自旋极化度对GaAs量子阱中吸收饱和效应与载流子复合动力学的影响研究

本文研究了(001) GaAs量子阱薄膜中重空穴激子近共振抽运-探测的载流子自旋弛豫动力学, 发现载流子的自旋极化对传统的线偏振光吸收饱和效应和载流子复合动力学都有影响. 进一步的抽运流依赖的自旋弛豫和复合动力学研究表明, 自旋极化对线偏振光的吸收饱和效应的影响随抽运流降低而变弱. 在低激发流时, 自旋极化对线偏振吸收饱和效应的影响才可忽略. 然而, 又显现出自旋极化对复合动力学的影响. 分析表明复合动力学的自旋极化依赖性起源于重空穴激子形成浓度的自旋极化依赖性. 复合动力学的自旋极化依赖性表明自旋弛豫时间计算中所涉及的复合时间应该使用自旋极化载流子的复合时间. 基于二维质量作用定律的激子浓度计算表明, 库仑屏蔽效应对激子形成的影响在较低激发载流子浓度下可以忽略.     

Exciton warming in III–V semiconductors and microcavities

We present a time resolved experiment in which we dynamically tailor the occupation and temperature of a photogenerated exciton distribution in QWs by excitation with two delayed picosecond pulses. The modification of the excitonic distribution results in ultrafast changes in the PL dynamics. Our experimental results are well accounted by a quasiequilibrium thermodynamical model, which includes the occupation and momentum distribution of the excitons. We use this model and the two-pulse experimental technique to study the polariton dynamics in InGaAs-based microcavities in the strong coupling regime. In particular, we demonstrate that resonantly injected upper polaritons mainly relax to the lower polariton branch via scattering to large momentum polariton states, producing the warming of the polariton reservoir.     

Exciton-exciton collisions and conversion of interwell excitons in GaAs/AlGaAs superlattices

The ratio of the densities of intra-and interwell excitons in a symmetric system of coupled quantum wells — a superlattice based on a GaAs/AlGaAs heterostructure — is investigated over a wide range of optical excitation power densities. Conversion of interwell excitons into intrawell excitons as a result of exciton-exciton collisions is observed at high exciton densities. Direct evidence for such a conversion mechanism is the square-root dependence of the interwell exciton density on the optical excitation level. The decrease in the lifetime of interwell excitons with increasing excitation density, as measured directly by time-resolved spectroscopy methods, confirms the explanation proposed for the effect. Pis’ma Zh. éksp. Teor. Fiz. 65, No. 8, 623–628 (25 April 1997)     

Relaxation time for a charge carrier due to its scattering from other charge carriers in superlattices

A calculation of relaxation time for (i) electron–electron scattering in a modulation-doped superlattice of type-I and (ii) electron–electron, hole–hole and electron–hole scattering processes in a compositional superlattice of type-II has been performed, using Fermi's golden rule. As compared to a two-dimensional electron gas system, both intralayer and interlayer interactions, between charge carriers in a superlattice, contribute to relaxation time. It is found that scattering processes at all possible value of momentum transfer contribute to relaxation time, for a given value of temperature and carrier density. We further find interlayer interactions in a superlattice make a significant contribution to relaxation time. Relaxation time is found to decrease on increasing temperature, carrier density and single particle energy, in a superlattice. The computed relaxation time for an electron (hole) in a superlattice enhances on increasing the width of layer consisting of electrons (holes). The electron–hole (hole–electron) scattering process in a type-II superlattice yields maximum contribution to the relaxation time when a hole layer lies exactly in between two consecutive electron layers.     

Influence of acoustic phonons on dephasing of free excitons in quantum wells

A theory of the dephasing rate of quasi-2D free excitons due to acoustic phonon interaction at low exciton densities is presented. Both deformation potential and piezoelectric couplings are considered for the exciton–phonon interaction in quantum wells. Using the derived interaction Hamiltonian obtained recently by us, exciton linewidth and dephasing rate are calculated as a function of the exciton density, exciton temperature, exciton momentum and lattice temperature.     

Interwell excitons in GaAs superlattices

The formation of spatially indirect excitons in superlattices with narrow minibands is investigated experimentally. The interwell exciton is similar to the first Wannier–Stark localized exciton of an electrically biased superlattice. However, in the present case the localization is mediated by the Coulomb interaction of the electron and the hole without external fields.     

Femtosecond time-resolved interferences of resonantly excited excitons in bulk GaN

It is shown that excitonic transients of bulk GaN can be accurately measured by an interferometric correlation technique used in reflection geometry. This is demonstrated for resonantly excited excitons in high quality GaN epilayers. The interferograms exhibit a clear modulation of the signal due the quantum beats between A and B excitons. The period of these beats is in good agreement with the A–B exciton energy splitting measured by means of frequency-resolved reflectivity. The decrease of the overall signal is mainly connected to the crystal quality and strongly dependent on the inhomogeneous broadening which can be extracted from the correlation spectra. These results are in agreement with numerical calculations based on the Fourier transform determination of the time-resolved reflection coefficient in the framework of linear semi-classical theory carried out in order to obtain the autocorrelation response.     

