Fine structure splitting and biexciton binding energy in single self-assembled InAs/AlAs quantum dots

We report on photoluminescence investigations of individual InAs quantum dots embedded in an AlAs matrix which emit in the visible region, in contrast to the more traditional InAs/GaAs system. Biexciton binding energies, considerably larger than for InAs/GaAs dots, up to 9 meV are observed. The biexciton binding energy decreases with decreasing dot size, reflecting a possible crossover to an antibinding regime. Exciton and biexciton emission consists of linearly cross polarized doublets due to a large fine structure splitting up to 0.3 meV of the bright exciton state. With increasing exciton transition energy the fine structure splitting decreases down to zero at about 1.63 eV. Differences with InAs/GaAs QDs may be attributed to major dot shape anisotropy and/or larger confinement due to higher AlAs barriers.     

Coherent dynamics in InGaAs quantum dots and quantum dot molecules

We measure the dephasing time of the exciton ground state transition in InGaAs quantum dots (QD) and quantum dot molecules (QDM) using a sensitive four-wave mixing technique. In the QDs we find experimental evidence that the dephasing time is given only by the radiative lifetime at low temperatures. We demonstrate the tunability of the radiatively limited dephasing time from 400 ps up to 2 ns in a series of annealed QDs with increasing energy separation of 69–330 meV from the wetting layer continuum. Furthermore, the distribution of the fine-structure splitting δ₁ and of the biexciton binding energy δ_B is measured. δ₁ decreases from 96 to with increasing annealing temperature, indicating an improving circular symmetry of the in-plane confinement potential. The biexciton binding energy shows only a weak dependence on the confinement energy, which we attribute to a compensation between decreasing confinement and decreasing separation of electron and hole. In the QDM we measured the exciton dephasing as function of interdot barrier thickness in the temperature range from 5 to 60 K. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed, showing how the quantum mechanical coupling in the molecules affects the exciton lifetime and acoustic-phonon interaction.     

利用N型半导体纳米材料抑制单量子点的荧光闪烁特性

利用N型半导体纳米材料氧化铟锡(ITO)作为单CdSe/ZnS量子点的基质来抑制单量子点的荧光闪烁特性. 实验采用激光扫描共聚焦显微成像系统测量了单量子点荧光的亮、暗态持续时间的概率密度分布的指数截止的幂律特性, 并与直接吸附在SiO₂玻片上的单CdSe/ZnS量子点的荧光特性进行比较. 研究发现处于ITO中的单量子点比SiO₂玻片上的单量子点荧光亮态持续时间提高两个数量级, 掺杂于ITO中的单量子点的荧光寿命约减小为SiO₂玻片上的单量子点的荧光寿命的41%, 并且寿命分布宽度变小50%.     

Surface integral determination of built-in electric fields and analysis of exciton binding energies in nitride-based quantum dots

We present a simple analytical approach to calculate the built-in strain-induced and spontaneous piezoelectric fields in nitride-based quantum dots (QDs) and then apply the method to describe the variation of exciton, biexciton and charged exciton energy with dot size in GaN/AlN QDs. We first present the piezoelectric potential in terms of a surface integral over the QD surface, and confirm that, due to the strong built-in electric field, the electrons are localised near the QD top and the holes are localised in the wetting layer just below the dot. The strong localisation and smaller dielectric constant results in much larger Coulomb interactions in GaN/AlN QDs than in typical InAs/GaAs QDs, with the interaction between two electrons, J_ee, or two holes, J_hh, being about a factor of three larger. The electron–hole recombination energy is always blue shifted in the charged excitons, X⁻ and X⁺, and the biexciton, and the blue shift increases with increasing dot height. We conclude that spectroscopic studies of the excitonic complexes should provide a useful probe of the structural and piezoelectric properties of GaN-based QDs.     

Near-field optical mapping of exciton wave functions in a GaAs quantum dot

Near-field photoluminescence imaging spectroscopy of naturally occurring GaAs quantum dots (QDs) is presented. We successfully mapped out center-of -mass wave functions of an exciton confined in a GaAs QD in real space due to the enhancement of spatial resolution up to 30 nm. As a consequence, we discovered that the spatial profile of the exciton emission, which reflects the shape of a monolayer-high island, differs from that of biexciton emission, due to different distributions of the polarization field for the exciton and biexciton recombinations. This novel technique can be extensively applied to wave function engineering in the design and the fabrication of quantum devices.     

Extremely large binding energy of biexcitons in an organic-inorganic quantum-well material (C4H9NH3)2PbBr4

We have confirmed biexciton formation in an organic-inorganic hybrid quantum-well material (C₄H₉NH₃)₂PbBr₄ by photoluminescence and two-photon absorption measurements. The biexciton has extremely large binding energy, 60 meV, which to our knowledge is the largest value ever reported for a semiconductor. By analyzing the spectrum of biexciton luminescence, the biexciton gas temperature was found to be much higher than the bath temperature due to a higher local temperature arising from the large biexciton binding energy.     

