Picosecond excitonic luminescence in ZnO and other wide-gap semiconductors

Radiative lifetimes of free-atom transitions, scaled by ω³ for comparison at 368 nm, are not faster than about 6.9 ns. BaF₂ core-valence luminescence, scaled in the same way from 220 to 368 nm, corresponds to 4.1 ns. In contrast, excitonic transitions in wide-gap semiconductors display subnanosecond radiative lifetimes, and in particular ZnO has radiative lifetimes measured at 50–300 ps for D^o,X and 400–900 ps for free excitons. The “giant oscillator strength” corresponding to these lifetimes can be explained by theories developed initially for defect-bound excitons, then quantum wells, and nanoparticles. An exciton is a coherent array of N dipoles, where N is the number of sites covered by coherent translational motion of the exciton. This is not essentially a phenomenon of multiple excitons, but applies as well to single-exciton decay. It differs in that regard from the more familiar Dicke giant dipole of N coherently excited atoms lacking translational periodicity. The phenomenon suggests possibilities for achieving ultrafast scintillators and high light yield.     

Ⅲ-Ⅴ族化合物中氮束缚激子发光的动力学研究

用发光动力学的分析方法,研究了Ⅲ—Ⅴ族化合物中N束缚激子的发光强度与温度的关系,得到的理论公式与实验结果符合得较好。我们的分析指出,由于无辐射能量传递的存在,束缚激子的△J=2跃迁的发光效率低于△J=1跃迁的发光效率,致使低温(T<50K)下束缚激子的发光强度可能随温度的下降而变弱。另外,N杂质对自由激子再俘获的可能性的大小直接影响束缚激子发光的热猝灭过程:束缚激子可能因热离解成自由激子或自由的电子和空穴。我们找到了区分这两类情况的条件。     

Exciton absorption of light in a smooth random field

A study is made of interband absorption of light in a smooth random field that varies slowly in space. When the exciton energy in the random field is much less than the exciton binding energy, the influence of the random field on the discrete spectrum of the exciton is expressed through the appearance of an exponential “tail” to every exciton line. But if the exciton energy in the random field is much greater than the exciton binding energy, the exciton effects are unimportant because the random field breaks up the excitons.     

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.     

Theory and ab initio calculation of radiative lifetime of excitons in semiconducting carbon nanotubes

We present a theoretical analysis and first-principles calculation of the radiative lifetime of excitons in semiconducting carbon nanotubes. An intrinsic lifetime of the order of 10 ps is computed for the lowest optically active bright excitons. The intrinsic lifetime is, however, a rapid increasing function of the exciton momentum. Moreover, the electronic structure of the nanotubes dictates the existence of dark excitons near in energy to each bright exciton. Both effects strongly influence measured lifetime. Assuming a thermal occupation of bright and dark exciton bands, we find an effective lifetime of the order of 10 ns at room temperature, in good accord with recent experiments.     

Photon Echo from Localized Excitons in Semiconductor Nanostructures

An overview on photon echo spectroscopy under resonant excitation of the exciton complexes in semiconductor nanostructures is presented. The use of four-wave-mixing technique with the pulsed excitation and heterodyne detection allowed us to measure the coherent response of the system with the picosecond time resolution. It is shown that, for resonant selective pulsed excitation of the localized exciton complexes, the coherent signal is represented by the photon echoes due to the inhomogeneous broadening of the optical transitions. In case of resonant excitation of the trions or donor-bound excitons, the Zeeman splitting of the resident electron ground state levels under the applied transverse magnetic field results in quantum beats of photon echo amplitude at the Larmor precession frequency. Application of magnetic field makes it possible to transfer coherently the optical excitation into the spin ensemble of the resident electrons and to observe a long-lived photon echo signal. The described technique can be used as a high-resolution spectroscopy of the energy splittings in the ground state of the system. Next, we consider the Rabi oscillations and their damping under excitation with intensive optical pulses for the excitons complexes with a different degree of localization. It is shown that damping of the echo signal with increase of the excitation pulse intensity is strongly manifested for excitons, while on trions and donor-bound excitons this effect is substantially weaker.     

镓铟磷三元化合物中的自由激子和杂质N发光中心的结构位形

我们研究了GaxIn1-xP:N(x=0.99,0.98,0.96)的发光光谱,用Ar+离子激光器的458nm线激发。N的浓度为5×1017cm-3。图1示出了在6K下Ga0.99In0.01P:N的发光光谱。Mariette和Chevallier[1,2]以及Nelson和Holonyak,Jr[3]。认为Nx0带起源于束缚在孤立N中心上激子的辐射复合。     

Linear and nonlinear optical properties of excitons in semiconductor quantum wells and microcavities

Linear and nonlinear light propagation in single and multiple quantum wells and in semiconductor microresonators are studied on the basis of Maxwell’s equations. The treatment includes radiative broadening of quantum-confined excitons, radiative coupling between quantum wells as well as coupling of quantum wells to the cavity field of a microresonator for steady state or ultrashort pulse excitation. The dynamical evolution of the coherent quantum-well polarization under the influence of many-body effects is studied within a microscopic model. The theory is used to investigate the influence of exciton saturation and dephasing on pulse propagation and excitonic normal-mode coupling.     

