Excited states of bound excitons in ZnO

The bound exciton lines I₅, I₆, and I_{$\text{7}\text{8}$} in ZnO at 5 K are studied in the energetic region of the free excitons and below by means of excitation spectroscopy. Apart from the maxima at the free exciton energies, additional resonances are observed and interpreted as the direct creation of bound excitons in excited states which lie 6meV and 4.5 meV above the ground states.     

Luminescence of impurity-bound excitons in corundum

The luminescence characteristics of M ³⁺: Al₂O₃ crystals, where M ³⁺ stands for an isoelectronic cation impurity with a filled electron shell, namely, Sc³⁺, Y³⁺, or La³⁺, were studied. The luminescence of excitons bound (BE) to these impurities was detected. The position of the BE energy states at the long-wavelength absorption edge as a function of the M ³⁺ ionic radius was established. The energies of the long-wavelength BE creation threshold and of the maximum of the BE luminescence band were approximated empirically by third-order polynomials of the Toyozawa polynomial type, which describes electron-phonon interaction. The energy and spatial structure of the BE was found to be similar to that of a self-trapped exciton (STE). The BE and STE states are separated by an energy barrier, and energy transfer from the STE to BE is frozen at low temperatures.     

Study of shallow impurity states in compound semiconductors using high resolution photoluminescence spectroscopy

In this paper we review briefly the use of high resolution photoluminescence to study the behavior of shallow impurity states in compound semiconductors. As an illustration we focus our review on GaAs. The binding energies of the ground state and of several low-lying excited states of the impurity centers are determined by studying the radiative transitions associated with excitons bound to neutral donors or acceptors. The difference between the binding energies of different donors in GaAs is rather small. Thus to resolve transitions associated with different chemical donors a magnetic field is used. This has the effect of sharpening the transitions as well as increasing the separation between them. One can identify donors in samples with total impurity concentrations as high as 5X10¹⁵/cm³. The binding energies of different chemical acceptors in GaAs are much higher. Thus the radiative transitions associated with excitons bound to neutral acceptors can be resolved in zero magnetic field. Energy levels of shallow donors and acceptors in GaAs are reviewed.     

Donor-like excited states of exciton bound to neutral acceptor in ZnTe

Photoexcitation spectroscopy has been used to study the excited states of the neutral c-acceptor bound exciton complex A^c₁ in ZnTe. We have detected four excited states at ～ 11.2 meV above the bound exciton ground state. Zeeman effects on these excited states have also been studied. The results show that they correspond to excitations of the bound electron to donor-like 2p and 2s orbital states. This represents an unambiguous experimental evidence of the pseudo-donor model previously suggested by Rühle and Bimberg for acceptor bound exciton complexes when m_e ? m_h.     

Direct and spatially indirect excitons in GaAs/AlGaAs superlattices in strong magnetic fields

Luminescence and luminescence excitation spectra are used to study the energy spectrum and binding energies of direct and spatially indirect excitons in GaAs/AlGaAs superlattices having different electron and hole miniband widths in high magnetic fields perpendicular to the heterolayers. The ground state of the indirect excitons formed by electrons and holes which are spatially distributed among neighboring quantum wells is found to lie between the ground 1s state of the direct excitons and the threshold of the continuum of dissociated exciton states in the minibands. The indirect excitons have a substantial oscillator strength when the binding energy of the exciton exceeds the scale of the width of the resulting miniband. It is shown that a high magnetic field shifts a system of symmetrically bound quantum wells toward weaker bonding. At high exciton concentrations, spatially indirect excitons are converted into direct excitons through exciton-exciton collisions. Fiz. Tverd. Tela (St. Petersburg) 40, 833–836 (May 1998)     

Electronic structure of the self-trapped exciton in rare gas solids

The Rydberg-like series of the self-trapped exciton R₂¹ in rare gas solids (Ar, Kr and Xe) are obtained by solving the effective mass equation which incorporates different corrections, including the central cell correction. The results are in good agreement with the recent transient optical absorption data in which the electron is excited into higher excited states. The origin of the luminescence bands is interpreted by analogy with a similar structure of the self-trapped excitons in alkali halides.     

Oscillator strengths for excitons bound to impurities and quantum wells

It is argued that electron-hole correlation can have a large effect on the oscillator strengths of bound excitons, and may help to explain the observations of shallow excited states for donor bound excitons in direct gap semiconductors. For quantum wells it is found that compression of the exciton wave function yields a $\text{1}\text{L}$ dependence of oscillator strength on well width L for narrow wells.     

Evidence for exciton binding at Ni impurity sites in ZnSe

A broad charge transfer band is observed in the photoluminescence excitation (PLE) spectrum of the 2.5 μ Ni²⁺ luminescence in ZnSe : Ni. This band lies above the highest energy d-d excitation bands and exhibits a ZPL at 1.8163 eV and LO(#38;0lambda;) phonon replicas at higher energy. In contrast, PLE spectra of Co²⁺ luminescence in ZnSe:Co contain only d-d excitation bands. The charge transfer band in ZnSe:Ni is interpreted as evidence for bound exciton formation at the Ni site. The recombination energy of this exciton is transferred efficiently to the excited d-band states of the Ni ion, leading to characteristic Ni²⁺d-d luminescence.     