Impact of shell thickness on exciton and biexciton binding energies of a ZnSe/ZnS core–shell quantum dot

Impact of shell structure on the exciton and biexciton binding energies has been studied in a ZnSe/ZnS core–shell quantum dot using Wentzel–Kramers–Brillouin (WKB) approximation. For excitons, the binding is caused by the Coulombic as well as the confinement potentials while biexciton binding energy is determined by taking into account the exchange and correlation effects. The exciton binding energy was found to increase initially with increasing shell thickness which reaches saturation at larger shell thickness. On the other hand, the biexciton binding energy exhibits a crossover from the bonding to antibonding state with increasing shell thickness for smaller core radius of the quantum dot.     

Self-consistent calculations of exciton, biexciton and charged exciton energies in InGaN/GaN quantum dots

We present theoretical calculations of the variation of exciton energies in truncated conical InGaN quantum dots (QDs) in a GaN matrix with dot size and indium composition. We compute the built-in strain-induced and spontaneous piezoelectric fields using a surface integral method that we have recently derived, and confirm that the built-in fields can be of the order of a few MV/cm, resulting in a spatial separation of the electrons and holes. The ground state wavefunctions of the exciton (X⁰), biexciton (2X⁰) and the two charged excitons (X⁻ and X⁺) are then calculated in the Hartree approximation, using a self-consistent finite difference method. We find that the electron–hole recombination energy is always blue-shifted for the charged excitons X⁻ and X⁺, with a further blue-shift for the biexciton, and this blue-shift increases with increasing indium content. We describe the trends in interband transition energy and the scale of the blue-shift with dot size, shape and composition. We conclude that spectroscopic studies of the exciton, charged excitons and biexciton should provide a useful probe of the structural and piezoelectric properties of GaN-based QDs.     

Biexciton binding energy in Cu2O

The problem of the biexciton molecule in Cu₂O is considered from the theoretical point of view. The possible biexciton levels are classified using the symmetry of the crystal and the band structure scheme proposed by Elliott. The binding energy of the lowest state is computed on the basis of variational calculations with inclusion of the electron—hole exchange contribution. This contribution tends to make the biexciton unbound, the largest possible value of the binding energy being 0.2 meV. We conclude that no biexciton can exist in Cu₂O at any temperature, in agreement with the views of Petroff, Yu and Shen and in disagreement with those of Gross and Kreingold.     

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.     

Luminescence of excitonic molecules in AgBr

Luminescence spectra of AgBr at the temperature range 5–50 K and under pulse excitation intensity up to ～ 0.7 MW cm^?2 are investigated. Intensity and temperature dependences of biexciton emission line (2.67 eV) yield thermodynamic determination of biexciton binding energy in agreement with the spectroscopic value (6.7 meV). The behaviour of biexciton emission in the investigated temperature range is explained by the concept of “biexciton pocket”. Some questions of the electron-hole liquid recombination radiation (2.60 eV) are discussed as well.     

Biexciton stability in carbon nanotubes

We have applied the quantum Monte Carlo method and tight-binding modeling to calculate the binding energy of biexcitons in semiconductor carbon nanotubes for a wide range of diameters and chiralities. For typical nanotube diameters we find that biexciton binding energies are much larger than previously predicted from variational methods, which easily brings the biexciton binding energy above the room temperature threshold.     

Effect of interchain coupling on a biexciton in organic polymers

The effect of interchain coupling on the formation and the stability of a biexciton is studied in poly (p-phenylene vinylene) chains in the framework of the tight-binding approach. We obtain an intrachain exciton and biexciton as well as an interchain exciton and biexciton through a double-photon excitation. It is found that a biexciton is energetically favourable to two single excitons even when there exists an interchain coupling. There is a turnover value t_⊥C of the interchain coupling for the formation of a biexciton, beyond which two excitons are combined into one biexciton. The binding energy of a biexciton is calculated to decrease with the increase of interchain coupling, which indicates that a biexciton is relatively stable in polymers with a weak interchain coupling. The conclusion is consistent with the experimental observations. In addition, a suggestion about how to improve the yielding efficiency or the formation of biexcitons in actual applications is given.     