Polariton-mode lasing and Bose condensate of dipolar excitons in heterostructures

The analysis of the polariton modes in 2D traps based on heterostructures with quantum wells for Bose-Einstein condensation of dipolar excitons is presented. The characteristic equation of such modes is derived with allowance for the polarization relaxation of excitons and radiative losses from the trap. The spectrum and structure of high-quality modes are analytically and numerically studied. It is demonstrated that several modes become unstable at a high enough density of excitons and a long relaxation time of the exciton polarization. In accordance with the estimations, such an instability can be reached in the experiments on the Bose-Einstein condensation of dipolar excitons and can be used to interpret the corresponding coherent emission.     

多组分纠缠在光子晶体中的存储

研究了激子的多组分纠缠相干态保真度在各向异性光子晶体中的演化行为.结果表明,当激子的跃迁频率处于光子晶体带隙时,保真度随时间变化作周期振荡,这与激子处于真空环境时,保真度振荡衰减的演化行为不同.此外,当激子跃迁频率离光子晶体带边较远时,其多组分纠缠相干态越容易被保存.     

Optoelectronic characteristics of CdTe/HgTe/CdTe quantum-dot quantum-well nanoparticles

Optoelectronic characteristics of CdTe/HgTe/CdTe quantum-dot quantum-well (QDQW) nanoparticles synthesized by the colloidal method are investigated in this study. Strong exciton bands were observed in absorption and photoluminescence (PL) spectra taken for the CdTe/HgTe/CdTe QDQW nanoparticles. The energy difference between the exciton absorption and PL bands is larger than those obtained with CdTe and HgTe nanoparticles. Photocurrent-voltage curves and time-dependent photocurrent curves were obtained for the CdTe/HgTe/CdTe QDQW nanoparticles. With regard to the photocurrent mechanism of these QDQW nanoparticles, those charge carriers participating in the formation of excitons may not contribute to the photocurrent, because of the large binding energy of the excitons. Moreover, it is suggested in this paper that free holes in the HgTe quantum-well in the valance band, rather than free electrons, are the main contributors to the photocurrent.     

Interwell excitons in GaAs/AlGaAs double quantum wells and their collective properties

Luminescence spectra of interwell excitons in GaAs/AlGaAs double quantum wells with electric-field-tilted bands (n-i-n) structures were studied. In these structures the electron and the hole in the interwell exciton are spatially separated between neighboring quantum wells by a narrow AlAs barrier. Under resonant excitation by circularly polarized light the luminescence line of the interwell excitons exhibited appreciable narrowing as their concentration increased and the degree of circular polarization of the photoluminescence increased substantially. Under resonant excitation by linearly polarized light the alignment of the interwell excitons increased as a threshold process with increasing optical pumping. By analyzing time-resolved spectra and the kinetics of the photoluminescence intensity under pulsed excitation it was established that under these conditions the rate of radiative recombination increases substantially. The observed effect occurs at below-critical temperatures and is interpreted in terms of the collective behavior of the interwell excitons. Studies of the luminescence spectra in a magnetic field showed that the collective exciton phase is dielectric and in this phase the interwell excitons retain their individual properties.     

Cathodoluminescence of iodine dimers in KCl:I crystals

Radiative characteristics of localized exciton states in a KCl:I crystal have been studied in the temperature range 27–200 K by pulsed optical spectroscopy with nanosecond-range time resolution. Besides the bands investigated earlier in KCl:I crystals at impurity concentrations above 0.1 mol %, a strong band peaked at 3.8 eV was detected. The temperature dependences of the decay times, amplitude values of the intensity, and light sums of the 3.8-and 3.4-eV bands were studied. These bands are shown to originate from radiative decay of localized excitons bound to the impurity dimers.     

Optical nonlinearities in GaSe and InSe crystals upon laser excitation

The nonlinear absorption of light and its temporal evolution in the vicinity of exciton resonance in layered GaSe and InSe crystals under high optical excitation have been experimentally investigated. The decisive factor for the observed temporal dependence of the absorption coefficient and its dependence on the excitation intensity is screening excitons by nonequilibrium-carrier plasma. It is shown that the increase in the transmittance in the absorption-band edge in GaSe with a simultaneous blue shift of the band edge is caused by filling the energy bands under high optical excitation.     

Stimulated light backscattering from exciton Bose condensate

A new effect—light backscattering from exciton Bose-condensate—is considered. This effect is connected with the photoinduced coherent recombination of two excitons in the condensate with the production of two photons with opposite momenta. The effect of two-exciton coherent recombination leads also to the appearance of the second-order coherence in exciton luminescence connected with squeezing between photon states with opposite momenta. The estimations given for Cu₂O and GaAs excitons show that the effect of stimulated light backscattering can be detected experimentally. Moreover, in the system of 2D excitons in coupled quantum wells, the effect of stimulated anomalous light transmission must also take place. Anologous effects can also take place in systems of Bose-condensed atoms in excited (but metastable) states.     