Shallow acceptor bound exciton and free exciton states in high-purity zinc telluride

We investigated excitons bound to shallow acceptors in high-purity ZnTe and measured excitation spectra of two-hole luminescence lines at 1.6 K using a tunable dye-laser. The electron-hole coupling in the bound exciton (BE) states appears to be very different for the various acceptors even for almost identical exciton localisation energies. Three different types of BE are reported. For the Li-acceptor BE we observe three sub-components separated by 0.22 and 0.17 meV and interpreted as J = $\text{1}\text{2}$, $\text{3}\text{2}$, $\text{5}\text{2}$ states. The Ag-acceptor BE exhibits a strong ground state and a weak excited state at 1.3 meV higher energy. For the as yet unidentified k-acceptor we observe a single BE level, degenerate with the Ag-acceptor BE ground state. Dips in the excitation spectra due to absorption into free exciton 1S, 2S, and 3S states yield an exciton Rydberg R₀ = 12.8±0.3 meV and a free exciton binding energy FE(1S) = 13.2±0.3 meV.     

Far-infrared magneto-absorption of donor-bound excitons in germanium: Pseudo-acceptor model

The magneto-oscillatory absorption spectrum of the arsenic-bound excitons in germanium observed at 118.6 μm reveals a series of absorption lines similar to the Zeeman spectrum of the acceptor impurity. This fact indicates that the bound excitons have the excited states associated with the light-hole Landau ladders and these excited states can be described by the model of a hole bound to the D^- state, i.e. the pseudo-acceptor model. The hole binding energy of the ground state of the bound excitons has been obtained to be 4.7 meV, which is smaller compared with the binding energy of the acceptor impurity.     

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.     

Exciton lifetime in quantum well with vicinal high-density excitons

Radiative lifetime of an exciton in a GaAs quantum well (QW) is controlled by high-density excitons, which restrict the exciton coherence through scattering. In order to circumvent the phase space filling effect of high-density excitons, we have prepared a QW structure in such a way that a reservoir for high-density excitons is separated from the QW. The lifetime increases (up to 30%) with the exciton density in the reservoir and saturates at 1×10¹⁷/cm³. The upper bound lifetime is determined by the excitonic relative motion.     

Exciton and phonon spectra of acoustooptic Tl3AsS3 crystals

The λ-modulated exciton reflection spectra of Tl₃AsS₃ crystals are investigated at 8 and 77 K, in which the ground (n=1) and excited (n=2, 3) exciton states are revealed. Taking into account the spatial dispersion, the shapes of λ-modulated reflection spectra of the n=1 line are calculated and the basic parameters of excitons and bands are determined (the translational and reduced masses of excitons and the effective masses of electrons and light and heavy holes). The one-phonon reflection spectra are studied in the region from 50 to 500 cm^?1 in polarizations E ∥ c and E ⊥ c. The shapes of one-phonon reflection spectra are calculated and the parameters of vibrational modes E and A ₂ are determined.     

Photoluminescence characterization of vertically aligned ZnO microrods

A detailed optical characterization of vertically aligned ZnO microrods (μRs) grown using a Ni-based catalyst was carried out by excitation-power- and temperature-dependent photoluminescence (PL) measurements. Low-temperature PL spectra of ZnO μRs are dominated by near-band-edge (NBE) emission consisted of a series of sharp lines typical for the bulk ZnO. Starting from the higher energy free exciton (FX) emission feature, the majority of them can be explained by radiative recombination of excitons bound to neutral donors (D⁰X), defect bound exciton (DBX), two-electron satellites emission, free-to-bound, i.e. free electrons to the neutral acceptors (eA⁰) transition, as well as their longitudinal-optical phonon replicas. An additional excitonic line located in between the FX and D⁰X lines, denoted as the surface excitons (SX) for ZnO μRs is observed. The intensity of the SX line is found to be smaller than that of the nanosized counterpart and has been attributed to the surface–volume ratio effects. The excitation-power-dependent results of FX line at low and high power regimes show quite close values corresponding to, respectively, p=2 and p=1 limits of the theoretical power law expression I～L^p and larger deviations for the D⁰X, SX and DBX lines. The temperature-dependent measurements confirmed the presence of eA⁰ line showing kT/2 influence to the position of eA⁰ emission line in comparison with FX. FX emissions persist up to 300 K and together with the dominant eA⁰ emission govern the line shape of the NBE emission range, while D⁰X and SX lines are quenched completely at 150 K.     

