodulation spectroscopy of excitons: High field regime

The effects of electric field on excitons have been investigated experimentally by means of electroabsorption (EA). The behavior of excitons with ionization fields F_I of the same order of magnitude as or smaller than typical applied fields is reported. EA spectra associated with excitons in TlBr, PbI₂, BiI₃, trigonal Se, and α-monoclinic Se will illustrate this case. In this situation the EA signal arises principally from the effect on the exciton ground state, and no finer structure could be detected. The exciton ground state undergoes a shift to higher energies with the applied field. Characteristic dependences with field of the sizes, energy position of the peaks, and zero crossing points of the EA signals have been found. Estimates of exciton parameters can be readily obtained from the EA spectra. Unusual features of the exciton EA spectra PbI₂ are discussed. Qualitatively, at least, theoretical predictions are obeyed.     

Nonlinear absorption microspectroscopy of single perylene nanocrystals with a multichannel double lock-in amplifier

Nonlinear confocal absorption microspectroscopy of single nanocrystals at low temperatures was introduced in the study of perylene nanocrystals. By the stationary pump-probe method, single nanocrystals were photoexcited into metastable excited states, and difference absorption spectra due to excited-state absorption and ground-state depletion were simultaneously recorded using a multichannel lock-in amplifier. It was revealed that the free Frenkel exciton band for single perylene nanocrystals is broader in width than that for the bulk crystal at low temperatures, suggesting that the exciton band is inhomogeneously broadened even for single perylene nanocrystals.     

Hybrid excitons in organic–inorganic semiconducting quantum wells in a microcavity

We investigate theoretically the optical properties of composite organic–inorganic semiconductor quantum wells. These properties are dominated by hybrid Frenkel (or charge-transfer) and Wannier–Mott excitonic states. An important effect is the possibility of using the Stark shift to tune the resonance between Frenkel and Wannier–Mott excitons. This fact is very important from a practical point of view because it may be difficult to grow such a structure exactly at resonance. We also discussed the coupling of Frenkel or charge transfer and Wannier–Mott exciton through a microcavity photon. We evaluate the hybrid exciton-polariton Rabi splitting. In the strong coupling regime the Rabi splitting depends essentially on the oscillator strength of the Frenkel or charge-transfer exciton.     

Exciton binding energy and excitonic absorption spectra in a parabolic quantum wire under transverse electric field

The effects of transverse electric field on the energy levels of electron and heavy hole, exciton binding energy and excitonic absorption spectra of GaAs parabolic quantum wire are theoretically investigated in detail. The results indicate that the electron and hole energy levels, exciton binding energy, excitonic absorption coefficient and absorption energy becomes smaller with the increase of electric field. That is more significant at the condition of weaker parabolic confinement potential. The phenomena can be explained by the separation of overlap integral of the electron and hole at the ground states.     

Amplitude scaling behavior of band center states of Frenkel exciton chains with correlated off-diagonal disorder

We report the amplitude scaling behavior of Frenkel exciton chains with nearest-neighbor correlated off-diagonal random interactions. The band center spectrum and its localization properties are investigated through the integrated density of states and the inverse localization length. The correlated random interactions are produced through a binary sequence similar to the interactions in spin glass chains. We produced sets of data with different interaction strength and “wrong” sign concentrations that collapsed after scaling to the predictions of a theory developed earlier for Dirac fermions with random-varying mass. We found good agreement as the energy approaches the band center for a wide range of concentrations. We have also established the concentration dependence of the lowest order expansion coefficient of the scaling amplitudes for the correlated case. The correlation causes unusual behavior of the spectra, i.e., deviations from the Dyson-type singularity.     

