Scaling and universality in the optics of disordered exciton chains

The joint probability distribution of exciton energies and transition dipole moments determines a variety of optical observables in disordered exciton systems. We demonstrate numerically that this distribution obeys a one-parameter scaling, originating from the fact that both the energy and the dipole moment are determined by the number of coherently bound molecules. A universal underlying distribution is found, which is identical for uncorrelated Gaussian disorder in the molecular transition energies or in the intermolecular transfer interactions. The universality breaks down for disorder in the transfer interactions resulting from variations in the molecular positions. We suggest the possibility to probe the joint distribution by means of single-molecule spectroscopy.     

Exciton trapping, binding and diamagnetic shift in T-shaped quantum wires

We determine the exciton states of T-shaped quantum wires. We use anisotropic effective-mass models to describe the electron and hole states. Pair correlation along the wire axis and in the lateral directions is included. We accurately model the measured redshifts between exciton photoluminescence in quantum wells and T-shaped wires. This redshift arises from enhanced exciton binding and the difference between well and wire confinement energy. We predict a large enhancement of binding energy only when lateral correlation is included, indicating that T-shaped wires arequasirather thanquantum1D wires. We calculate exciton shapes and diamagnetic shifts to determine how the exciton is distorted when confined in a T-wire.     

Polarization spectra of excitonic luminescence of bare ZnCdSe/ZnSe quantum wires

Linearly polarized luminescence spectra of bare (unburied) semiconductor structures with ZnCdSe/ZnSe quantum wires, obtained by reactive ion etching, were investigated. It was found that, regardless of the orientation of the linear polarization of the exciting light, the luminescence radiation of the quantum wires is polarized parallel to the axis of the wires, while the radiation of the buffer layer of the isotropic ZnSe barrier material is oriented perpendicular to the axis of the wires. The polarization features found are due to the modification of the modes of the electromagnetic field near open quantum wires, which occurs as a result of the presence of the vertical interfaces between media with strongly different permittivities. It was also found that, when linearly polarized excitation is used, the alignment of exciton dipole moments strongly influences the polarization properties of the luminescence. Fiz. Tverd. Tela (St. Petersburg) 40, 1559–1562 (August 1998)     

Exciton self-trapping in molecular media with an elastic dipole moment

Exciton self-trapping in a molecular medium is considered within a self-consistent model taking into account the change in the dipole moment as a result of a displacement of molecules and the resonance interaction with an electromagnetic field. New mechanisms and specific features of the formation of localized structures in quasi-one-dimensional molecular structures are investigated. It is shown that the dependence of the dipole moment on molecular vibrations leads to new conditions for exciton self-trapping and intrinsic optical bistability, as well as for the formation of electromagnetically induced transparency. The theory proposed is used to explain the specific features of exciton self-trapping in a conjugated polymer and J aggregates of dyes under the action of an external laser field.     

Determination of a merocyanine J-aggregate structure and the significant contribution of the electric dipole interaction to the exciton band wavelength

The molecular alignment of a merocyanine (MC) J-aggregate monolayer at the air-water interface was determined by a grazing incidence x-ray diffraction method. The obtained molecular arrangement apparently shows that the conventional formula, which accounts only for the transition dipole interaction, is not sufficient to figure out the exciton band wavelength, suggesting the importance of the electric dipole (ED) interaction. We derived a simple formula for the ED interaction energy under an extended dipole approximation and clarified the ED contribution in the MC J aggregate.     

Exciton-photon interaction in low-dimensional semiconductor microcavities

The structure of the photon states and dispersion of cavity polaritons in semiconductor microcavities with two-dimensional optical confinement (photon wires), fabricated from planar Bragg structures with a quantum well in the active layer, are investigated by measuring the angular dependence of the photoluminescence spectra. The size quantization of light due to the wavelength-commensurate lateral dimension of the cavity causes additional photon modes to appear. The dispersion of polaritons in photon wires is found to agree qualitatively with the prediction for wires having an ideal quantum well, for which the spectrum is formed by pairwise interaction between exciton and photon modes of like spatial symmetry. The weak influence of the exciton symmetry-breaking random potential in the quantum well indicates a mechanism of polariton production through light-induced collective exciton states. This phenomenon is possible because the light wavelength is large in comparison with the exciton radius and the dephasing time of the collective exciton state is long. Zh. éksp. Teor. Fiz. 114, 1329–1345 (October 1998)     

Solitary Frenkel Excitons in One-Dimensional Molecular Aggregates with Static Dipole Moment

It is shown theoretically that solitary Frenkel excitons in one-dimensional molecular aggregates can exist and propagate when the Frenkel exciton is accompanied by a static dipole moment along the aggregate axis.     

