纳米结构ZnO晶体薄膜室温紫外激光发射

文章综述了纳米结构的氧化锌半导体薄膜在室温下自由激子的自发辐射以及由自由激子引起的受激发射的特性，阐述了在不同激发密度下室温紫外受激发射的机理．纳米结构氧化锌半导体薄膜是用激光分子束外延(L-MBE)技术生长在蓝宝石衬底上的．薄膜由密集而规则排列的纳米尺度的六角柱组成．这些纳米六角柱起着限制激子运动的作用，激子的量子尺寸效应，使激子的跃迁振子强度大幅度增强．同时六角柱之间的晶面组成了一个天然的激光谐振腔．室温下用三倍频的YAG脉冲激光激发，可从这些纳米结构的氧化锌薄膜中观测到很强的紫外激光发射．研究发现，在中等激发密度下，紫外受激发射是由于激子与激子间碰撞而引起的辐射复合．在高密度激发条件下，由于激子趋于离化，紫外受激发射主要由电子-空穴等离子体的辐射复合引起．由于纳米结构中激子的跃迁振子增强效应，在室温下测量到的光学增益高达320cm^-1，这比在同样条件下测量到的块状氧化锌晶体的光学增益要高一个量级以上．与传统的电子-空穴等离子体激光辐射相比，激子引起的受激发射可在较低的激发密度条件下实现．这在实际应用上很有价值．     

Random lasing in ZnO nanocrystals

Nanocrystalline ZnO powders can act as gain and scattering medium in a random laser where the light emission can be strongly amplified. In this work, we compare the luminescence properties of samples with different particle sizes in the regime of linear and nonlinear optics. In the high-excitation regime random lasing is observed in all samples. Here, the lasing threshold depends strongly on the size distribution in the ensemble. Additional characterization of the samples has been done by determining the absolute quantum efficiency of the radiative processes in the powder. The values are in the 10% range and the near-edge luminescence is strongly influenced by the particle sizes. We show that by annealing the nanocrystals coalesce to larger polycrystalline grains, which results in a new emission band at 3.333 eV due to the grain boundaries. Furthermore, it is found that in the annealed samples the threshold for random lasing could be considerably decreased.     

纳米ZnO薄膜的激子光致发光特性

报道了纳米ZnO薄膜激子光致发光(PL)与温度的关系。首先利用低压金属有机化学气相沉积(LPMOCVD)技术生长ZnS薄膜,然后将ZnS薄膜在氧气中于800℃下热氧化2h获得纳米ZnO薄膜。X射线衍射(XRD)结果表明,纳米ZnO薄膜具有六角纤锌矿多晶结构且具有择优(002)取向。室温下观察到一束强的紫外(326eV)光致发光(PL)和很弱的深能级(DL)发射。根据激子峰的半高宽(FWHM)与温度的关系,确定了激子纵向光学声子(LO)的耦合强度(ГLO)。     

Room-temperature laser emission of ZnO nanowires explained by many-body theory

Are excitons involved in lasing in ZnO nanowires or not? Our recently developed and experimentally tested quantum many-body theory sheds new light on this question. We measured the laser thresholds and Fabry-Pérot laser modes for three radically different excitation schemes. The thresholds, photon energies, and mode spacings can all be explained by our theory, without invoking enhanced light-matter interaction, as is needed in an earlier excitonic model. Our conclusion is that lasing in ZnO nanowires at room temperature is not of excitonic nature, as is often thought, but instead is electron-hole plasma lasing.     

Temperature dependence of excitonic luminescence from nanocrystalline ZnO films

The properties of the excitonic luminescence for nanocrystalline ZnO thin films are investigated by using the dependence of excitonic photoluminescence (PL) spectra on temperature. The ZnO thin films are prepared by thermal oxidation of ZnS films prepared by low-pressure metalorganic chemical vapor deposition (LP-MOCVD) technique. The X-ray diffraction (XRD) indicates that ZnO thin films have a polycrystalline hexagonal wurtzite structure with a preferred (0 0 2) orientation. A strong ultraviolet (UV) emission peak at 3.26 eV is observed, while the deep-level emission band is barely observable at room temperature. The strength of the exciton-longitudinal-optical (LO) phonon coupling is deduced from the temperature dependence of the full-width at half-maximum (FWHM) of the fundamental excitonic peak, decrease in exciton-longitudinal-optical (LO) phonon coupling strength is due to the quantum confinement effect.     

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.     

Electroluminescence study on electron hole plasma in strained SiGe epitaxial layers

The electroluminescence (EL) of thick fully strained SiGe layers is investigated in order to clarify the recombination mechanisms. In the investigated temperature range of 20–80 K and for SiGe thickness of 70–450 nm an electron–hole plasma (EHP) is observed even at low current densities of 1 Acm⁻². In SiGe-based quantum devices the EHP condition is expected to be attained at even lower injection levels. We used the band filling model for EHP to extract the renormalized gap of SiGe in dependence on the plasma density by performing a line shape analysis of EL spectra. The results were compared with the theoretical prediction. Based on this analysis as well as on measurements and modelling of the spectral photocurrent and the external quantum efficiency, we were able to evaluate parameters of recombination transitions for EHP in SiGe. Above 200 K there is an important contribution to EL from the silicon regions. For a better evaluation of the SiGe contribution, we compared EL of SiGe diodes with EL of pure silicon diodes.     

