Nonradiative recombination effect on photoluminescence decay dynamics in GaInNAs/GaAs quantum wells

The influence of nonradiative recombination on the photoluminescence (PL) decay dynamics in GaInNAs/GaAs quantum wells is studied by time-resolved photoluminescence under various excitation intensities. It is found that the PL decay process strongly depends on the excitation intensity. In particular, under the moderate excitation levels the PL decay curves exhibit unusual nonexponential behavior and show a convex shape. By introducing a new parameter of the effective concentration of nonradiative recombination centers into a rate equation, the observed results are well simulated. The cw PL data further demonstrate the nonradiative recombination effect on the optical properties of GaInNAs/GaAs quantum wells. (c) 2006 American Institute of Physics.

Nonradiative recombination effect on photoluminescence decay dynamics in GaInNAs/GaAs quantum wells - art. no. 61180Z

The nonradiative recombination effect on the photoluminescence (PL) decay dynamics in GaInNAs/GaAs quantum wells is studied by photoluminescence and time-resolved photoluminescence under various excitation intensities and temperatures. It is found that the PL decay dynamics strongly depends on the excitation intensity. In particular, under the moderate excitation levels the PL decay curves exhibit unusual non-exponential behavior and show a convex shape. By introducing a new concept of the effective concentration of nonradiative recombination centers into a rate equation, the observed results are well simulated. In the cw PL measurement, a rapid PL quenching is observed even at very low temperature and is of the excitation power dependence. These results further demonstrate that the non-radiative recombination process plays a very important role on the optical properties of GaInNAs/GaAs quantum wells.

Effect of nonradiative recombination on carrier dynamics in GaInNAs/GaAs quantum wells

The nonradiative recombination effect on carrier dynamics in GaInNAs/GaAs quantum wells is studied by time-resolved photoluminescence (TRPL) and polarization-dependent TRPL at various excitation intensities. It is found that both recombination dynamics and spin relaxation dynamics strongly depend on the excitation intensity. Under moderate excitation intensities the PL decay curves exhibit unusual non-exponential behaviour. This result is well stimulated by a rate equation involving both the radiative and non-radiative recombinations via the introduction of a new parameter of the effective concentration of nonradiative recombination centres in the rate equation. In the spin dynamics study, the spin relaxation also shows strong excitation power dependence. Under the high excitation power an increase of spin polarization degree with time is observed. This new finding provides a useful hint that the spin process can be controlled by excitation power in GaInNAs systems.

Nonradiative recombination centers in Ga(As,N) and their annealing behavior studied by Raman spectroscopy

Nitrogen-related defects in diluted Ga(As,N) have been detected by Raman scattering in resonance with the localized E+ transition. These defects are attributed to local vibrational modes of nitrogen dimers on Ga- and As-lattice sites. Rapid thermal annealing under appropriate conditions is found to be able to remove the nitrogen dimers. The required minimum annealing temperature coincides with the threshold-like onset of strong, near-band-gap photoluminescence. This finding suggests that the nitrogen dimers are connected with nonradiative recombination centers. (C) 2004 American Institute of Physics.

Effect of Calcination Temperature on Structural, Photoluminescence, and Thermo luminescence Properties of Y2O3:Eu3+ Nanophosphor

Red light emitting cubic Y1.95Eu0.05O3 nanophosphors have been synthesized by a low temperature solution combustion method using ethylene diamine tetra acetic acid (EDTA) as fuel. The systematic studies on the effect of calcination temperature on its structural, photoluminescence (PL), and thermoluminescence (TL) properties were reported. The crystallinity of the samples increases, and the strain is reduced with increasing calcination temperature. SEM micrographs reveal that samples lose their porous nature with an increase in calcination temperature. PL spectra show that the intensity of the red emission (611 nm) is highly dependent on the calcination temperature and is found to be 10 times higher when compared to as-formed samples. The optical band gap (E-g) was found to reduce with an increase of calcination temperature due to reduction of surface defects. The thermoluminescence (TL) intensity was found to be much enhanced in the 1000 degrees C calcined sample. The increase of PL and TL intensity with calcination temperature is attributed to the decrease of the nonradiative recombination probability, which occurs through the elimination of quenching defects. The trap parameters (E, b, s) were estimated from Chen's glow peak shape method and are discussed in detail for their possible usage in dosimetry.

