Influence of Mg Composition on Optical Properties of Exciton Confinement in Strained Wurtzite ZnO/MgxZn1-xO Cylindrical Quantum Dots

Based on the effective-mass approximation and variational approach, excitonic optical properties are investigated theoretically in strained wurtzite (WZ) ZnO/Mg_xZn_1-xO cylindrical quantum dots (QDs) for four different Mg compositions: x=0.08, 0.14, 0.25, and 0.33, with considering a three-dimensional carrier confinement in QDs and a strong built-in electric field effect due to the piezoelectricity and spontaneous polarization. The ground-state exciton binding energy, the interband emission wavelength, and the radiative lifetime as functions of the QD structural parameters (height and radius) are calculated in detail. The computations are performed in the case of finite band offset. Numerical results elucidate that Mg composition has a significant influence on the exciton states and optical properties of ZnO/Mg_xZn_1-xO QDs. The ground-state exciton binding energy increases with increasing Mg composition and the increment tendency is more prominent for small height QDs. As Mg composition increases, the interband emission wavelength has a blue-shift if the dot height L<3.5 nm, but the interband emission wavelength has a red-shift when L>3.5 nm. Furthermore, the radiative lifetime increases rapidly with increasing Mg composition if the dot height L>3 nm and the increment tendency is more prominent for large height QDs. The physical reason has been analyzed in depth.     

Influence of Mg content on optical properties of exciton confinement in wurtzite ZnO/MgxZn1−xO coupled quantum dots

Based on the framework of effective-mass approximation and variational approach, optical properties of exciton are investigated theoretically in ZnO/Mg_xZn_1−xO vertically coupled quantum dots (QDs), with considering the three-dimensional confinement of electron and hole pair and the strong built-in electric field effects. The exciton binding energy, the emission wavelength and the oscillator strength as functions of the structural parameters (the dot height, the barrier thickness between the coupled wurtzite ZnO QDs and Mg content x in the barrier layers) is calculated in detail. The results elucidate that Mg content have a significant influence on the exciton state and optical properties of ZnO coupled QDs. When Mg content x increases, the strong built-in electric field increases and leads to the redshift of the effective band gap of the Mg_xZn_1−xO layer. These theoretical results are useful for design and application of some important photoelectronic devices constructed by using ZnO strained QDs.     

Radiative life time of an exciton confined in a strained GaN/Ga1-xAlxN cylindrical dot: built-in electric field effects

The binding energy of an exciton in a wurtzite GaN/GaAlN strained cylindrical quantum dot is investigated theoretically.The strong built-in electric field due to the spontaneous and piezoelectric polarizations of a GaN/GaAlN quantum dot is included.Numerical calculations are performed using a variational procedure within the single band effective mass approximation.Valence-band anisotropy is included in our theoretical model by using different hole masses in different spatial directions.The exciton oscillator strength and the exciton lifetime for radiative recombination each as a function of dot radius have been computed.The result elucidates that the strong built-in electric field influences the oscillator strength and the recombination life time of the exciton.It is observed that the ground state exciton binding energy and the interband emission energy increase when the cylindrical quantum dot height or radius is decreased,and that the exciton binding energy,the oscillator strength and the radiative lifetime each as a function of structural parameters (height and radius) sensitively depend on the strong built-in electric field.The obtained results are useful for the design of some opto-photoelectronic devices.     

Hydrostatic pressure effects on exciton states in InAs/GaAs quantum dots

Based on the effective-mass approximation, the hydrostatic pressure effects on exciton states in InAs/GaAs self-assembled quantum dots (QDs) are studied by means of a variational method. Numerical results show that the exciton binding energy has a minimum with increasing dot height for any hydrostatic pressure. The interband emission energy increases when the hydrostatic pressure increases. In particular, we find that hydrostatic pressure has a remarkable effect on exciton states for small QD size. Our results are in agreement with experiment measurements.     

Optical properties of exciton confinement in wurtzite ZnO/MgxZn1−xO coupled quantum dots

Based on the framework of effective-mass approximation and variational approach, optical properties of exciton are investigated theoretically in ZnO/Mg_xZn_1−xO vertically coupled quantum dots (QDs), with considering the three-dimensional confinement of electron and hole pair and the strong built-in electric field effects due to the piezoelectricity and spontaneous polarization. The exciton binding energy, the emission wavelength and the oscillator strength as functions of the different structural parameters (the dot height and the barrier thickness between the coupled wurtzite ZnO QDs) are calculated with the built-in electric field in detail. The results elucidate that structural parameters have a significant influence on the exciton state and optical properties of ZnO coupled QDs. These results show the optical and electronic properties of the quantum dot that can be controlled and also tuned through the nanoparticle size variation.     

