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⁾.     

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.     

Pressure-induced threshold optical pump intensity in a CdTe/ZnTe quantum dot

Pressure-induced binding energies of an exciton and a biexciton are studied taking into account the geometrical confinement effect in a CdTe/ZnTe quantum dot. Coulomb interaction energy is obtained using Hartree potential. The energy eigenvalue and wave functions of exciton and the biexciton are obtained using the self-consistent technique. The effective mass approximation and BenDaniel-Duke boundary conditions are used in the self-consistent calculations. The pressure-induced nonlinear optical absorption coefficients for the heavy hole exciton and the biexciton as a function of incident photon energy for CdTe/ZnTe quantum dot are investigated. The optical gain coefficient with the injection current density, in the presence of various hydrostatic pressure values, is studied in a CdTe/ZnTe spherical quantum dot. The pressure-induced threshold optical pump intensity with the dot radius is investigated. The results show that the pressure-induced electronic and optical properties strongly depend on the spatial confinement effect.     

Coherent control in a single semiconductor quantum dot exhibiting excitonic and biexcitonic features

We have developed a simplified theoretical model to analyze the phenomenon of coherent control in a single semiconductor quantum dot excited by a pair of optical pulses. The first pulse populates a biexciton state by two-photon absorption while the second pulse generates population in the exciton state via deexcitation from the biexciton state. We have used density-matrix analysis for a 3-level system to calculate the time dependent biexciton and exciton state populations. The usual 9×9 matrix has been reduced to a 6×6 matrix. The time variation of the population in each state and it’s dependence on the pulse delay manifest coherent control. Numerical estimates made for In_0.5Ga_0.5As/GaAs single quantum dots qualitatively agree with the recent experimental results. PACS 78.67.Hc; 42.50.Md; 78.55.Cr     

The correlation energies and nonlinear optical absorptions of an exciton in a disc-like quantum dot

Using exact diagonalization techniques, the low-lying states of an exciton, and the linear and nonlinear optical absorptions in a disc-like quantum dot are theoretically studied. The numerical results for the typical GaAs material show the so-called quantum size effect. Also, our study is restricted on the transition between the S state (L = 0) and the P state (L = 1). The optical absorption coefficients are greatly enhanced because of the induced size confinement. Meantime, we find that the total optical absorption coefficient is about two times bigger than that obtained by without considering exciton effects. Additionally, the optical absorption saturation intensity can be controlled by the incident optical intensity I.     

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.     

Effective nonlinear optical properties of shape distributed composite media

The effective linear and nonlinear optical properties of metal/dielectric composite media, in which ellipsoidal metal inclusions are distributed in shape, are investigated. The shape distribution function P(L _x, L _y) is assumed to be 2Δ^-2θ(L _x - 1/3 + Δ/3)θ(L _y - 1/3 + Δ/3)θ(2/3 + Δ/3 - L _x - L _y), where θ( ^{. . .} ) is the Heaviside function, Δ is the shape variance and L_i are the depolarization factors of the ellipsoidal inclusions along i-symmetric axes (i = x, y). Within the spectral representation, we adopt Maxwell-Garnett type approximation to study the effect of shape variance Δ on the effective nonlinear optical properties. Numerical results show that both the effective linear optical absorption α ∼ ωIm() and the modulus of the effective third-order optical nonlinearity enhancement |χ⁽³⁾ _e|/χ⁽³⁾ ₁ exhibit the nonmonotonic behavior with Δ. Moreover, with increasing Δ, the optical absorption and the nonlinearity enhancement bands become broad, accompanied with the decrease of their peaks. The adjustment of Δ from 0 to 1 allows us to examine the crossover behavior from no separation to large separation between optical absorption and nonlinearity enhancement peaks. As Δ → 0, i.e., the ellipsoidal shape deviates slightly from the spherical one, the dependence of |χ⁽³⁾ _e|/χ⁽³⁾ ₁ on Δ becomes strong first and then weak with increasing the imaginary part of inclusions' dielectric constant. In the dilute limit, the exact formula for the effective optical nonlinearity is derived, and the present approximation characterizes the exact results better than old mean field one does. Received 10 December 2002 Published online 4 June 2003 RID="a" ID="a"e-mail: lgaophys@pub.sz.jsinfo.net     

