Electron capture and intra-band relaxation by means of Auger processes in colloidal semiconductor nanocrystals

The electron relaxation dynamics in combination with LO phonon-assisted electron capture and intra-dot Auger scattering processes in a spherical quantum dot embedded in non-polar matrix is presented theoretically. The electron capture efficiency is investigated as a function of the lattice temperature and quantum dot radius for a deferent injected electron concentration, taking into account the confinement effect of the polar optical phonons in spherical quantum dots. Exact numerical calculations for the phonon-assisted electron capture rate as well as for the Auger scattering rate in colloidal CdSe quantum dot have been carried out. These calculations are consistent with experiment.     

Electron spin relaxation in very diluted CdMnTe quantum wells

Electron spin dephasing is studied by time-resolved Kerr rotation in n-type modulation-doped CdMnTe quantum wells with very dilute Mn content. We find good agreement between measured and calculated electron spin relaxation times, considering relaxation induced by fluctuating exchange field created by the Mn spins, and taking into account inhomogeneous heating of the Mn spins by laser pulses.     

Luminescence related processes in semiconductor nanocrystals —The strong confinement regime

This paper summarizes systematic studies on the luminescence from CdSe nanocrystals in the situation of strong zero-dimensional confinement. We discuss the role of surface and defect states, the origin of the photo-darkening and demonstrate by calorimetric adsorption measurements that the internal quantum efficiency is in the range of some 10%. The lifetimes of the intrinsic excitations are strongly size-dependent. While the radiative recombination (≈ 1 ns) is dominant for larger nanocrystals, we observe a dramatic increase of the non-radiative rate below 4 nm as a result of the reduced volume to surface ratio. The combination of ultra-fast and size-selective excitation allows us to observe a progression of sharp LO-phonon lines signifying the zero-dimensional character of the nanocrystals and providing information on the strength of the phonon coupling and the homogeneous width of the quantum-confined ground state.     

Transient gain-absorption of the probe field in asymmetric semiconductor quantum wells

Under the weak-probe approximation, we theoretically investigate the transient gain-absorption property of the probe field in a four-level asymmetric semiconductor quantum well system. We find that the strength of Fano interference and the energy splitting affect the transient gain-absorption property of the weak continuous-wave (CW) probe field or Gaussian-pulse probe field dramatically. The dependence of transient gain-absorption property of the probe field on the intensity and the frequency detuning of the strong coupling field is also given. Our study is much more practical than its atomic counterpart due to its flexible design and the controllable interference strength. Thus, it may provide some new possibilities for technological applications.     

半导体量子阱中电子自旋弛豫和动量弛豫

根据电子自旋轨道耦合对自旋极化弛豫影响的DP机理进一步导出了半导体中电子自旋弛豫与动量弛豫及载流子浓度的关系，并采用飞秒抽运探测技术在室温下测量AlGaAs/GaAs 多量子阱中载流子浓度在 1×10¹⁷—1×10¹⁸cm^-3范围内，电子自旋弛豫时间由58ps增加至82 ps的变化情况，与理论计算值符合，说明了随着载流子浓度的增加，载流子间的频繁散射加速了电子动量驰豫，减弱了电子自旋轨道耦合作用，从而延长了电子自旋寿命. 关键词： 电子自旋轨道耦合 电子自旋弛豫和动量弛豫 飞秒光谱技术     

Persistent hole burning in semiconductor nanocrystals

The persistent spectral hole burning (PSHB) phenomenon was found to occur in many kinds of nanocrystalline semiconductors, such as CdSe, CdS, CuCl, CuBr and CuI, embedded in crystals, glass or polymers. In inhomogeneously broadened exciton absorption spectra of these nanocrystals, the spectral hole and its associated structure were created by the narrow-band laser excitation and were conserved for more than several hours at 2 K. Hole depth grew in proportion to the logarithm of the burning fluence. Thermally-annealing and light-induced hole-filling phenomena were observed. The hole burning takes place by the tunneling process through potential barriers with broadly distributed barrier height and thickness. Unusual luminescence behaviors related to the PSHB phenomena were also observed. They are luminescence elongation with increase of the light exposure and hole burning in the luminescence spectrum. The observed PSHB phenomena are explained by the exciton localization and the succeeding ionization of nanocrystals. The energy of the photoionized nanocrystal is released from the original energy and the new energies depend on the spatial arrangement of the trapped carriers. Quantum confinement of carriers and resulting strong Coulomb interaction between confined carriers and trapped carriers are essential for the energy change. Possible applications of the PSHB phenomenon is discussed.     

Photoluminescence polarization of semiconductor nanocrystals

We review the polarization properties of photoluminescence (PL) in nanocrystals (NCs) from both theoretical and experimental points of view. We show that, under linearly polarized excitation, NCs emit partly polarized light owing to their uniaxial structure or their anisotropic shape. In elongated NCs, the anisotropy may have two origins, the electronic confinement or the effect of depolarizing field created by the light-induced charges on the interfaces. Results of polarization studies in porous silicon are presented. They are explained by the shape of the Si NCs. Experiments in CdSe NCs reveal the fine structure of the excitonic levels and show evidence of the enhancement of the electron-hole exchange energy with decreasing NC size. Spin orientation in wurtzite-type NCs is achieved by optical pumping with circularly polarized light. The effect of a magnetic field on the degree of circular polarization and the mechanisms of spin relaxation are discussed. Results in large-size NCs are presented.     