Exciton states and optical transitions in InGaN/GaN quantum dot nanowire heterostructures: Strong built-in electric field and dielectric mismatch effects

Considering the strong built-in electric field (BEF), dielectric-constant mismatch and 3D confinement of the electron and hole, the exciton states and interband optical transitions in [0 0 0 1]-oriented Ga-rich wurtzite In_xGa_1−xN/GaN strained quantum dot (QD) nanowire heterostructures are investigated theoretically using a variational approach under the effective mass approximation. We find that the strong BEF gives rise to an obvious reduction of the effective band gap of QDs and leads to a remarkable electron-hole spatial separation. The BEF, QD height and radius, and dielectric mismatch effects have a significant influence on exciton binding energy, electron interband optical transitions, and the radiative decay time. Our calculations show that the radiative decay time of the redshifted transitions is large and increases almost exponentially when the QD height increases, which is in good agreement with the previous experimental and theoretical results.     

Electronic and optical properties of CdS/CdZnS nanocrystals

Cd1-x ZnxS nanocrystals are prepared by a co-precipitation method with different atomic fractions of Zn.The texture,structural transformation and optical properties with increasing x value in Cd1-x ZnxS are studied with scanning electron microscopy,electron diffraction patterning,and absorption spectra respectively.Quantum confinement in a strained CdS/Cd1-xZnxS related nanodot with various Zn content values is investigated theoretically.Binding energies on exciton bound CdS/CdxZn1-xS quantum dot are computed,with consideration of the internal electric field induced by the spontaneous and piezoelectric polarizations,and thereby the interband emission energy is calculated as a function of the dot radius.The optical band gap from the UV absorption spectrum is compared with the interband emission energy computed theoretically.Our results show that the average diameter of composite nanoparticles ranges from 3 nm to 6 nm.The X-ray diffraction pattern shows that all the peaks shift towards the higher diffracting angles with an increase in Zn content.The lattice constant gradually decreases as the Zn content increases.The strong absorption edge shifts towards the lower wavelength region and hence the band gap of the films increases as the Zn content increases.The values of the absorption edge are found to shift towards the shorter wave length region and hence the direct band gap energy varies from 2.5 eV for the CdS film and 3.5 eV for the ZnS film.Our numerical results are in good agreement with the experimental results.     

Ionized Acceptor Bound Exciton States in Wurtzite GaN/Al_xGa(1-x)N Cylindrical Quantum Dot

Based on the framework of the effective-mass approximation,the ionized acceptor bound exciton(A-,X) binding energy and the emission wavelength are investigated for a cylindrical wurtzite(WZ) GaN/Al x Ga1-x N quantum dot(QD) with finite potential barriers by means of a variational method.Numerical results show that the binding energy and the emission wavelength highly depend on the QD size,the position of the ionized acceptor and the Al composition x of the barrier material Al x Ga1-x N.The binding energy and the emission wavelength are larger when the acceptor is located in the vicinity of the left interface of the QD.In particular,the binding energy of(A-,X) complex is insensitive to the dot height when the acceptor is located at the left boundary of the QD.The ionized acceptor bound exciton binding energy and the emission wavelength are both increased if Al composition x is increased.     

Exciton states in zinc-blende InGaN/GaN quantum dot

Within the framework of effective-mass approximation, exciton states confined in zinc-blende(ZB) InGaN/GaN quantum dot(QD) are investigated by means of a variational approach, considering finite band offsets. The ground-state exciton binding energy and the interband emission energy are investigated as functions of QD structural parameters in detail. Numerical results show clearly that both the QD size and In content of InGaN have a significant influence on the exciton states and interband optical transitions in the ZB InGaN/GaN QD.     

Non-radiative exciton recombination through excitation energy transfer in quantum dot clusters

Excitation energy transfer (EET) processes in CdSe/CdZnS quantum dot (QD) clusters have been investigated in this study by measuring their time-resolved and spectrally resolved fluorescence intensities. The contributions of radiative and non-radiative exciton recombination through EET are evaluated, where the latter is expected to occur in a large class of QD ensembles because of the presence of nonluminescent QDs. It appears that the fluorescence decay in larger QDs serving as acceptor does not show an initial rise, in addition the lifetime of the acceptor QD is independent of the excitation wavelength, suggesting that an EET is followed mostly by non-radiative recombination.     