Optical absorption and refraction index change of a confined exciton in a spherical quantum dot nanostructure

Electronic energies of an exciton confined in a strained Zn_1−x Cd _x Se/ZnSe quantum dot have been computed as a function of dot radius with various Cd content. Calculations have been performed using Bessel function as an orthonormal basis for different confinement potentials of barrier height considering the internal electric field induced by the spontaneous and piezoelectric polarizations. The optical absorption coefficients and the refractive index changes between the ground state (L = 0) and the first excited state (L = 1) are investigated. It is found that the optical properties in the strained ZnCdSe/ZnSe quantum dot are strongly affected by the confinement potentials and the dot radii. The intensity of the total absorption spectra increases for the transition between higher levels. The obtained optical nonlinearity brings out the fact that it should be considered in calculating the optical properties in low dimensional semiconductors especially in quantum dots.     

Optical absorptions of a biexciton quantum dot

A investigation of the linear and nonlinear optical properties for intersubband electronic transitions associated with a biexciton in a quantum dot has been performed by using the method of few-body physics. The optical absorption coefficients and the refractive index changes have been examined based on the computed energies and wave functions. It is over two orders of magnitude higher than that obtained in an exciton quantum dot. The results show that the optical absorption saturation intensity can be controlled by the confinement potential frequency and the relaxation time.     

The control of the nonlinear optical response of semiconductor quantum dots

In the present work, we investigate the nonlinear optical properties emerged from excitonic features in an experimentally realized spherical parabolic semiconductor quantum dot (QD). The lowest exciton states together with relevant wave functions are calculated through the expansion method with direct matrix diagonalization method within the effective mass approximation. The effect of the size of QD and confinement potential in exciton state is studied in details. Results show that with increasing the size of the QD the energy of exciton decreases because of decreasing of the effect of coulomb potential. Using the compact density matrix formalism second order nonlinear optical rectification (χ(2)${\chi }^{(2)}$) are obtained. By means of the applied electric and magnetic field we manipulate the exciton states and control the nonlinear optical response in a typical GaAs, InAs, CdSe QDs. Our model system presents a way to control the performance of excitonic optoelectronic devices based on semiconductor nanostructures.     

Three-photon absorption coefficients in ZnSe/ZnS0.18Se0.82 strained-layer superlattices

Summary We provide the first experimental determination of three-photon absorption (ThPA) coefficients α⁽³⁾ in a quasi-bidimensional structure. The measurements of α⁽³⁾ have been performed on a sample of a ZnSe/ZnS_0.18Se_0.82 strainedlayer superlattice at fixed excitation energies corresponding to the exciton resonances near the direct band gap. The evidence of the ThPA process in such energy range points out the huge enhancement of exciton non-linearities in quantum-confined systems.     

Biexciton quantum coherence in a single quantum dot

Nondegenerate (two-wavelength) two-photon absorption using coherent optical fields is used to show that there are two different quantum mechanical pathways leading to formation of the biexciton in a single quantum dot. Of specific importance to quantum information applications is the resulting coherent dynamics between the ground state and the biexciton from the pathway involving only optically induced exciton/biexciton quantum coherence. The data provide a direct measure of the biexciton decoherence rate which is equivalent to the decoherence of the Bell state in this system, as well as other critical optical parameters.     

Frequency and density dependent radiative recombination processes in III–V semiconductor quantum wells and superlattices

In this paper we review the radiative recombination processes occurring in semiconductor quantum wells and superlattices under different excitation conditions. We consider processes whose radiative efficiency depends on the photogenerated density of elementary excitations and on the frequency of the exciting field, including luminescence induced by multiphoton absorption, exciton and biexciton radiative decay, luminescence arising from inelastic excitonic scattering, and electron-hole plasma recombination.