Energy relaxation of excitonlike polaritons in semiconductor microcavities: Effect on the parametric scattering of polaritons

Polariton emission in GaAs-based microcavities has been studied under variable conditions, which made it possible to excite (a) polaritons from the upper polariton branch and hot free polaritons and electrons, (b) polaritons from the lower polariton branch (LPB) and localized excitons, and (c) the mixed system. Variation of the excitation conditions leads to substantial differences in the energy distributions of polaritons and in the temperature dependences of polariton emission. It is established that the energy relaxation of resonantly excited LPB polaritons via polariton and localized exciton states at liquid helium temperatures is ineffective. Instead, the relaxation bottleneck effect is suppressed with increasing temperature by means of exciton delocalization (due to thermal excitation by phonons). The most effective mechanism of relaxation to the LPB bottom is via scattering of delocalized excitons on hot free carriers. It is found that the slow energy relaxation of polaritons excited below the free exciton energy can be significantly accelerated at low temperatures by means of additional weak generation of hot excitons and, especially, hot electrons. This acceleration of the energy relaxation of polaritons by means of additional overbarrier photoexcitation sharply decreases the barrier for stimulated parametric scattering of polaritons excited at an LPB inflection point. Therefore, additional illumination can be used to control the polariton-polariton scattering.     

Primary photoexcitations and the origin of the photocurrent in rubrene single crystals

By simultaneously measuring the excitation spectra of transient luminescence and transient photoconductivity after picosecond pulsed excitation in rubrene single crystals, we show that free excitons are photoexcited starting at photon energies above 2.0 eV. We observe a competition between photoexcitation of free excitons and photoexcitation into vibronic states that subsequently decays into free carriers, while molecular excitons are instead formed predominantly through the free exciton. At photon energies below 2.25 eV, free charge carriers are created only through a long-lived intermediate state with a lifetime of up to 0.1 ms and no free carriers appear during the exciton lifetime.     

Femtosecond dynamics of secondary radiation formation from quantum well excitons

The time-resolved secondary emission of resonantly created excitons in GaAs quantum wells is studied using femtosecond up-conversion spectroscopy. The behaviour of the rise and decay of the secondary emission and reflectivity in quantum wells is strongly dependent upon the disorder at the interfaces, the exciton density and the temperature. In the case of low densities and temperatures the emission is independent of the exciton density and rises quadratically in time, in excellent agreement with recent theory for Rayleigh scattering from two-dimensional excitons subjected to disorder. These rise times are compared directly with times measured by time-integrated four-wave mixing (FWM). The comparison of the dynamics displayed in time-resolved secondary radiation and time-integrated FWM provide a clear understanding of the coherence properties of QW excitons in the first few picoseconds after excitation. High-contrast oscillations that are due to quantum beats between the heavy- and light-hole 1s-states are seen. The visibility decay at very low densities is long ps and is related to the action of potential fluctuations on the scattering of heavy-hole and light-hole excitons.     

Excitonic transitions in GaAs---GaAlAs superlattices under a weak electric field

We report a study of the photoluminescence spectra of GaAs---Ga_0.65Al_0.35As superlattice under an electric field of about 10 kVcm⁻¹, from 9 K up to 80 K; the ratio of the intensities of the −1 and 0 peaks of the Wannier-Stark ladder varies with the temperature T. To fit these variations, we assume for both transitions, a trapped exciton density of states with a gaussian distribution of eigenenergies, and a two dimensional density of states for free excitons. We show that above about 50 K there is a thermal equilibrium between direct and crossed free excitons whereas at low temperatures, the equilibrium statistics are not respected: the excitons trap into the direct state rather than to the crossed one.     

Efficiency of exciton and charge carrier photogeneration in a semiconducting polymer

We determine the efficiencies for the formation of excitons and charge carriers following ultrafast photoexcitation of a semiconducting polymer (MEH-PPV). The simultaneous, quantitative determination of exciton and charge photoyields is achieved through subpicosecond studies of both the real and the imaginary components of the complex conductivity over a wide frequency range. Predominantly excitons, with near-unity quantum efficiency, are generated on excitation, while only a very small fraction (<10(-2)) of free charges are initially excited, consistent with rapid ( approximately 100 fs) hot exciton dissociation. These initial charges are very short lived, decaying on subpicosecond time scales.     