Effect of the ratio of TMIn flow to group III flow on the properties of InGaN/GaN multiple quantum wells

Triple-axis x-ray diffraction (TXRD) and photoluminescence (PL) spectra are used to assess the influence of the ratio of TMIn flow to group III flow on structural defects, such as dislocations and interface roughness, and optical properties of multiple quantum wells(MQWs). In this paper the mean densities of edge and screw dislocations in InGaN/GaN MQWs are obtained by W scan of every satellite peak of (0002) symmetric and (1012) asymmetric diffractions. At the same time, the interface roughness is measured by the radio of the full width at half maximum of satellite peaks to the peak orders. The experimental results showed that the density of dislocation, especially of edge dislocation, and interface roughness increase with the increase of the ratio, which leads to the decrease of PL properties. It also can be concluded that the edge dislocation acts as nonradiative recombination centers in InGaN/GaN MQWs. Also noticed is that the variation of the ratio has more influence on edge dislocation than on screw dislocation.

Effect of trimethylgallium flow on the structural and optical properties of InGaN/GaN multiple quantum wells

InGaN/GaN multiple quantum wells (MQWs) are grown by metal-organic chemical vapour deposition on (0001) sapphire substrates. Triple-axis X-ray diffraction (TXRD) and photoluminescence (PL) spectra are used to assess the influence of trimethylgallium (TMGa) flow on structural defects, such as dislocations and interface roughness, and the optical properties of the MQWs. In this paper, a method, involving an ! scan of every satellite peak of TXRD, is presented to measure the mean dislocation density of InGaN/GaN MQWs. The experimental results show that under certain conditions which keep the trimethlyindium flow constant, dislocation density and interface roughness decrease with the increase of TMGa flow, which will improve the PL properties. It can be concluded that dislocations, especially edge dislocations, act as nonradiative recombination centres in InGaN/GaN MQWs. Also noticed is that changing the TMGa flow has more influence on edge dislocations than screw dislocations.

POWER DEPENDENCE OF THE RECOMBINATION PROCESSES IN THE INXGA1-XAS/GAAS SINGLE-QUANTUM-WELL

We have measured the power dependence of the photoluminesence spectra from a set of strained InxGa1-xAs/GaAs single quantum wells. The result shows that the excitation power has important effect on the carrier recombination processes. When the power increases from 0.5 to 14 mW, the photoluminescence from the barrier becomes more intense than that from the well and the trapping efficiency decreases. At high excitation level, the ratio of the radiative recombination rate to the nonradiative recombination rate of the barrier increases ten times than that at lower excitation level, while it only doubles for the well.

Photoacoustic study of the effect of doping concentration on the transport properties of GaAs epitaxial layers

We report a photoacoustic (PA) study of the thermal and transport properties of a GaAs epitaxial layer doped with Si at varying doping concentration, grown on GaAs substrate by molecular beam epitaxy. The data are analyzed on the basis of Rosencwaig and Gersho’s theory of the PA effect. The amplitude of the PA signal gives information about various heat generation mechanisms in semiconductors. The experimental data obtained from the measurement of the PA signal as a function of modulation frequency in a heat transmission configuration were fitted with the phase of PA signal obtained from the theoretical model evaluated by considering four parameters—viz., thermal diffusivity, diffusion coefficient, nonradiative recombination time, and surface recombination velocity—as adjustable parameters. It is seen from the analysis that the photoacoustic technique is sensitive to the changes in the surface states depend on the doping concentration. The study demonstrates the effectiveness of the photoacoustic technique as a noninvasive and nondestructive method to measure and evaluate the thermal and transport properties of epitaxial layers.

Effective recombination velocity of textured surfaces

Surface texturization is an effective way to enhance the absorption of light for optoelectronic devices but it also aggravates the surface recombination by enlarging the surface area. In order to evaluate the influence of texture structures on the surface recombination, an effective surface recombination velocity is defined which is assumed to have an equivalent recombination effect on a flat surface. Based on numerical and analytical calculation, the dependences of effective surface recombination on the pattern geometry, the surface recombination velocity, and the diffusion length are analyzed.

Spin-Polarized Localized Exciton Photoluminescence Dynamics in GaInNAs Quantum Wells

We have investigated spin polarization-related localized exciton photoluminescence (PL) dynamics in GaInNAs quantum wells by time-resolved PL spectroscopy. The emission energy dependence of PL polarization decay time as well as polarization-independent PL decay time suggests that the acoustic phonon scattering in the process of localized exciton transfer from the high-energy localized states to the low-energy ones dominates the PL polarization relaxation. By increasing the excitation power from 1 to 10 mW, the PL polarization decay time is changed from 0.17 to more than 1 ns, which indicates the significant effect of the trapping of localized electrons by nonradiative recombination centers. These experimental findings indicate that the spin-related PL polarization in diluted nitride semiconductors can be manipulated through carrier scattering and recombination process. (C) 2009 The Japan Society of Applied Physics

Dependence of optical properties on the structure of multi-layer self-organized InAs quantum dots emitting near 1.3 mu m