Uniaxial stress effects and excited states for multiple bound excitons

The theoretical model for multiple bound excitons (MBE) recently introduced by Dean et al¹ is used to discuss uniaxial stress effects in silicon. The fine structures observed in MBE spectra for SiC and Si are qualitatively strikingly similar. However, the interpretation of the strongest features in terms of a specific model for excited states suggested by Kirczenow² and Thewalt³ is not valid for SiC.     

Exciton dynamics at interfaces of organic semiconductors

We review recent progress of using time-resolved two-photon photoelectron spectroscopy (2PPE) to study the energetics and dynamics of excitons at surfaces and interfaces of two prototypical organic semiconductors: C₆₀ and pentacene. For C₆₀ thin films epitaxially grown on Au(1 1 1) and Cu(1 1 1) surfaces, we observe both charge transfer and exciton states. For excitons in C₆₀, the proximity of a metal surface leads to rapid, exciton band-mediated quenching. At the surface of pentacene thin films we observe a series of charge-transfer excitons where the electron and the photohole are bound across the interface. The ability of 2PPE to measure and directly relate exciton levels to single-electron levels is illustrated.     

Direct and spatially indirect excitons in GaAs/AlGaAs superlattices in strong magnetic fields

Luminescence and luminescence excitation spectra are used to study the energy spectrum and binding energies of direct and spatially indirect excitons in GaAs/AlaAs superlattices, with different widths of the electron and hole minibands, located in a high magnetic field perpendicular to the heterolayers. It is found that the ground state of the indirect excitons formed by electrons and holes and spatially separated between neighboring quantum wells lies between the ls ground state of the direct excitons and the continuum threshold for dissociated exciton states in the minibands. Indirect excitons in superlattices have a significant oscillator strength when the binding energy of the exciton exceeds the order of the width of the resulting miniband. The behavior of the binding energy of direct and indirect heavy hole excitons during changes in the tunneling coupling between the quantum wells is established. It is shown that a strong magnetic field, which intensifies the Coulomb interaction between the electron and hole in an exciton, weakens the bond in a system of symmetrically bound quantum wells. The spatially indirect excitons studied here are analogous to first order Wannier-Stark localized excitons in superlattices with inclined bands (when an electrical bias is applied), but in the present case the localization is of purely Coulomb origin. Zh. éksp. Teor. Fiz. 112, 1106–1118 (September 1997)     

Two-photon correlations of luminescence at the Bose-Einstein condensation of dipolar excitons

Correlations of the luminescence intensity (the second-order correlation function g ⁽²⁾(τ)), where τ is the delay time between the photons detected in pairs) under the conditions of the Bose-Einstein condensation (BEC) of dipolar excitons has been studied in a temperature range of 0.45–4.2 K. Photoexcited dipolar excitons have been accumulated in a lateral trap in a GaAs/AlGaAs Schottky diode with a 25-nm wide single quantum well with an electric bias applied across the heterolayers. Two-photon correlations have been measured with the use of a two-beam intensity interferometer with a time resolution of }~0.4 ns according to the well-known classical Hanbury-Brown-Twiss scheme. The photon bunching has been observed at the onset of Bose-Einstein condensation manifested by the appearance of a narrow exciton condensate line in the luminescence spectrum at an increase in the optical pumping (the line width near the threshold is ?200 μeV). At the same time, the two-photon correlation function itself obeys the super-Poisson distribution, g ⁽²⁾(τ) > 1, at time scale τ_c ? 1 ns of the system coherence. The photon bunching is absent at a pumping level substantially below the condensation threshold. The effect of bunching also decreases at pumping significantly above the threshold, when the narrow exciton condensate line starts to dominate in the luminescence spectra, and finally disappears with the further increase in the optical excitation. In this region, the distribution of pair photon correlations is a Poisson distribution manifesting the united quantum coherent state of the exciton condensate. Under the same conditions, the first-order spatial correlation function g ⁽¹⁾(r) determined from the interference pattern of the luminescence signals from the spatially separated parts of the condensate at constant pumping remains noticeable at distances of no less than 4 μm. The discovered effect of photon bunching is very sensitive to temperature and decreases by several times with a temperature increase in the range of 0.45–4.2 K. Assuming that the luminescence of the dipolar excitons directly reflects the coherence properties of the gas of interacting excitons, the discovered photon bunching at the onset of condensation, where the fluctuations of the exciton density and, consequently, of the luminescence intensity are most significant, indicates a phase transition in the interacting Bose gas of excitons, which is an independent way of detecting the Bose-Einstein condensation of excitons.     

The trion as an exciton interacting with a carrier

The X⁻ trion is essentially an electron bound to an exciton. However, due to the composite nature of the exciton, there is no way to write an exciton-electron interaction potential. We can overcome this difficulty by using a commutation technique similar to the one we introduced for excitons interacting with excitons, which allows to take exactly into account the close-to-boson character of the excitons. From it, we can obtain the X⁻ trion creation operator in terms of excitons and electrons. We can also derive the X⁻ trion ladder diagram between an exciton and an electron. These are the basic tools for future works on many-body effects involving trions.