Semiconductor quantum wells are ideal systems for the investigation of radiative recombination processes at different carrier densities owing to the peculiar wavefunction confinement which enhances the optical non-linearities and the bistable behaviour of the crystal. Radiative recombination processes induced by multi-photon absorption processes can be studied by exciting the crystal in the transparency region under an intense photon flux. The application of this non-linear spectroscopy gives direct access to the excited excitonic states in the quantum wells owing to the symmetry properties and the selection rules for artificially layered semiconductor heterostructures.

Different radiative recombination processes can be selectively tuned at exciting photon energies resonant with real states or in the continuum of the conduction band depending on the actual density of photogenerated carriers. We define three density regimes in which different quasi-particles are responsible for the dominant radiative recombination mechanisms of the crystal: (i) The dilute boson gas regime, in which exciton density is lower than 10¹⁰ cm^-2. Under this condition the decay of free and bound excitons is the main radiative recombination channel in the crystal. (ii) The intermediate density range (n < 10¹¹ cm^-2) at which excitonic molecules (biexcitons) and inelastic excitonic scattering processes contribute with additional decay mechanisms to the characteristic luminescence spectra. (iii) The high density range (n ?10¹² cm^-2) where screening of the Coulomb interaction leads to exciton ionization. The optical transitions hence originate from the radiative decay of free-carriers in a dense electron-hole plasma.

The fundamental theoretical and experimental aspects of the radiative recombination processes are discussed with special attention to the GaAs/Al _x Ga_1-x As and Ga _x In_1-x As/Al _y In_1-y As materials systems. The experimental investigations of these effects are performed in the limit of intense exciting fields by tuning the density of photogenerated quasi-particles and the frequency of the exciting photons. Under these conditions the optical response of the quantum well strongly deviates from the well-known linear excitonic behaviour. The optical properties of the crystal are then no longer controlled by the transverse dielectric constant or by the first-order dielectric susceptibility. They are strongly affected by many-body interactions between the different species of photogenerated quasi-particles, resulting in dramatic changes of the emission properties of the semiconductor.

The systematic investigation of these radiative recombination processes allows us to selectively monitor the many-body induced changes in the linear and non-linear optical transitions involving quantized states of the quantum wells. The importance of these effects, belonging to the physics of highly excited semiconductors, lies in the possibility of achieving population inversion of states associated with different radiative recombination channels and strong optical non-linearities causing laser action and bistable behaviour of two-dimensional heterostructures, respectively.     

The generalized dynamical equation and the vacuum polarization effect in hydrogenlike atoms

Based on the generalized dynamical equation, vacuum polarization effects are studied within the scope of the bound state theory in quantum electrodynamics. We find a vacuum-polarization correction to the Lamb shift for the 1S state of the hydrogen atom on the order of (α/π)²(Zα)⁴ that is not considered in the standard theory of bound states in quantum electrodynamics.     

Intrinsic luminescence of amorphous and disordered crystalline systems

A unified method is developed for describing the steady-state luminescence of exciton fluctuation states for weak excitation in different disordered systems. The phononless luminescence band is found to be formed by “radiative” states of the fluctuation tail in the density of states, i.e., by states for which nonradiative states are either nonexistent or have a low probability. The shape of the emission spectra calculated including the phonon interaction is in good agreement with experimental luminescence spectra of α Si:H and of solid solutions of ZnSe_(1−c)Te_c and CdS_(1−c)Se_c. Fiz. Tverd. Tela (St. Petersburg) 40, 890–891 (May 1998)     