Self-organized InAs quantum dots (QDs) have been fabricated by molecular beam epitaxy and characterized by photoluminescence (PL). For both single- and multi-layer QDs, PL intensity of the first excited state is larger than that of the ground state at 15 K. Conversely, at room temperature (RT), PL intensity of the first excited state is smaller than that of the ground state. This result is explained by the phonon bottleneck effect. To the ground state, the PL intensities of the multi-layer QDs are larger than that of the single-layer QDs at 15 K, while the intensities are smaller than that of the single-layer QDs at RT. This is due to the defects in the multi-layer QD samples acting as the nonradiative recombination centers. The inter-diffusion of Ga and In atoms in the growth process of multi-layer QDs results in the PL blueshift of the ground state and broadening of the full-width at half-maximum (FWHM), which can be avoided by decreasing the spacers' growth temperature. At the spacers' growth temperature of 520degreesC, we have prepared the 5-layer QDs which emit near 1.3 mum with a FWHM of 31.7 meV at RT, and 27.9 meV at 77 K. (C) 2002 Published by Elsevier Science B.V.

Characterization of recombination centres in n-type Hg1-xCdxTe

The defect levels in Hg1-xCdxTe P+N junction photodiodes (x = 0.4) were first studied using deep-level transient spectroscopy. Two electron traps, E(1)(0.06) and E(2)(0.15), and two hole traps, H-1(0.075) and H-2(0.29), were obtained, Characteristic parameters-the minority lifetime of the devices and the dynamic resistance-area product at zero bias-are estimated according to these levels. Results show that these two minority levels may be important in controlling lifetime. We have studied the recombination mechanism of the hole trap H-2(0.29) further. It has a large activation energy and satisfies the formula sigma(T) = sigma(x) exp(-E(F)/E(T)). This reflects the fact that its recombination mechanism is multiphonon nonradiative recombination, which is rarely reported in narrow-bandgap materials.

Photoacoustic measurement of transport properties in doped GaAs epitaxial layers

The photoacoustic technique under heat transmission configuration is used to determine the effect of doping on both the thermal and transport properties of p- and n-type GaAs epitaxial layers grown on GaAs substrate by the molecular beam epitaxial method. Analysis of the data is made on the basis of the theoretical model of Rosencwaig and Gersho. Thermal and transport properties of the epitaxial layers are found by fitting the phase of the experimentally obtained photoacoustic signal with that of the theoretical model. It is observed that both the thermal and transport properties, i.e. thermal diffusivity, diffusion coefficient, surface recombination velocity and nonradiative recombination time, depend on the type of doping in the epitaxial layer. The results clearly show that the photoacoustic technique using heat transmission configuration is an excellent tool to study the thermal and transport properties of epitaxial layers under different doping conditions.