The temperature dependence of the photoluminescence from overgrown GaAs/Al0.3Ga0.7As quantum dots and wires

Photoluminescence measurements on GaAs/Al_0.3Ga_0.7As quantum dots and wires fabricated using electron bears lithography and reactive ion etching are reported both before and after regrowth with a layer of Al_0.4Ga_0.6As. Dots exhibit little change in luminescence efficiency from the bulk with a reduction in diameter either before or after regrowth. Surface recombination therefore appears to be suppressed. In wires, however, luminescence intensity is very sensitive to wire width, decreasing rapidly with this parameter, but recovers and becomes independent of size after overgrowth. The temperature dependence of the photoluminescence from the dots and wires showed that dots and wires less than 150nm in width luminesced to higher temperatures than the larger diameter structures and dots liminesced to higher temperatures than wires of comparable width. This suggests that there is a finite coherence area effect which increases the radiative lifetimes of excitons in the quantum structures due to the geometric constraint, in the lateral direction in the wires and in all three directions in the dots. Below 20K bound exciton luminescence dominates in the dots but not in the wires. In wires it is still possible for the excitons to diffuse to nonradiative sites within the exciton lifetime. Regrowth at 750°C causes migration of aluminium into the quantum well and causes the shape of the well to become parabolic resulting shifts in the exciton emission to shorter wavelengths, making it difficult to separate the effect of processing from those due to quantum confinement.     

Broadening of triplet-triplet absorption band in molecular structures with different spatial dimensionalities

Within the framework of a dipole approximation, the form of the light absorption band for exciton transitions between triplet zones in one-, two-, and three-dimensional periodic molecular structures is calculated. Allowance is made for exciton attenuation as a frequency-independent parameter. The analytical expressions obtained make it possible to analyze the band for molecular structures of different spatial dimensionalities as a function of the difference in bandwidths, attenuation, and lattice temperature. Institute of the Surface Chemistry, National Academy of Sciences of Ukraine, 31, Nauka Ave., Kiev 252022, Ukraine. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 64, No. 5, pp. 586–590, September–October, 1997.     

Quantum wire lasers with high uniformity formed by cleaved-edge overgrowth with growth-interrupt anneal

High-quality T-shaped quantum wire lasers are fabricated by cleaved-edge overgrowth with the molecular beam epitaxy on the interface improved by a growth-interrupt high-temperature anneal. Micro-photoluminescence (PL) and PL excitation spectroscopy reveals unprecedented high quality of the wires, and structures of one-dimensional (1D) free excitons and 1D continuum states. At high pumping levels, PL evolves from a sharp free exciton peak via a biexciton peak to a red-shifted broad band. Lasing has been achieved with low lasing threshold. The lasing energy is on the red-shifted broad band and is about 5 meV below the free exciton. The observed shift excludes free excitons in lasing, and suggests contribution of highly Coulomb-correlated electron-hole plasma.     

Ultrafast exciton relaxation in microcrystalline pentacene films

The exciton dynamics in microcrystalline pentacene films is investigated by transient absorption measurements with 30 fs time resolution. It is found that the emission from photoexcited Frenkel excitons decays within 70 fs due to the ultrafast formation of an excitonic species with a strongly reduced transition dipole to the ground state and an absorption dipole in the plane of the film. We propose that an excimer exciton is formed and stabilized by changes of the local crystal structure. The subsequent dynamics is dominated by diffusion controlled annihilation and trapping.     

Temperature dependent time-resolved exciton luminescence in GaAs/AlGaAs quantum wires and dots

Transient photoluminescence of GaAs/AlGaAs quantum wires and quantum dots formed by strain confinement is studied as a function of temperature. At low temperature, luminescent decay times of the wires and dots correspond to the radiative decay times of localized excitons. The radiative decay time can be either longer or shorter than that of the host quantum well, depending on the size of the wires and dots. For small wires and dots (∼ 100 nm stressor), the exciton radiative recombination rate increases due to lateral confinement. Exciton localization due to the fluctuation of quantum well thickness plays an important role in the temperature dependence of luminescent decay time and exciton transfer in quantum wire and dot structures up to at least ∼ 80 K. Lateral exciton transfer in quantum wire and dot structures formed by laterally patterning quantum wells strongly affects the dynamics of wire and dot luminescence. The relaxation time of hot excitons increases with the depth of strain confinement, but we find no convincing evidence that it is significantly slower in quasi 1-D or 0-D systems than in quantum wells.     