Exciton dynamics in nanostar dendritic systems using a quantum master equation approach: core monomer effects and possibility of energy transport control

The directional energy transport, i.e. exciton migration, in nanostar dendritic systems composed of two-state monomer units is studied using a quantum master equation approach. We examine the effects of the variation in the excitation energy of the monomer in the core region (core monomer) on the multistep exciton migration from the periphery to the core based on the relaxation factors among exciton states originating in weak exciton-phonon coupling. It turns out that when the core monomer possesses both an excitation energy slightly lower than that of the first generation and a partial exciton overlap with the first generation, more efficient and rapid exciton migration to the core is expected as compared with other core monomer cases with the energy level closer to or much lower than that of the first generation.     

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.     

Exciton migration in a fluctuating medium I

A statistical mechanical theory of exciton migration in a fluctuating environment is developed with the use of the time-convolutionless equation formalism. This gives a satisfactory result when the stochastic perturbations acting on excitons are assumed to be Gaussian.Our theory is valid for any timescale and is applicable to the case of off-diagonal randomness as well as the diagonal randomness. For the Gaussian-Markoffian process, a basic equation can be solved analytically to give optical absorption spectra and the density of states. These quantities show systematic variations when certain characteristic parameters are changed.     

Discovery of bound exciton in ZnSe : Cu

A new bound exciton with the dissociation energy of 32 meV was observed in ZnSe : Cu by electroabsorption. The dependence of the electroabsorption peak on an electric field, the absorption and the photoluminescence spectra show that the bound exciton is associated with Cu²⁺.     

玻璃中CdSSe纳米晶体的光谱性能

对掺有镉、硒、硫的玻璃在650—800℃退火4?h，生长了不同尺寸的CdS0.13Se0.87纳米晶体，测量了纳米晶体的吸收光谱、光致发光（PL）谱和电调制光谱，确定了纳米晶体部分电子态的能量，讨论了CdSSe纳米晶体的光学性质与其尺寸之间的依赖关系.随着纳米晶体尺寸的增大，对应激子的吸收峰、PL峰及电吸收信号发生红移，表现出明显的量子尺寸效应.小尺寸纳米晶体的电吸收表现为量子受限的Stark效应，而大尺寸纳米晶体的电吸收线形与体材料的相似；随着纳米晶体尺寸的增大，电吸收信号增强.所有尺寸的纳米晶体都表现 关键词： CdSSe纳米晶体 吸收光谱 光致发光谱 电光响应     

Elucidation of the electronic structure of semiconducting single-walled carbon nanotubes by electroabsorption spectroscopy

We report benchmark calculations of electroabsorption in semiconducting single-walled carbon nanotubes that provide motivation to perform electroabsorption measurement on these systems. We show that electroabsorption can detect the continuum bands in different energy manifolds. Direct determination of the binding energies of excitons in higher manifolds thereby becomes possible. We also find that electroabsorption can provide evidence for Fano-type coupling between the second exciton and the lowest continuum band states.     

Backscattering of light by a finite two-dimensional crystal plate in the region of exciton resonance: Antispecular reflection

It is shown that scattering of a plane monochromatic wave by a finite two-dimensional crystal (quantum well or Langmuir-Blodgett film) in the region of exciton resonance shows, along with the peak of specular reflection, a peak of comparable magnitude corresponding to backward scattering propagating toward the incident beam (antispecular reflection). The effect is related to reflection of the exciton by the boundary of the two-dimensional crystal. The solution of the scattering problem for a simple model system with a Frenkel exciton, demonstrating this phenomenon, is given.     

Non-radiative transformation of a singlet exciton into a triplet one in organic molecular crystals

The probability of non-radiative transformation of a singlet exciton into a triplet one in organic molecular crystals is calculated. Mechanisms caused by intermolecular interactions apparent at grouping molecules into a crystal together with spin-orbital molecular interactions are considered as mechanisms of non-radiative transformation. Dependence of the calculated probability on the temperature and the character of an energetic spectrum of a singlet and a triplet exciton is discussed. On the basis of the calculated probabilities for various specific mechanisms the influence of intermolecular interactions, when arranging molecules into a crystal, on the intensity of non-radiative transitions between singlet and triplet excited states of molecules in the crystal is analyzed.Na Slovance 2, Praha 8, Czechoslovakia.