Identifying multi‐excitons in quantum dots: the subtle connection between electric dipole moments and emission linewidths

The emission linewidths of excitonic complexes confined in quantum dots (QDs) mirror their interaction with a defect‐induced, fluctuating charge environment, a phenomenon known as spectral diffusion. Interestingly, extended excitonic complexes that comprise several interacting excitons exhibit significantly smaller emission linewidths if compared to the optical fingerprint of their building block, a sole exciton. Hence, it is not the absolute, but the relative electric dipole moment that governs the directly accessible emission linewidths. Exemplarily we investigate this matter based on differing exciton and biexciton emission linewidths of single GaN QDs with varying emission energies, i.e. QD dimensions. Our results establish the full width at half maximum (FWHM) or any other linewidths criterion for the identification of excitonic complexes, a technique that can directly be applied to polar but even non‐polar QD materials. Additionally, we find an emission energy dependent trend for the FWHM ratios of the biexciton and the exciton (XX_FWHM/X_FWHM) in perfect agreement with their relative dipole moment ratios as derived from our 8‐band‐ k · p based treatment of the Coulomb and exchange interaction within these multi‐particle complexes. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Biexciton in nanosystem of quantum dots of cadmium sulfide in a dielectric matrix

A significant increase in the binding energy of the singlet ground state of biexciton (of spatially separated electrons and holes) in a nanosystem that consists of CdS quantum dots grown in a borosilicate glass matrix has been predicted; the effect is almost two orders of magnitude larger than the binding energy of biexciton in a sulfide cadmium single crystal.     

Fractional-dimensional approach for biexcitons in GaAs/AlxGa1−xAs quantum wells

The energy of a biexciton in a GaAs/Al_xGa_1?xAs quantum well structure with finite barriers is investigated by using the geometrical model of two-dimensional biexcitons proposed by Singh et al. [J. Singh, D. Birkedal, V.G. Layssenko, J.M. Hvam, Phys. Rev. B 53 (1996) 15909; I.-K. Oh, J. Singh, Phys. Rev. B 60 (1999) 2528]. A fractional-dimensional approach is used to obtain the binding energy of the biexciton in both square quantum wells and parabolic quantum wells. Theoretical results show that the binding energy of a biexciton in a finite quantum well exhibits a maximum with increasing well width. The ratio of the binding energy of a biexciton to that of an exciton in a quantum well structure is found to be sensitive to the electron-to-hole mass ratio and larger than that in the three-dimensional system. The results agree fairly well with previous experimental results. The results of our approach are also compared with those of earlier theories.     

Many-exciton effects in the biexciton bound-state potential

Starting from a previously derived many-particle equation describing biexciton states, the influence of dynamical exciton-exciton scattering effects on the biexciton binding energy has been calculated. As a result, we obtain density effects in bound states. In qualitative agreement with experimental data only a small density-induced shift of the biexcitonic luminescence should be observed.     

Control of structural and excitonic properties of self-organized InAs/GaAs quantum dots

A systematic dependence of excitonic properties on the size of self-organized InAs/GaAs quantum dots is presented. The bright exciton fine-structure splitting changes from negative values to more than 0.5 meV, and the biexciton binding energy varies from antibinding to binding, as the height of truncated pyramidal dots increases from 2 to above 9 InAs monolayers. A novel mode of metalorganic vapor phase epitaxy was developed for growing such quantum dots with precise shape control. The dots consist of pure InAs and feature heights varying in steps of complete InAs monolayers. Such dot ensembles evolve from a strained, rough two-dimensional layer with a thickness close to the critical value for the onset of the 2D–3D transition. Dots with a common height represent subensembles with small inhomogeneous broadening. Tuning of subensemble emission energy is achieved by varying the mean lateral extension of the respective QDs. Detailed knowledge of the structural properties of individual dots enable realistic k·p calculations to analyze the origin of the observed excitonic properties. The binding energies of charged and neutral excitons increase due to correlation by the gradually increasing number of bound states for increasing dot size. The monotonously increasing magnitude of the fine-structure splitting with dot size is shown to be caused by piezoelectricity. The identification of key parameters allows to tailor exciton properties, providing a major step towards the development of novel applications.     

Excitation spectroscopy on the M-band of red HgI2

The luminescence of red HgI₂ is investigated as a function of excitation intensity and -wavelength. At low excitation, emission is due to free and bound exciton recombination, at high levels a “M-band” is dominating. This M-band is partially ascribed to biexciton decay, this assumption being supported by resonances found in the excitation spectra. The biexciton binding energy is determined to be 6±1 meV.     

Nonlinear optical properties of biexciton states in GaN quantum disks

The ground state energy of an exciton and biexciton states, in a GaN/Al_xGa_1-xN quantum disk are investigated by the variation method, within envelope function and effective mass approximations. Exciton and biexciton binding energy, and the dipole moments related to the transition between ground, exciton and biexciton states, are calculated as a function of quantum disk geometry. The optical nonlinearity via the exciton and biexciton states is studied on the basis of a three level model through the density matrix formalism. The behavior of different terms of third order susceptibility χ⁽³⁾, are studied around resonance frequencies and for different geometries of disk. The effect of values of the decay rates on χ⁽³⁾ are studied. It is found that these values have remarkable effect on the second term of, χ⁽³⁾.