闪锌矿GaN/AlGaN量子点中激子态及光学性质的研究

在有效质量近似的框架下,运用变分方法研究闪锌矿GaN/AlGaN量子点中的激子态及相关光学性质,探讨电子与空穴在量子点中的三维空间受限和有限势效应.数值计算结果显示,当量子点的尺寸增加时, 量子尺寸效应对电子和空穴的影响减弱,基态激子结合能和带间光跃迁能也都降低;而当该量子点中垒层AlGaN中 Al含量增加时,提高了量子点对电子和空穴的束缚作用, 同时基态激子结合能和带间光跃迁能都增加.数值的理论结果与相关实验测量结果一致.     

Electric field effects on optical properties in zinc-blende InGaN/GaN quantum dot

The effect of electric field on exciton states and optical properties in zinc-blende (ZB) InGaN/GaN quantum dot (QD) are investigated theoretically in the framework of effective-mass envelop function theory. Numerical results show that the electric field leads to a remarkable reduction of the ground-state exciton binding energy, interband transition energy, oscillator strength and linear optical susceptibility in InGaN/GaN QD. It is also found that the electric field effects on exciton states and optical properties are much more obvious in QD with large size. Moreover, the ground-state exciton binding energy and oscillator strength are more sensitive to the variation of indium composition in InGaN/GaN QD with small indium composition. Some numerical results are in agreement with the experimental measurements.     

Excited states and multi-exciton complexes in single CdTe quantum dots

We present an optical study of excited states in single CdTe quantum dot (QDs). Using micro-photoluminescence excitation spectroscopy, absorption up to two confined excited levels have been observed in some dots. Power-dependent micro-photoluminescence is then used to study the occupation of excited states. The emission pattern is characteristic of the increase of the exciton number in the QD (shell-filling). A clear identification of the different multi-exciton complexes has been obtained in a highly symmetric dot. The evolution of the different multi-exciton intensities can then be reproduced by solving the rate equations for multi-exciton state occupancy and the fit by this simple model provides an estimate of the radiative lifetime of the different multi-exciton complexes.     

Mg掺杂ZnO纳米晶的低温共沉淀法制备及光学性质

采用共沉淀(co-precipitation)法制备了Mg掺杂ZnO纳米晶,分别用X射线衍射(XRD)、傅立叶变换红外光谱(FTIR)、紫外可见吸收(UV-Vis)光谱、光致发光(PL)光谱、透射电镜(TEM)、电子顺磁共振(EPR)等分析手段对样品进行了表征。探究了Mg离子在ZnO纳米晶中的存在状态,ZnO纳米晶颗粒尺寸和发射光谱随Mg掺杂浓度的变化,并对其发光机理进行了分析。结果表明:Mg离子在ZnO晶格中以部分晶格位,部分间隙位的方式存在,没有形成MgO表面壳层结构;随Mg掺杂浓度的增大,ZnO纳米晶的颗粒尺寸变小,发射光的光强增大。发射光的最佳激发波长为342nm,中心波长为500nm,荧光量子产率为22.8%。实验分析表明:Mg离子的掺杂在ZnO纳米晶中引入了锌空位(VZn),间隙位的镁离子(IMg),提供了新的复合中心,从而增强了ZnO纳米晶的光致发光。     

铜掺杂氧化锌纳米棒的非线性光学响应竞争特性

利用飞秒脉冲激光激发Cu掺杂ZnO纳米棒,研究其特有的非线性光学性质和激发机制。在激发波长为750 nm的荧光光谱中,二次谐波峰非常弱,几乎可以忽略,存在非常强的激子发光峰和Cu掺杂导致缺陷发光峰。激发强度的增大会导致这两个发光峰强度呈非线性增大,激子发光峰位产生明显红移,而缺陷发光峰位没有变化。进一步增大激发强度,缺陷发光峰强度会出现饱和甚至有所下降,而激子发光峰强度持续增大。当激发波长增加到760 nm时,从样品的荧光光谱可以清楚地识别到二次谐波峰和激子发光峰以及缺陷发光峰并存。随着激发波长的进一步增加,二次谐波强度不断增大,而激子发光峰和缺陷发光峰的强度却随之下降。当激发波长为790 nm和800 nm时,未发现激子发光峰和缺陷发光峰,非线性光谱以二次谐波为主导。研究结果表明,通过选择合适的激发波长和激发强度,可以实现发光颜色的转变,使得Cu掺杂ZnO纳米棒在全光显示方面具有潜在的发展前景。     

Photo-physical and lasing characterisation of a polyparaphenylenevinylene (PPV) neat film

The wave-guided travelling-wave laser action (amplified spontaneous emission) of a neat film of poly(p-phenylenevinylene) (PPV) on a quartz glass substrate prepared by a sulfinyl precursor technique is studied. The samples are transversally pumped with picosecond excitation pulses (wavelength 347.15 nm, duration 35 ps). Lasing occurs at 550 nm. The optical constants of the neat films are determined by transmittance measurements exploiting the multiple beam interference in the transparency region. A fluorescence spectroscopic characterisation is carried out determining the fluorescence quantum distribution, fluorescence quantum yield, degree of fluorescence polarisation, and fluorescence lifetime. The emitting chromophore size (emitting singlet exciton extension) is determined by the ratio of exciton radiative lifetime to repeat-unit based radiative lifetime. The obtained size of about two repeat units is discussed in a disordered solid-state polymer model.     