Water-soluble, cyclodextrin-functionalized semiconductor nanocrystals: Preparation and pH-dependent aggregation and emission properties

Using peramino-functionalized β-cyclodextrin molecules for phase.transfer of hydrophobic CdSe multishell nanocrystals into water, we obtained hydrophilic nanoparticles with high quantum yield (up to 50%). At pH > 9, the aqueous solution of these nanocrystals remained stable for several months. The nanoparticles showed a strong influence of the pH of the aqueous solution on the emission of the nanocrystals: the quantum yield varied reversible from ∼10% at pH=6 to ∼50% at pH=14, an effect which according to particle size characterization by dynamic light-scattering and asymmetric flow field-flow fractionation has mainly been attributed to reversible partial aggregation of the hydrophilic nanocrystals at lower pH-values. Additionally, prolonged irradiation in the presence of oxygen led to a strong enhancement of the photoluminescence intensity of the nanocrystals.     

Trions in quantum wells

An overview is given of our investigation of the energy levels and of the correlation functions of the negatively and positively charged excitons (also called trions) in quantum wells in the presence of a perpendicular magnetic field. A detailed comparison is made with available experimental data in III–V and II–VI semiconductor quantum wells.     

Spectroscopic ellipsometry of layer by layer deposited colloidal HgTe nanocrystals exhibiting quantum confinement

We have explored the optical properties of bilayers of Mercury telluride (HgTe) nanocrystals (NCs) embedded in polymer which were prepared from a colloidal solution. These NCs show strong luminescence in the near infrared at room temperature, which makes them an interesting material for the telecommunication area. The emission wavelength can efficiently be tuned by controlling the size of the NCs. We report spectroscopic ellipsometry measurements, which clearly show an energy shift of the critical points (CPs) in the dielectric function to higher energies compared to the HgTe bulk properties. This is caused by quantum confinement in the crystals. The exact peak energies of the transitions are fitted with line-shape models for CPs. Surprisingly, concepts coming from semiconductor bulk optics, as CPs, can be applied to NCs with a diameter of less than 5 unit cells.     

Exciton relaxation in self-assembled semiconductor quantum dots

The present study focuses on the effect of excited states on the exciton–polaron spectrum for self-assembled InAs/GaAs semiconductor quantum dots. The analytical model takes into account the Coulomb interactions between the electron and the hole as well as, each carrier, the coupling with the longitudinal optical phonon field. Furthermore, the key role played by the exciton continuum in the dot spectrum is also introduced. Such an approach is well fitted to analyze recent experimental findings about single-dot spectroscopy and allows peaks assignment, line width estimation, relaxation time evaluation, etc., necessary steps toward an understanding of the internal dynamics of quantum dots.     

Intersubband absorption in highly photoexcited semiconductor quantum wells

Transient mid infrared (MIR) absorption spectroscopy is used to investigate transitions between higher electronic subbands in semiconductor quantum well (QW) structures after interband photoexcitation with intense picosecond pulses in the visible spectral range. Our investigation focuses on the e₂–e₃ intersubband transition in an asymmetric undoped GaAs/AlGaAs QW structure. At an injected nonequilibrium carrier density of 1×10¹³ cm⁻²/QW, an e₂–e₃ absorption band at 99 meV with a spectral width of 5 meV is found. For a higher density studied, 3×10¹³ cm⁻²/QW, the band is broadened and blueshifted by 30 meV. Intersubband absorption signals are distinguished from free-carrier absorption signals in the MIR by their characteristic time behavior.     

Investigation of Auger recombination in Ge and Si nanocrystals embedded in SiO2 matrix

We study theoretically the optical properties of embedded Ge and Si nanocrystals (NCs) in wide band-gap matrix and compared the obtained results for both NCs embedded in SiO₂ matrix. We calculate the ground and excited electron and hole levels in both Ge and Si nanocrystals (quantum dots) in a multiband effective mass approximation. We use the envelope function approximation taking into account the elliptic symmetry of the bottom of the conduction band and the complex structure of the top of the valence band in both Si and Ge (NCs). The Auger recombination (AR) in both nanocrystals is thoroughly investigated. The excited electron (EE), excited hole (EH) and biexciton AR types are considered. The Auger recombination (AR) lifetime in both NCs has been estimated and compared.     

