Photoluminescence and optical absorption properties of silicon quantum dots embedded in Si-rich silicon nitride matrices

Silicon nitride (SiN_x) films were prepared with a gas mixture of SiH₄ and NH₃ on Si wafers using the plasma-enhanced chemical vapor deposition (PECVD) method. High-resolution transmission electron microscopy and infrared absorption have been used to reveal the existence of the Si quantum dots (Si QDs) and to determine the chemical composition of the silicon nitride layers. The optical properties of these structures were studied by photoluminescence (PL) spectroscopy and indicate that emission mechanisms are dominated by confined excitons within Si QDs. The peak position of PL could be controlled in the wavelength range from 1.5 to 2.2 eV by adjusting the flow rates of ammonia and silane gases. Absorbance spectra obtained in the transmission mode reveal optical absorption from Si QDs, which is in good correlation with PL properties. These results have implications for future nanomaterial deposition controlling and device applications.     

Electroluminescence with micro-watt output from ultra-small sized Si quantum dots/amorphous SiO2 multilayers prepared by laser crystallization method

We report the fabrication of Si quantum dots (QDs)/SiO₂ multilayers by using KrF excimer laser (248 nm) crystallization of amorphous Si/SiO₂ multilayered structures on ITO coated glass substrates. Raman spectra and transmission electron microscopy demonstrate the formation of Si QDs and the size can be controlled as small as 1.8 nm. After laser crystallization, Al electrode is evaporated to obtain light emitting devices and the room temperature electroluminescence (EL) can be detected with applying the DC voltage above 8 V on the top gate electrode. The luminescent intensity increases with increasing the applied voltage and the micro-watt light output is achieved. The EL behaviors for samples with different Si dot sizes are studied and it is found that the corresponding external quantum efficiency is significantly enhanced in sample with ultra-small sized Si QDs.     

Optical properties of Si-doped InAs/InP quantum dots

InAs quantum dots (QDs) were grown on InP substrates by low pressure-metalorganic chemical vapor deposition. Disilane (Si₂H₆) was used as an n-type dopant. The positions of Si doping were varied: buffer layer, capping layer, modulation doping, and QD itself. Surface treatment of InP by Si₂H₆ was also performed to see the effect of Si on InAs QD. Photoluminescence (PL) and atomic force microscopy (AFM) were used to characterize optical and structural properties of QDs, respectively. It was found that the PL peak positions varied from 0.73 to 0.88 eV with the position of Si doping. PL peak blue shift in modulation doped sample was explained in terms of state filling effect. It was found that Si doping at QD itself was the most effective way to obtain the strongest integrated PL intensity without degrading the QD size distribution.     

Quantum emission efficiency of nanocrystalline and amorphous Si quantum dots

The paper presents the comparison of emission efficiencies for crystalline Si quantum dots (QDs) and amorphous Si nanoclusters (QDs) embedded in hydrogenated amorphous (a-Si:H) films grown by the hot wire-CVD method (HW-CVD) at the variation of technological parameters. The correlations between the intensities of different PL bands and the volumes of Si nanocrystals (nc-Si:H) and/or an amorphous (a-Si:H) phase have been revealed using X-ray diffraction (XRD) and photoluminescence (PL) methods. These correlations permit to discuss the PL mechanisms in a-Si:H films with embedded nc-Si QDs. The QD parameters of nc-Si:H and a-Si:H QDs have been estimated from PL results and have been compared (for nc-Si QDs) with the parameters obtained by the XRD method. Using PL and XRD results the relations between quantum emission efficiencies for crystalline (η_cr) and amorphous (η_am) QDs have been estimated and discussed for all studied QD samples. It is revealed that a-Si:H films prepared by HW-CVD with the variation of wire temperatures are characterized by better passivation of nonradiative recombination centers in comparison with the films prepared at the variation of substrate temperatures or oxygen flows.     

Photoconductivity of Si/Ge/SiO<Subscript>x</Subscript> and Si/Ge/Si structures with germanium quantum dots

A nonmonotonic dependence of the lateral photoconductivity (PC) on the interband light intensity is observed in Si/Ge/Si and Si/Ge/SiO_x structures with self-organized germanium quantum dots (QDs): in addition to a stepped increase in PC, a stepped decrease in PC is also observed. The effect of temperature and drive field on these features of the PC for both types of structures with a maximum nominal thickness of the Ge layer (N_Ge) is studied. The results obtained are discussed in the context of percolation theory for nonequilibrium carriers localized in different regions of the structure: electrons in the silicon matrix and holes in QDs.     