Synthesis and surface modification of semiconductor nanocrystals

The last decade has witnessed an exponential growth of activities in the field of nanoscience and nanotechnology worldwide, driven both by the excitement of understanding new science and by the potential hope for applications and economic impacts. The largest activity in this field up to date has been in the synthesis and characterization of new materials consisting of particles with dimensions in the order of a few nanometers, so-called nanocrystalline materials. [1-8] Semiconductor nanomaterials such as III/V or II/VI compound semiconductors exhibit strong quantum confinement behavior in the size range from 1 to 10 nm. Therefore, preparation of high quality semiconductor nanocrystals has been a challenge for synthetic chemists, leading to the recent rapid progress in delivering a wide variety of semiconducting nanomaterials. Semiconductor nanocrystals, also called quantum dots, possess physical properties distinctly different from those of the bulk material. Typically, in the size range from 1 to 10 nm, when the particle size is changed, the band gap between the valence and the conduction band will change, too. In a simple approximation a particle in a box model has been used to describe the phenomenon[9]: at nanoscale dimensions the degenerate energy states of a semiconductor separate into discrete states and the system behaves like one big molecule. The size-dependent transformation of the energy levels of the particles is called “quantum size-effect”. Quantum confinement of both the electron and hole in all three dimensions leads to an increase in the effective bandgap of the material with decreasing crystallite size. Consequently, both the optical absorption and emission of semiconductor nanaocrystals shift to the blue (higher energies) as the size of the particles gets smaller. This color tuning is well documented for CdSe nanocrystals whose absorption and emission covers almost the whole visible spectral range. As particle sizes become smaller the ratio of surface atoms to those in the interior increases, which has a strong impact on particle properties, too. Prominent examples are the low melting point [8] and size/shape dependent pressure resistance [10] of semiconductor nanocrystals. Given the size dependence of particle properties, chemists and material scientists now have the unique opportunity to change the electronic and chemical properties of a material by simply controlling the particle size. In particular, CdSe nanocrystals have been widely investigated. Mainly due to their size-dependent optoelectronic properties [11, 12] and flexible chemical processibility [13], they have played a distinguished role for a number of seminal studies [11, 12, 14, 15]. Potential technical applications have been discussed, too. [8, 16-27] Improvement of the optoelectronic properties of semiconductor nanocrystals is still a prominent research topic. One of the most important approaches is fabricating composite type-I core-shell structures which exhibit improved properties, making them attractive from both a fundamental and a practical point of view. Overcoating of nanocrystallites with higher band gap inorganic materials has been shown to increase the photoluminescence quantum yields by eliminating surface nonradiative recombination sites. [28] Particles passivated with inorganic shells are more robust than nanocrystals covered by organic ligands only and have greater tolerance to processing conditions necessary for incorporation into solid state structures or for other applications. Some examples of core-shell nanocrystals reported earlier include CdS on CdSe [29], CdSe on CdS, [30], ZnS on CdS, [31] ZnS on CdSe[28, 32], ZnSe on CdSe [33] and CdS/HgS/CdS [34]. The characterization and preparation of a new core-shell structure, CdSe nanocrystals overcoated by different shells (CdS, ZnS), is presented in chapter 4. Type-I core-shell structures as mentioned above greatly improve the photoluminescence quantum yield and chemical and photochemical stability of nanocrystals. The emission wavelengths of type-I core/shell nanocrystals typically only shows a small red-shift when compared to the plain core nanocrystals. [30, 31, 35] In contrast to type-I core-shell nanocrystals, only few studies have been conducted on colloidal type-II core/shell structures [36-38] which are characterized by a staggered alignment of conduction and valence bands giving rise to a broad tunability of absorption and emission wavelengths, as was shown for CdTe/CdSe core-shell nanocrystals. [36] The emission of type-II core/shell nanocrystals mainly originates from the radiative recombination of electron-hole pairs across the core-shell interface leading to a long photoluminescence lifetime. Type-II core/shell nanocrystals are promising with respect to photoconduction or photovoltaic applications as has been discussed in the literature.[39] Novel type-II core-shell structures with ZnTe cores are reported in chapter 5. The recent progress in the shape control of semiconductor nanocrystals opens new fields of applications. For instance, rod shaped CdSe nanocrystals can enhance the photo-electro conversion efficiency of photovoltaic cells, [40, 41] and also allow for polarized emission in light emitting diodes. [42, 43] Shape control of anisotropic nanocrystals can be achieved by the use of surfactants, [44, 45] regular or inverse micelles as regulating agents, [46, 47] electrochemical processes, [48] template-assisted [49, 50] and solution-liquid-solution (SLS) growth mechnism. [51-53] Recently, formation of various CdSe nanocrystal shapes has been reported by the groups of Alivisatos [54] and Peng, [55] respectively. Furthermore, it has been reported by the group of Prasad [56] that noble metal nanoparticles can induce anisotropic growth of CdSe nanocrystals at lower temperatures than typically used in other methods for preparing anisotropic CdSe structures. Although several approaches for anisotropic crystal growth have been reported by now, developing new synthetic methods for the shape control of colloidal semiconductor nanocrystals remains an important goal. Accordingly, we have attempted to utilize a crystal phase control approach for the controllable synthesis of colloidal ZnE/CdSe (E = S, Se, Te) heterostructures in a variety of morphologies. The complex heterostructures obtained are presented in chapter 6. The unique optical properties of nanocrystals make them appealing as in vivo and in vitro fluorophores in a variety of biological and chemical investigations, in which traditional fluorescence labels based on organic molecules fall short of providing long-term stability and simultaneous detection of multiple emission colours [References]. The ability to prepare water soluble nanocrystals with high stability and quantum yield has led to promising applications in cellular labeling, [57, 58] deep-tissue imaging, [59, 60] and assay labeling [61, 62]. Furthermore, appropriately solubilized nanocrystals have been used as donors in fluorescence resonance energy transfer (FRET) couples. [63-65] Despite recent progress, much work still needs to be done to achieve reproducible and robust surface functionalization and develop flexible (bio-) conjugation techniques. Based on multi-shell CdSe nanocrystals, several new solubilization and ligand exchange protocols have been developed which are presented in chapter 7. The organization of this thesis is as follows: A short overview describing synthesis and properties of CdSe nanocrystals is given in chapter 2. Chapter 3 is the experimental part providing some background information about the optical and analytical methods used in this thesis. The following chapters report the results of this work: synthesis and characterization of type-I multi-shell and type-II core/shell nanocrystals are described in chapter 4 and chapter 5, respectively. In chapter 6, a high–yield synthesis of various CdSe architectures by crystal phase control is reported. Experiments about surface modification of nanocrystals are described in chapter 7. At last, a short summary of the results is given in chapter 8.