Optical properties of glasses in the Li2O–MoO3–P2O5 system

Glasses xLi₂O–(50-x)(MoO₃)₂–50P₂O₅ with x = 10, 20, 30, and 40 mol% were prepared and their optical and electrical properties were investigated. Analysis of the IR spectra revealed that the Li⁺ ions act as a glass modifier that enter the glass network by breaking up other linkages and creating non-bridging oxygens in the network. The optical absorption edge of the glasses was measured for specimens in the form of thin blown films and the optical absorption spectra of those were recorded in the range 200–800 nm. From the optical absorption edges studies, the optical band gap (E _opt) and the Urbach energy (E _e) values have been evaluated by following the available semi-empirical theories. The linear variation of (αhν)^1/2 with hν, is taken as evidence of indirect interband transitions. The E _opt values were found to decrease with increasing Li₂O content by causing increase in the number of non-bridging oxygens in network. The Urbach tail analysis gives the width of localized states between 0.48 and 0.74 eV.     

Third-order nonlinear optical properties of excitonic state in a semiconductor quantum dot

By considering usual matrix procedures we examine how the exciton affects the nonlinear optical properties of 3-D semiconductor GaAs quantum dot. We calculate the third-order optical susceptibility of the GaAs (well) Al_xGaAs_1?x (barrier), and consequently the refractive index and the absorption coefficient. By increasing the Al content (x) in barrier material, carrier relaxation time is enhanced and the susceptibility peaks and their positions showed a blue shift, which agrees with the existing experimental work. For an anisotropic QD, the third-order nonlinear absorption coefficient depends strongly on the quantum dot width.     

The nonlinear optical rectification of a confined exciton in a quantum dot

An exciton in a disc-like quantum dot (QD) with the parabolic confinement, under applied electric field, is studied within the framework of the effective-mass approximation. The nonlinear optical rectification between the ground and the first-excited states has been examined through the computed energies and wave functions in details for the excitons. The results show that the optical rectification susceptibility obtained in a disc-like QD reach the magnitude of 10⁻² m/V, which is 3-4 orders of magnitude higher than in one-dimensional QDs. It is found that the second-order nonlinear optical properties of exciton states in a QD are strongly affected by the confinement strength and the electric field.     

Weak chaos and metastability in a symplectic system of many long-range-coupled standard maps

We introduce, and numerically study, a system of N symplectically and globally coupled standard maps localized in a d=1 lattice array. The global coupling is modulated through a factor r^-α, being r the distance between maps. Thus, interactions are long-range (nonintegrable) when 0≤α≤1, and short-range (integrable) when α>1. We verify that the largest Lyapunov exponent λ_M scales as λ_M ∝ N^-κ(α), where κ(α) is positive when interactions are long-range, yielding weak chaos in the thermodynamic limit N↦∞ (hence λ_M→0). In the short-range case, κ(α) appears to vanish, and the behaviour corresponds to strong chaos. We show that, for certain values of the control parameters of the system, long-lasting metastable states can be present. Their duration t_c scales as t_c ∝N^β(α), where β(α) appears to be numerically in agreement with the following behavior: β>0 for 0 ≤α< 1, and zero for α≥1. These results are consistent with features typically found in nonextensive statistical mechanics. Moreover, they exhibit strong similarity between the present discrete-time system, and the α-XY Hamiltonian ferromagnetic model.     

Impurity and exciton effects on the nonlinear optical properties of a disc-like quantum dot under a magnetic field

A detailed investigation of the nonlinear optical properties of the (D⁺, X) complex in a disc-like quantum dot (QD) with the parabolic confinement, under applied magnetic field, has been carried by using the perturbation method and the compact density-matrix approach. The linear and nonlinear optical absorption coefficients between the ground (L = 0) and the first excited state (L = 1) have been examined based on the computed energies and wave functions. The competition between the confinement and correlation effects on the one hand, and the magnetic field effects on the other hand, is also discussed. The results show that the confinement strength of QDs and the intensity of the illumination have drastic effects on the nonlinear optical properties. In addition, we note that the absorption coefficients of an exciton in QDs depend strongly on the impurity but weakly on the magnetic field. Furthermore, the light and heavy hole excitons should be taken into account when we study the optical properties of an exciton in a disc-like QD.