Direct observation of the mott transition in an optically excited semiconductor quantum well

We have studied density-dependent time-resolved photoluminescence from a 80 A InGaAs/GaAs single quantum well excited by picosecond pulses. We succeed in giving evidence for the transition from an exciton-dominated population to an unbound electron-hole pair population as the pair density increases. For pair densities below this excitonic Mott transition we observe a spectrally separate emission from free electron-hole pairs in addition to excitonic luminescence, thereby proving the coexistence of both species. Exciton binding energy and band gap remain unchanged even near the upper bound of this coexistence region. Above the Mott density we observe a purely exponential high energy tail of the photoluminescence and a redshift of the band gap with pair density. The transition occurs gradually between 1 x 10(10) and 1 x 10(11) cm(-2) at the carrier temperatures of our experiment.     

半导体微结构物理效应及其应用讲座第三讲半导体的激子效应及其在光电子器件中的应用

人们对半导体中的电子空穴对在库仑互作用下形成的激子态及其有关的物理性质进行了深入研究.激子效应对半导体中的光吸收、发光、激射和光学非线性作用等物理过程具有重要影响,并在半导体光电子器件的研究和开发中得到了重要的应用.与半导体体材料相比,在量子化的低维电子结构中,激子的束缚能要大得多,激子效应增强,而且在较高温度或在电场作用下更稳定.这对制作利用激子效应的光电子器件非常有利.近年来量子阱、量子点等低维结构研究获得飞速的进展,已大大促进了激子效应在新型半导体光源和半导体非线性光电子器件领域的应用.     

水溶性CdTe量子点的稳态和纳秒时间分辨光致发光光谱

报道了以飞秒脉冲激光为激发光源的水溶性CdTe量子点(QDs)的稳态荧光光谱和纳秒时间分辨荧光光谱.实验发现CdTe量子点的荧光光谱峰值位置随激发波长变化发生明显移动，激发脉冲波长越长，荧光峰位红移越大.荧光动力学实验数据显示，在400nm和800nm脉冲激光激发下，水溶性CdTe量子点的荧光光谱中均含有激子态和诱捕态两个衰减成分，两者的发射峰相距很近，诱捕态的发射峰波长较长.在800nm脉冲激光激发下的诱捕态成分占总荧光强度的比重比400nm激发下的约高3倍，其相对强度的这种变化导致了稳态荧光发射峰位的红移. 关键词： CdTe 量子点 时间分辨 荧光光谱 上转换荧光     

Pump power dependence of the electron-hole plasma luminescence in Ga-doped ZnO film

Time resolved two-photon absorption induced electron-hole plasma (EHP) luminescence of Ga-doped ZnO thin film was measured by an ultrafast optical Kerr gate (OKG) in femtosecond time regime. Experimental results showed that the buildup time of the EHP luminescence was strongly dependent on the excitation fluence. The dependence of the buildup time of EHP on excitation fluence probably arose mainly from the relaxation of the hot carriers due to the carrier-carrier interaction, which increased with the increase of excitation fluence.     

Exciton binding energies in II–VI compound strained layer superlattices

II–VI strained-layer superlattices are very efficient emitters of visible light. The dependence of the luminescence intensity on the excitation power density allows us to characterise the recombination processes involved in the emission. At low temperatures excitonic processes are dominant whereas electron-hole recombinations feature at room temperature. No special evidence of the dual nature of the emission is observed at intermediate temperatures because the optical transitions are broadened by well-width fluctuations. In spite of this we may estimate the exciton binding energy from the temperature dependence of the photoluminescence intensity, as long as the photoluminescence remains excitonic. This is the case for narrow wells in CdS---ZnS superlattices over the temperature range zero to room temperature. The estimated exciton binding energy measured in this way approaches the two dimensional limit but does not exceed it.     

Luminescence study of Si/Ge quantum dots

We present a photoluminescence (PL) study of Ge quantum dots embedded in Si. Two different types of recombination processes related to the Ge quantum dots are observed in temperature-dependent PL measurements. The Ge dot-related luminescence peak near 0.80 eV is ascribed to the spatially indirect recombination in the type-II band lineup, while a high-energy peak near 0.85 eV has its origin in the spatially direct recombination. A transition from the spatially indirect to the spatially direct recombination is observed as the temperature is increased. The PL dependence of the excitation power shows an upshift of the Ge quantum dot emission energy with increasing excitation power density. The blueshift is ascribed to band bending at the type-II Si/Ge interface at high carrier densities. Comparison is made with results derived from measurements on uncapped samples. For these uncapped samples, no energy shifts due to excitation power or temperatures are observed in contrast to the capped samples.     