Design,fabrication and optical characterization of GaAs photonic crystal nanocavity lasers with InAs quantum dots gain wafer-bonded onto Si substrates

We designed and fabricated III–V compound semiconductor two-dimensional photonic crystal (PhC) thin film slabs with quantum dots (QDs) inside formed on Si substrates for highly integrated silicon photonic circuits with built-in nanolasers. Defect-shifted L3 type PhC nanocavities formed in GaAs thin films embedding 1.3 μm-emitting InAs QDs layer-transferred onto Si substrates were investigated. Quality factors <1000 for the PhC nanocavities on SiO₂ were enhanced up to ∼8000 by removing SiO₂ to form air-bridge structures, resulting in room temperature, continuous wave lasing.     

Modulation of the photoluminescence of Si quantum dots by means of CO2 laser pre-annealing

Si quantum dots (QDs) embedded in SiO₂ can be normally prepared by thermal annealing of SiO_x (x < 2) thin film at 1100 °C in an inert gas atmosphere. In this work, the SiO_x thin film was firstly subjected to a rapid irradiation of CO₂ laser in a dot by dot scanning mode, a process termed as pre-annealing, and then thermally annealed at 1100 °C for 1 h as usual. The photoluminescence (PL) intensity of Si QD was found to be enhanced after such pre-annealing treatment. This PL enhancement is not due to the additional thermal budget offered by laser for phase separation, but attributed to the production of extra nucleation sites for Si dots within SiO_x by laser irradiation, which facilitates the formation of extra Si QDs during the subsequent thermal annealing.     

Effect of water and UV passivation on the luminescence of suspensions of silicon quantum dots

This article presents the evolution of the photo-luminescence (PL) of silicon quantum dots (QDs) with an average diameter of 5–6 nm dispersed in alcohol under different conditions. Two samples were considered after alcohol dispersion: freshly synthesized (kept in air for 2 days) QDs which do not exhibit luminescence and air-aged (kept in air for 2 years) QDs exhibiting red-IR luminescence. Experiments performed with addition of a small volume of water, followed by heating for different times showed that the oxidation occurs gradually until transforming totally the initial material in SiO₂. The oxidation process does not enable the appearance of PL from the Si core for dispersed non-aged powders, while it results in a blue shift of the PL maximum intensity for the aged ones. The results obtained after UV illumination clearly indicate an effect of the UV irradiation on the luminescence of QDs dispersed in aqueous environment, and the treatments with acidic water lead to the conclusion of a possible enhancement of the PL by hydrogen passivation of the non-radiative defects. This result should be taken into account for post-production treatments and applications, more particularly, considering a controlled and safe use of luminescent Si QDs.     

Carrier gas effects on the SiGe quantum dots formation

SiGe quantum dots (QDs) grown by ultra-high vacuum chemical vapor deposition using H₂ and He carrier gases are investigated and compared. SiGe QDs using He carrier gas have smaller dot size with a better uniformity in terms of dot height and dot base as compared to the H₂ carrier gas. There is a higher Ge composition and less compressive strain in the SiGe QDs grown in He than in H₂ as measured by Raman spectroscopy. The Ge content is higher for He growth than H₂ growth due to hydrogen induced Si segregation and the lower interdiffusivity caused by the more strain relaxation in the He-grown SiGe dots. The photoluminescence also confirms more compressive strain for H₂ growth than He growth. Hydrogen passivation and Ge-H cluster formation play an important role in the QDs growth.     

Water‐Dispersible Silicon‐Quantum‐Dot‐Containing Micelles Self‐Assembled from an Amphiphilic Polymer

The dispersion of silicon quantum dots (Si QDs) in water has not been established as well as that in organic solvents. It is now demonstrated that the excellent dispersion of Si QDs in water with photoluminescence (PL) quantum yields (QYs) comparable to those for hydrophobic Si QDs can be realized by combining the processes of hydrosilylation and self‐assembly. Hydrogen‐passivated Si QDs are initially hydrosilylated with 1‐dodecence. The toluene solution of the resulting dodecyl‐passivated Si QDs is mixed with the water solution of the amphiphilic polymer of Pluronic F127 to form an emulsion. Dodecyl‐passivated Si QDs are encapsulated in the micelles self‐assembled from F127 in the emulsion. The size of the Si‐QD‐containing micelles may be tuned in the range from 10 to 100 nm. Although self‐assembly in the emulsion causes the PL QY of Si QDs to decrease, after a few days of storage in ambient conditions, Si QDs encapsulated in the water‐dispersible micelles exhibit recovered PL QYs of ≈24% at the PL wavelength of ≈680 nm. The intensity of the PL from Si QDs encapsulated in the water‐dispersible micelles is >90% of the original value after 60 min ultraviolet illumination, indicating excellent photostability.     