Multi-spin-subband structure of dilute magnetic semiconductor quantum wells: Feedback mechanism

Using a fully self-consistent envelope function approach, we focus on wide conduction band NMS (non-magnetic semiconductor)/DMS (dilute magnetic semiconductor)/NMS quantum wells, under weak external parallel magnetic field, where many spin-subbands are usually present. We concentrate on small values of the magnetic field because we want to investigate the influence of the feedback mechanism due to the difference of the concentrations of spin-up and spin-down carriers which could induce spontaneous spin-polarization i.e. in the absence of a magnetic field. We study the spin-subband structure, the spin-subband populations and the spin-polarization as functions of the sheet carrier concentration, _Ns$N_s$, for different values of the magnitude of the exchange interaction, |J|$\left|J\right|$, between the itinerant carriers and the magnetic impurities. Our calculations for 0.01 T show that at 20 K the values of |J|$\left|J\right|$ necessary to make this feedback mechanism sufficiently strong are too high compared to the |J|$\left|J\right|$ values of common Mn-doped systems in the conduction band. However, the feedback mechanism will be sufficiently strong at low enough temperatures below 20 K for realistic values of |J|$\left|J\right|$. Moreover, we explain how increasing the sheet carrier concentration the heterostructure is transformed from an almost square quantum well to a system of two coupled heterojunctions with an intermediate soft barrier.     

Stark effect of negatively and positively charged excitons in semiconductor quantum wells

We study the effect of an electric field applied normal to the layers on the binding energy of charged excitons (or trions) in GaAs quantum wells. We find that, in contrast to the neutral exciton, their binding energy is sharply reduced by modest electric fields. The effect is stronger for the positively charged exciton than the negatively charged one. The ionisation of the excess carrier is explained by the field-induced polarisation of the electron and hole subband wave functions.     

Gated spin relaxation in (1 1 0)-oriented quantum wells

Growth, photoluminescence characterisation and time-resolved optical measurements of electron spin dynamics in (1 1 0)-oriented GaAs/AlGaAs quantum wells are described. Conditions are given for MBE growth of good-quality quantum wells, judged by the width of low-temperature excitonic photoluminescence. At 170 K the electron spin relaxation rate in (1 1 0)-oriented wells shows a 100-fold reduction compared to equivalent (1 0 0)-oriented wells and also a 10-fold increase with applied electric field from 20 to 80 kV cm⁻¹. There is evidence for similar dramatic effects at 300 K. Spin relaxation is field independent below 20 kV cm⁻¹ reflecting quantum well asymmetry. The results indicate the achievability of voltage-gateable quantum well spin memory time longer than 10 ns at room temperature simultaneously with high electron mobility.     

Control of the probe absorption via incoherent pumping fields in asymmetric semiconductor quantum wells

In a three-level asymmetric semiconductor quantum well system, owing to the effects that result from the incoherent pumping fields, the probe absorption of probe field can be effectively controlled. The result is achieved by applying the two incoherent pumping fields, so it is different from the conventional way in ordinary laser-driven schemes that coherent driving fields are necessary to control the probe absorption. Otherwise, our study is much more practical than its atomic counterpart due to its flexible design and the controllable interference strength. Thus, it may provide some new possibilities for technological applications in optoelectronics and solid-state quantum information science.     

Spin relaxation and antiferromagnetic coupling in semiconductor quantum dots

We report carrier spin dynamics in highly uniform self-assembled InAs quantum dots and the observation of antiferromagnetic coupling between semiconductor quantum dots. The spin relaxation times in the ground state and the first excited state were measured to be 1.0 and 0.6 ns, respectively, without the disturbance of inhomogeneous broadening. The measured spin relaxation time decreases rapidly from 1.1 ns at 10 K to 200 ps at 130 K. This large change in the spin relaxation time is well-explained in terms of the mechanism of acoustic phonon emission. In coupled quantum dots, the formation of antiferromagnetic coupling is directly observed. Electron spins are found to flip at 80 ps after photoexcitation via the interdot exchange interaction. The antiferromagnetic coupling exists at temperatures lower than 50–80 K. A model calculation based on the Heitler–London approximation supports the finding that the antiferromagnetic coupling is observable at low temperature. These carrier spin features in quantum dots are suitable for the future quantum computation.     

Piecewise-constant approximation of the potential profile of multiple quantum well intrinsic heterostructures

Knowledge of the energy band diagram is very important in semiconductor physics due to the fact that the band diagram influences almost all parts of the physics of a semiconductor device. In this paper we examine a piecewise-constant approximation of the potential profile through a comparison with a comprehensive self-consistent model, with regard to the active regions of QW semiconductor lasers and amplifiers. The validity of this approximation is then defined, thus giving an insight into the physics of QW structures.     

Theory of radiative and nonradiative transitions for semiconductor nanocrystals

Existing calculations on the radiative and nonradiative transitions in semiconductor crystallites are reviewed with particular emphasis on indirect band-gap materials like silicon for which the quantum confinement effects are more spectacular. It is shown that the crystallite gaps and radiative recombination rates can be predicted with fair accuracy. Effects related to atomic relaxation in the excited state (Stokes shift) are calculated and it is shown that small enough crystallites lead to self-trapped excitons which provide another source of luminescence, much less dependent on size effects. Nonradiative processes are then examined: intrinsic, due to Auger recombination, and extrinsic, due to dangling bond surface states. Both are found to play an essential role in the interpretation of experimental data. Finally, dielectric screening is studied, justifying the use of a reduced internal dielectric constant and providing an estimate of the Coulomb shift due to charging effects.