高质量纳米ZnO薄膜的光致发光特性研究

报道了利用低压-金属有机物化学气相沉积技术生长纳米ZnS薄膜，然后，将ZnS薄膜在氧气中于800℃温度下进行热氧化制备高质量纳米ZnO薄膜.x射线衍射结果表明，纳米ZnO薄膜具有六角纤锌矿多晶结构.室温下观察到一束强的紫外(3.26 eV) 光致发光和很弱的深能级发射.根据激子峰的半高宽度与温度的关系确定了激子-纵向光学声子（LO）的耦合强度（ГLO）.由于量子限域效应使ГLO减少较多. 关键词： 光致发光 热氧化 激子 纳米ZnO薄膜     

Lasing behaviour from the condensation of polaronic excitons in a ZnO nanowire

Atoms under optical and magnetic trapping in a limited space at a very low temperature can lead to Bose-Einstein condensation (BEC),even in a one-dimensional (1D) optical lattice. However,can the confinment of dense excitons in a 1D semiconductor microstructure easily reach the excitonic BEC A lightly Mn(Ⅱ)-doped ZnO nanowire under a femtosecond laser pulse pump at room temperature produces single-mode lasing from coherent bipolaronic excitons,which is much like a macroscopic quantum state due to the condensation of the bipoaronic excitons if not real BEC. In this process,longitudinal biphonon binding with the exciton plays an important role. We revisit this system and propose possibility of bipolaronic exciton condensation. More studies are needed for this condensation phenomenon in 1D microcavity systems.     

量子点激子超辐射的条件和量子点集合的相干辐射

半导体量子点的激子超辐射出现的条件是本文激子超辐射的理论研究中的重点,我们的理论推导结果揭示要观测到半导体量子点的激子超辐射必须采用短于百飞秒的激发源。我们用ZnO单量子点观察到激子超辐射,同时测量和分析讨论了量子点集合的相干辐射性质,发现单量子点超辐射的二次方泵浦与辐射强度关系被大量量子点间的线性递增所掩盖。     

Metal-insulator transition in a HgTe quantum well under hydrostatic pressure

The 2D semimetal in a 20 nm (100) HgTe quantum well is characterized by a comparatively low overlap between the conduction and the valence bands induced by lattice mismatch. In the present paper we report the results of transport measurements in this quantum well under hydrostatic pressure of 14.4 kbar. By applying pressure we have further reduced the band overlap, thereby creating favorable conditions for the formation of the excitonic insulator state. As a result, we observed that the metallic-like temperature dependence of the conductivity at lowering temperature sharply changes to the activated behavior, signaling the onset of an excitonic insulator regime.     

Multi-photon-pumped stimulated emission from ZnO nanowires: A time-resolved study

In this work, we study temporal evolution of multi-photon-pumped stimulated emission from ZnO nanowires. In addition to second harmonic generation, ultraviolet stimulated emission is observed in ZnO nanowires under femtosecond pulse excitation at 800 nm. Sharp emission peaks appear when excitation flux reaches a threshold of 80 mJ/cm², which can be interpreted as lasing action in self-formed nanowire microcavities. Temporal evolution of the emission captured by Kerr shutter technique shows strong excitation-power dependence. The dynamic trace of stimulated emission exhibits a fast decay with a lifetime about 4.5 ps at intermediate excitation (∼100 mJ/cm²) and a lifetime about 2 ps at high excitation (>160 mJ/cm²). The difference in the lifetime can be attributed to different gain mechanisms related to excitonic interaction and electron-hole plasma, respectively.     

Effect of Droop Phenomenon in InGaN/GaN Blue Laser Diodes on Threshold Current

Electroluminescence(EL) and temperature-dependent photoluminescence measurements are performed to study the internal quantum efficiency droop phenomenon of blue laser diodes(LDs) before lasing. Based on the ABC mode, the EL result demonstrates that non-radiative recombination rates of LDs with threshold current densities of 4 and 6 kA/cm~2 are similar, while LD with threshold current density of 4 kA/cm~2 exhibits a smaller augerlike recombination rate compared with the one of 6 kA/cm~2. The internal quantum efficiency droop is more serious for LD with higher threshold current density. The internal quantum efficiency value estimated from temperature-dependent photoluminescence is consistent with EL measurements.     

ZnO粉末中无序激射现象时间分辨的研究

采用抽运-探测时间分辨方法实验研究了半导体材料ZnO纳米颗粒粉末中的无序激射现象.在2 67nm激光的抽运下，通过精确控制抽运光的能量和样品表面的抽运面积，获得了宽度小于1n m的单模无序激射光谱和多峰的多模无序激射光谱.时间分辨的抽运-探测结果显示，此时样 品的上能级寿命仅为几个皮秒，证明了ZnO粉末的单模无序光谱是受激辐射的结果. 关键词： 高散射介质 多重散射 抽运-探测 无序激射