Resonant Raman scattering of discrete hole states in self-assembled Si/Ge quantum dots

We report the first resonant electronic Raman spectroscopy study of discrete electronic transitions within small p-doped self-assembled Si/Ge quantum dots (QDs). A heavy hole (hh) to light hole (lh) Raman transition with a dispersionless energy of 105 meV and a resonance energy of the hh states to virtually localised electrons at the direct band gap of 2.5 eV are observed. The hh–lh transition energy shifts to lower values with increasing annealing temperature due to significant intermixing of Si and Ge in the QDs. Structural parameters of the small Si/Ge dots have been determined and introduced into 6-band k·p valence band structure calculations. Both the value of the electronic Raman transition of localised holes as well as the resonance energy at the E₀ gap are in excellent agreement with the calculations.     

硅BC8量子点太阳能电池中的多重激子效应

多重激子效应是指在纳米半导体晶体中,量子点吸收一个高能光子而产生多个电子-空穴对的过程,该效应可以提高单结太阳电池能量转换效率。利用碰撞电离机制和费米统计模型计算了工作温度300 K的单结硅BC8量子点太阳能电池在AM1.5G太阳光谱下的能量转换效率。对于波长在280~580 nm的入射光,多重激子效应可以大幅增强硅BC8量子点直径d>5.0 nm的量子点太阳电池的能量转换效率。硅纳米量子点的直径d=6.3~6.4 nm时,最大能量转换效率为51.6%。     

Optimum Quantum Yield of the Light Emission from 2 to 10 nm Hydrosilylated Silicon Quantum Dots

Optimizing the light‐emitting efficiency of silicon quantum dots (Si QDs) has been recently intensified by the demand of the practical use of Si QDs in a variety of fields such as optoelectronics, photovoltaics, and bioimaging. It is imperative that an understanding of the optimum light‐emitting efficiency of Si QDs should be obtained to guide the design of the synthesis and processing of Si QDs. Here an investigation is presented on the characteristics of the photoluminescence (PL) from hydrosilylated Si QDs in a rather broad size region (≈2–10 nm), which enables an effective mass approximation model to be developed, which can very well describe the dependence of the PL energy on the QD size for Si QDs in the whole quantum‐confinement regime, and demonstrates that an optimum PL quantum yield (QY) appears at a specific QD size for Si QDs. The optimum PL QY results from the interplay between quantum‐confinement effect and surface effect. The current work has important implications for the surface engineering of Si QDs. To optimize the light‐emission efficiency of Si QDs, the surface of Si QDs must be engineered to minimize the formation of defects such as dangling bonds at the QD surface and build an energy barrier that can effectively prevent carriers in Si QDs from tunneling out.     

Sensitizing effects of ZnO quantum dots on red-emitting Pr-doped SiO2 phosphor

In this study, red cathodoluminescence (CL) (λ_emission=614 nm) was observed from Pr³⁺ ions in a glassy (amorphous) SiO₂ host. This emission was enhanced considerably when ZnO quantum dots (QDs) were incorporated in the SiO₂:Pr³⁺ suggesting that the ZnO QDs transferred excitation energy to Pr³⁺ ions. That is, ZnO QDs acted to sensitize the Pr³⁺ emission. The sol–gel method was used to prepare ZnO–SiO₂:Pr³⁺ phosphors with different molar ratios of Zn to Si. The effects of the ZnO QDs concentration and the possible mechanisms of energy transfer from ZnO to Pr³⁺ are discussed. In addition, the electronic states and the chemical composition of the ZnO–SiO₂:Pr³⁺ phosphors were analyzed using X-ray photoelectron spectroscopy (XPS).     

Interband photoconductivity of Ge/Si structures with self-organized quantum rings

At low temperatures a lateral photoconductivity (PC) of Ge/Si (1 0 0) self-organized quantum rings (QRs) structures as a function of interband light intensity has been investigated for different values of lateral voltage and temperature. In contrast to self-organized Ge/Si quantum dots (QDs) structures (grown at the same conditions) where the stepped PC was registered, for QRs structures essential smoothing of PC steps was observed. Such behavior is determined by decreasing of strain potential around QRs in conductive Si matrix due to a transfer of Ge atoms from the center of QDs to its periphery accompanied by Ge/Si intermixing.     

Direct assembly of in situ templated CdSe quantum dots via crystalline lamellae structure of polyamide 66

A simple concept is proposed for templating in situ synthesised CdSe quantum dots (QDs) into an organised nano-pattern using the crystalline lamellae structure of polyamide 66 (PA66). The morphology obtained for PA66 and the hybrid material on Si/SiO _x solid substrate was characterised by means of atomic force microscope. Controlling the PA66 concentration in solution and the organic–inorganic interactions are found to be the keys factors to direct the assembly of CdSe QDs along the PA66 linear crystalline structure. This simple approach could be opened a new avenue for a large spectrum of innovative high-tech applications.     