The Paths of Excitation Energy Deactivation in LH1 Reduced Mutant and Wild-Type Strains of Rhodobacter sphaeroides

The P3 mutant of Rhodobacter sphaeroides had an altered ratio of reaction center to core (LH1) and peripheral (LH2) antenna complexes compared to the wild-type strain. Intracytoplasmic membranes from these two strains were purified and then resuspended in buffer or immobilized in isotropic and stretched polymer film. The absorption, photoacoustic, and delayed luminescence spectra were measured. The ratios of infrared absorption and photoacoustic bands (located at about 880 nm for LH1 and at 850 and about 800 nm for LH2) as well as the half-width of these bands are different for the LH2 and LH1 mutants and wild-type strain. The whole yields of thermal deactivation of the two strains were comparable, but in the absorption region of LH2 it was slightly lower in the case of the mutant than for the wild-type strain. The delayed luminescence main maxima were observed at about 860 and 700 nm. The first one could be due to emission of bacteriochlorophyll a of LH2 complexes. The emission at about 700 nm is probably due to dihydromesochlorophyll, which is usually, to some extent, produced from bacteriochlorophyll a in bacterial complexes. The delayed luminescence emission is competing with excitation energy transfer to the reaction center. The intensity of the delayed luminescence of the mutant strain was higher than that of the wild-type strain when both samples were excited in a region of carotenoid absorption. The mutant contains less carotenoids than the wild-type strain. Carotenoids work as efficient antenna. When they at a lower concentration the excitation can be trapped more easily by some chlorophyll-like pigment isolated from the excitation energy chain. The dependences of delayed luminescence spectra on the light polarization and excitation wavelengths for the wild-type strain and for the mutant were different. The anisotropy of delayed luminescence showed that bacteriochlorophyll a molecules of different orientations were contributing to the mutant and the wild-type strain emission. All the results suggest that the excitation energy transfer from the antenna to the reaction center in the mutant and the wild-type strain is similar.     

Weak exciton scattering in molecular nanotubes revealed by double-quantum two-dimensional electronic spectroscopy

The two-exciton manifold of a double-wall cylindrical molecular aggregate is studied using a coherent third order optical technique. Experiments reveal the anharmonic character of the exciton bands. Atomistic simulations of the exciton-exciton scattering show that the excitons can be treated as weakly coupled hard-core bosons. The weak coupling stems from the extended exciton delocalization made possible by the nanotube geometry.     

Exciton-polariton absorption in periodic and disordered quantum-well chains

The exciton-polariton transfer and absorption in regular and disordered structures with a finite number of quantum wells are studied theoretically. The transfer matrix method is invoked in the exciton resonance region to calculate the reflectivity, transmissivity, and absorptivity spectra, as well as the integrated absorptivity as a function of the γ/Γ₀ ratio of the parameters of nonradiative and radiative damping of quasi-two-dimensional excitons. It is shown that the integrated absorptivity as a function of γ (temperature) follows a universal pattern, more specifically, it increases monotonically from zero at γ = 0 to saturate at γ/Γ₀ ? 1. Because the exciton-polariton absorption being single mode, the integrated absorptivity in Bragg quantum-well structures is substantially lower than that in short-period structures, in which absorption involves the whole spectral multitude of modes. The intrawell disorder associated with fluctuations in the frequencies of exciton excitation in quantum wells enhances the integrated absorptivity to the level typical of light absorption with no resonance among excitons of different quantum wells. The interwell disorder originating from fluctuations in quantum-well separation likewise leads to an increase in the integrated absorptivity.     

Radiative recombination of excitons in semiconductors at high excitation intensities

The shape of the exciton luminescence band of the gaseous phase of free excitons in crystal Si is investigated under high level excitation. Only the exciton-exciton interaction is considered and the influence of collisions of excitons with phonons and electrons is not taken into account. The theoretical shape of the exciton luminescence band qualitatively agrees with experiment. The process of the radiative Auger-recombination of two indirect excitons without the participation of phonons is studied in Ge and Si. The expression for the frequency and temperature dependence of the probability of radiation is obtained. The band has the asymmetrical Gaussian form with the steep short-wave tail. The predicted luminescence band in Ge is shifted at the long-wavelength side from the well-known exciton luminescence bands with participation of the phonons. The selection rules for the probability amplitude of the process under consideration are obtained.     

Spin Physics of Excitons in Colloidal Nanocrystals

We present a review of spin-dependent properties of excitons in semiconductor colloidal nanocrystals. The photoluminescences (PL) properties of neutral and charged excitons (trions) are compared. The mechanisms and the polarization of radiative recombination of a “dark” (spin-forbidden) exciton that determines the low-temperature PL of colloidal nanocrystals are discussed in detail. The radiative recombination of a dark exciton becomes possible as a result of simultaneous flips of the surface spin and electron spin in a dark exciton that leads to admixture of bright exciton states. This recombination mechanism is effective in the case of a disordered state of the spin system and is suppressed if the polaron ferromagnetic state forms. The conditions and various mechanisms of formation of the spin polaron state and possibilities of its experimental detection are discussed. The experimental and theoretical studies of magnetic field-induced circular polarization of PL in ensembles of colloidal nanocrystals are reviewed.