Electronic excitations of CO adsorbed on MgO(001)

We report ab initio calculations of the quasiparticle band structure and the optical excitation spectrum of bulk MgO, the MgO(001) surface, and CO molecules adsorbed on MgO(001). Many-body exchange and correlation effects are included within the GW approximation of the electron self-energy operator and the corresponding electron–hole interaction. The excited electron–hole states are obtained from the Bethe–Salpeter equation. At the clean MgO(001) surface exciton states are found with binding energies that are significantly stronger than in the bulk. The exciton spectrum of the adsorbate system CO:MgO is dominated by charge-transfer excitons, which couple strongly to the molecular excitations of CO. PACS 73.20.At; 73.20.Hb; 34.70.+e     

Theory of the excitonic Mott transition in quasi-two-dimensional systems

The excitonic Mott transition in single and double quantum wells is studied using the Green’s function technique. An abrupt jump in the value of the ionization degree, which happens with an increase of the carrier density or temperature, is found in a certain density–temperature region. The opposite effect–the collapse of the electron–hole plasma into an insulating exciton system–is predicted to occur at lower densities. The critical density of the Mott transition for spatially indirect excitons may be much smaller than that for direct excitons.     

Electronic structure and absorption spectrum of biexciton obtained by using exciton basis

We approach the biexciton Schrödinger equation not through the free-carrier basis as usually done, but through the free-exciton basis, exciton–exciton interactions being treated according to the recently developed composite boson many-body formalism which allows an exact handling of carrier exchange between excitons, as induced by the Pauli exclusion principle. We numerically solve the resulting biexciton Schrödinger equation with the exciton levels restricted to the ground state and we derive the biexciton ground state as well as the bound and unbound excited states as a function of hole-to-electron mass ratio. The biexciton ground-state energy we find, agrees reasonably well with variational results. Next, we use the obtained biexciton wave functions to calculate optical absorption in the presence of a dilute exciton gas in quantum well. We find an asymmetric peak with a characteristic low-energy tail, identified with the biexciton ground state, and a set of Lorentzian-like peaks associated with biexciton unbound states, i.e., exciton–exciton scattering states. Last, we propose a pump–probe experiment to probe the momentum distribution of the exciton condensate.     

Bosonic stimulation of cold 1s excitons into a harmonic potential minimum in Cu2O

The density distribution of cold exciton clouds generated into a strain-induced potential well by two-photon excitation in Cu₂O is studied at 2 K. We find that an anomalous spike, which can be interpreted as accumulation of the excitons into the ground state, emerges at the potential minimum. The accumulation can be due to stimulated scattering of cold excitons, mediated by acoustic phonon emission. The possibility of the formation of the thermodynamic Bose-Einstein condensate of paraexcitons is discussed.     

Resonant exciton trapping at impurity states in silver bromide

Excitation spectra near the indirect exciton edge of AgBr at 1.8K are reported for several luminescence lines from weakly localized excitons. Excitation below the exciton absorption threshold reveals several excited bound exciton states the energetic positions of which are determined. For excitation above the threshold, strong energy dependent structure is observed. It is interpreted in terms of resonant trapping of free excitons in both ground and excited bound exciton states associated with emission of LO(Γ), long wavelength acoustic and intervalley TA(X) and LA(X) phonons as well as combinations and overtones of these. From measurements in doped crystals two bound exciton systems are found to be correlated with Cd²⁺ and Ca²⁺, respectively.     

Formation of excitons from free electron–hole pairs due to acoustic phonon interactions in quantum wells

A study of the process of exciton formation due to acoustic phonon interaction in quantum wells (QWs) is presented. Considering that excitons are formed from photoexcited free electron–hole pairs, we have derived the rate of such formation as a function of density and temperature of charge carriers and wavevectorK_|| of the center-of-mass motion of exciton, and finally applied our theory to GaAs/AlGaAs QWs. We have found that the formation of an exciton due to acoustic phonon emission is more efficient at relatively large values ofK_|| (hot excitons) whereas that due to longitudinal optical (LO) phonon emission is more efficient at relatively small values of K_||.     

Resonant Photon Drag of Dipolar Excitons

The theory of the photon drag of dipolar excitons in double-quantum-well nanostructures is presented. It is shown that the exciton-drag flux density features a resonant behavior if the photon frequency is close to some transition frequency in the discrete exciton spectrum. When the structure is irradiated with polarized light, the resonant enhancement of the drag current occurs when the photon energy coincides with the energy of an excited level of the exciton internal motion and the components of the angular momentum of internal motion in the initial and final states differ by one. The proposed effect can be used to control exciton transport in nanostructures based on a two-dimensional exciton gas.     

Barrier-disorder induced exciton relaxation via LO-phonons in GaAs/Al x Ga1−x As multiple quantum wells

Hot exciton relaxation is observed in GaAs/Al _x Ga_1–x As multiple quantum wells. The photolumnescence excitation spectra of the localized exciton emission at low temperatures and excitation densities are composed of narrow equidistant peaks exactly separated by the GaAs LO-phonon energy (36 meV). The relaxation mechanism via LO-phonons is found to be important for localized excitons in multiple quantum wells with GaAs layer thicknesses of about 50 Å, where pronounced alloy fluctuations in the barriers provide a strong additional lateral potential which suppresses the dissociation of hot excitons.