Growth of high-density InGaSb quantum dots on silicon atoms irradiated GaAs substrates

We discuss a technique that allows us to grow high-density GaSb and InGaSb quantum dots (QDs) on (0 0 1)-oriented GaAs substrates. We study the use of Si atom irradiation on the substrate surface as an anti-surfactant before the QDs fabrication. It is clear that the densities of GaSb and InGaSb QDs are drastically enhanced with the Si atom irradiation. Photoluminescence intensities from these QDs are also increased with the Si atom irradiation. These results indicate that the Si atom irradiation technique is useful to improve the properties of the Sb-based QDs.     

All‐optical modulation based on silicon quantum dot doped SiOx:Si‐QD waveguide

All‐optical modulation based on silicon quantum dot doped SiO_x:Si‐QD waveguide is demonstrated. By shrinking the Si‐QD size from 4.3 nm to 1.7 nm in SiO_x matrix (SiO_x:Si‐QD) waveguide, the free‐carrier absorption (FCA) cross section of the Si‐QD is decreased to 8 × 10⁻¹⁸ cm² by enlarging the electron/hole effective masses, which shortens the PL and Auger lifetime to 83 ns and 16.5 ps, respectively. The FCA loss is conversely increased from 0.03 cm⁻¹ to 1.5 cm⁻¹ with the Si‐QD size enlarged from 1.7 nm to 4.3 nm due to the enhanced FCA cross section and the increased free‐carrier density in large Si‐QDs. Both the FCA and free‐carrier relaxation processes of Si‐QDs are shortened as the radiative recombination rate is enlarged by electron–hole momentum overlapping under strong quantum confinement effect. The all‐optical return‐to‐zero on‐off keying (RZ‐OOK) modulation is performed by using the SiO_x:Si‐QD waveguides, providing the transmission bit rate of the inversed RZ‐OOK data stream conversion from 0.2 to 2 Mbit/s by shrinking the Si‐QD size from 4.3 to 1.7 nm.     

Si quantum dot structures and their applications

This paper presents briefly the history of emission study in Si quantum dots (QDs) in the last two decades. Stable light emission of Si QDs and NCs was observed in the spectral ranges: blue, green, orange, red and infrared. These PL bands were attributed to the exciton recombination in Si QDs, to the carrier recombination through defects inside of Si NCs or via oxide related defects at the Si/SiOx interface. The analysis of recombination transitions and the different ways of the emission stimulation in Si QD structures, related to the element variation for the passivation of surface dangling bonds, as well as the plasmon induced emission and rare earth impurity activation, have been presented.The different applications of Si QD structures in quantum electronics, such as: Si QD light emitting diodes, Si QD single union and tandem solar cells, Si QD memory structures, Si QD based one electron devices and double QD structures for spintronics, have been discussed as well. Note the significant worldwide interest directed toward the silicon-based light emission for integrated optoelectronics is related to the complementary metal-oxide semiconductor compatibility and the possibility to be monolithically integrated with very large scale integrated (VLSI) circuits. The different features of poly-, micro- and nanocrystalline silicon for solar cells, that is a mixture of both amorphous and crystalline phases, such as the silicon NCs or QDs embedded in a α-Si:H matrix, as well as the thin film 2-cell or 3-cell tandem solar cells based on Si QD structures have been discussed as well. Silicon NC based structures for non-volatile memory purposes, the recent studies of Si QD base single electron devices and the single electron occupation of QDs as an important component to the measurement and manipulation of spins in quantum information processing have been analyzed as well.     

掺杂对多层Ge/Si(001)量子点光致发光的影响

利用超高真空化学气相沉积设备, 在Si (001) 衬底上外延生长了多个四层Ge/Si量子点样品. 通过原位掺杂的方法, 对不同样品中的Ge/Si量子点分别进行了未掺杂、磷掺杂和硼掺杂. 相比未掺杂的样品, 磷掺杂不影响Ge/Si量子点的表面形貌, 但可以有效增强其室温光致发光; 而硼掺杂会增强Ge/Si量子点的合并, 降低小尺寸Ge/Si量子点的密度, 但其光致发光会减弱. 磷掺杂增强Ge/Si量子点光致发光的原因是, 磷掺杂为Ge/Si量子点提供了更多参与辐射复合的电子. 关键词： Ge/Si量子点 磷掺杂 光致发光