Exciton delocalization and superradiance in tetracene thin films and nanoaggregates

The structure and dynamics of luminescent excitons in tetracene thin films and nanoaggregates are investigated using time-resolved spectroscopy and theoretical calculations. The orientation of tetracene's transition dipole moment along its short molecular axis leads to properties qualitatively different from those observed in aggregates of phenylene-vinylene and thiophene oligomers, despite similar crystal structures. The spectral shape, temperature dependence, and radiative lifetime are consistent with a short-lived superradiant exciton delocalized over approximately 10 tetracene molecules.     

Linear and nonlinear excitonic absorption in semiconducting quantum wires crystallized in a dielectric matrix

Spectra of linear and nonlinear absorption of GaAs and CdSe semiconducting quantum wires crystallized in a transparent dielectric matrix (inside chrysotile-asbestos nanotubes) have been measured. Their features are interpreted in terms of excitonic transitions and filling of the exciton phase space in the quantum wires. The theoretical model presented here has allowed us to calculate the energies of excitonic transitions that are in qualitative agreement with experimental data. The calculated exciton binding energies in quantum wires are a factor of several tens higher than in bulk semiconductors. The cause of this increase in the exciton binding energy is not only the size quantization, but also the “dielectric enhancement,” i.e., stronger attraction between electrons and holes owing to the large difference between permittivities of the semiconductor and dielectric matrix. Zh. éksp. Teor. Fiz. 114, 700–710 (August 1998)     

Exciton effects on nonlinear electro-optic effects in semi-parabolic quantum wires

The nonlinear electro-optic effects in quasi-one-dimensional semi-parabolic quantum wires are studied, in which the exciton effects are taken into account. The analytical expression of the electro-optic co-efficient is derived by compact density-matrix approach. Finally, the numerical results are presented for GaAs/AlGaAs semi-parabolic quantum wires. The results show that the electro-optic coefficient is over two times bigger than that obtained by without considering exciton effects. Furthermore, the electro-optic coefficient is related to the relaxation time.     

The anisotropy of fluorescence in ring units III: Tangential versus radial dipole arrangement

The time dependence of the anisotropy of fluorescence can indicate the coherent exciton transfer regime in molecular rings. We are comparing time development of this quantity after an impulsive excitation obtained for the ring models of bacterial antenna complexes with tangential and radial optical transition dipole moments arrangement as in nonameric LH2 and octameric LH4 units. We use non-correlated static Gaussian disorder in the local exciton energies. We take into account simultaneously dynamic disorder using a Markovian treatment of the interaction with the bath. We show that the influence of dynamic disorder on difference of the anisotropy of fluorescence is more important then the influence of static disorder in consequence of different band width.     

Coulomb Drag of Dipole Excitons in a Hybrid Exciton–Electron System

The effect of Coulomb drag on a gas of dipole excitons in spatially separated two-dimensional quantum wells containing electron and exciton gases is studied theoretically. The Coulomb drag of excitons can be used to control exciton transport in transistor structures whose active element is a two-dimensional gas of dipole excitons. Expressions for the exciton cross conductivity as a function of temperature are obtained for the diffusion and ballistic transport regimes. For each regime, the limiting cases in terms of the ratio of the Coulomb interaction screening length to the distance between the gases are analyzed. It is shown that, at temperatures exceeding considerably the exciton-gas degeneracy temperature, the cross conductivity is independent of the temperature, while in the opposite case it vanishes exponentially.     

Real-time spectroscopy of Frenkel exciton system

We performed selective excitations of the first- and second-excited Frenkel exciton states (Q- and B-excitons) with use of sub-40-fs and sub-5-fs visible laser pulses. The transient absorption signals exhibit oscillatory features associated with molecular vibrations. From an analysis of the spectral profiles of the phase and amplitude of the oscillation, the experimental result is well explained by the modulated transition dipole moment, which is caused by the dynamic intensity borrowing from the intense B-transition to the weak Q-transition.     

Localization-dependent photoluminescence spectrum of biexcitons in semiconductor quantum wires

We study exciton and biexciton spectra in disordered semiconductor quantum wires by means of nanophotoluminescence spectroscopy. We demonstrate a close link between the exciton localization length along the wire and the occurrence of a biexciton spectral line. The biexciton signature appears only if the corresponding exciton state extends over more than a few tens of nanometers. We also measure a nonmonotonous variation of the biexciton binding energy with decreasing exciton localization length. This behavior is quantitatively well reproduced by the solution of the single-band Schr?dinger equation of the four-particle problem in a one-dimensional confining potential.     

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.