Exciton emission dynamics in single InAs/GaAs quantum dots due to the existence of plasmon-field-induced metastable states in the wetting layer

A very long lifetime exciton emission with non-single exponential decay characteristics has been reported for single InA-s/GaAs quantum dot(QD) samples,in which there exists a long-lived metastable state in the wetting layer(WL)through radiative field coupling between the exciton emissions in the WL and the dipole field of metal islands.In this article we have proposed a new three-level model to simulate the exciton emission decay curve.In this model,assuming that the excitons in a metastable state will diffuse and be trapped by QDs,and then emit fluorescence in QDs,a stretchedlike exponential decay formula is derived as I(t)=At~(β-1)e~(-(rt)β),which can describe well the long lifetime decay curve with an analytical expression of average lifetime     

Interband optical absorption in a strained CdxZn1−xO/ZnO quantum dot

Numerical calculations of the excitonic absorption spectra in a strained Cd_xZn_1−xO/ZnO quantum dot are investigated for various Cd contents. We calculate the quantized energies of the exciton as a function of dot radius for various confinement potentials and thereby the interband emission energy is computed considering the internal electric field induced by the spontaneous and piezoelectric polarizations. The optical absorption as a function of photon energy for different dot radii is discussed. Decrease of exciton binding energy and the corresponding optical band gap with the Cd concentration imply that the confinement of carriers decreases with composition x. The main results show that the confined energies and the transition energies between the excited levels are significant for smaller dots. Non-linearity band gap with the increase in Cd content is observed for smaller dots in the strong confinement region and the magnitude of the absorption spectra increases for the transitions between the higher excited levels.     

Exciton binding energy and the optical absorption coefficient in a strained CdxZn1−xO/ZnO quantum dot

Numerical calculations of the excitonic absorption spectra in a strained Cd_xZn_1?xO/ZnO quantum dot are investigated for various Cd contents. We calculate the quantized energies of the exciton as a function of dot radius for various confinement potentials and thereby the interband emission energy is computed considering the internal electric field induced by the spontaneous and piezoelectric polarizations. The optical absorption as a function of photon energy for different dot radii is discussed. Decrease of exciton binding energy and the corresponding optical band gap with the Cd concentration imply that the confinement of carriers decreases with composition x. The main results show that the confined energies and the transition energies between the excited levels are significant for smaller dots. Non-linearity band gap with the increase in Cd content is observed for smaller dots in the strong confinement region and the magnitude of the absorption spectra increases for the transitions between the higher excited levels.     

Effects of hydrostatic pressure on ionized donor bound exciton states in strained wurtzite GaN/AlxGa1−xN cylindrical quantum dots

Based on the effective-mass approximation and variational procedure, ionized donor bound exciton (D⁺, X) states confined in strained wurtzite (WZ) GaN/Al_xGa_1-xN cylindrical (disk-like) quantum dots (QDs) with finite-height potential barriers are investigated, with considering the influences of the built-in electric field (BEF), the biaxial strain dependence of material parameters and the applied hydrostatic pressure. The Schrödinger equation via the proper choice of the donor bound exciton trial wave function is solved. The behaviors of the binding energy of (D⁺, X) and the optical transition associated with (D⁺, X) are examined at different pressures for different QD sizes and donor positions. In our calculations, the effective masses of electron and hole, dielectric constants, phonon frequencies, energy gaps, and piezoelectric polarizations are taken into account as functions of biaxial strain and hydrostatic pressure. Our results show that the hydrostatic pressure, the QD size and the donor position have a remarkable influence on (D⁺, X) states. The hydrostatic pressure generally increases the binding energy of (D⁺, X). However, the binding energy tends to decrease for the QDs with large height and lower Al composition (x<0.3) if the donor is located at z₀≤0. The optical transition energy has a blue-shift (red-shift) if the hydrostatic pressure (QD height) increases. For the QDs with small height and low Al composition, the hydrostatic pressure dependence of the optical transition energy is more obvious. Furthermore, the relationship between the radiative decay time and hydrostatic pressure (QD height) is also investigated. It is found that the radiative decay time increases with pressure and the increment tendency is more prominent for the QDs with large height. The radiative decay time increases exponentially reaching microsecond order with increasing QD height. The physical reason has been analyzed in depth.