Silicon quantum wire array fabrication by electrochemical and chemical dissolution of wafers
TL;DR: In this paper, free standing Si quantum wires can be fabricated without the use of epitaxial deposition or lithography using electrochemical and chemical dissolution steps to define networks of isolated wires out of bulk wafers.
Abstract: Indirect evidence is presented that free‐standing Si quantum wires can be fabricated without the use of epitaxial deposition or lithography. The novel approach uses electrochemical and chemical dissolution steps to define networks of isolated wires out of bulk wafers. Mesoporous Si layers of high porosity exhibit visible (red) photoluminescence at room temperature, observable with the naked eye under <1 mW unfocused (<0.1 W cm−2) green or blue laser line excitation. This is attributed to dramatic two‐dimensional quantum size effects which can produce emission far above the band gap of bulk crystalline Si.
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TL;DR: It is demonstrated that light amplification is possible using silicon itself, in the form of quantum dots dispersed in a silicon dioxide matrix, which opens a route to the fabrication of a silicon laser.
Abstract: Adding optical functionality to a silicon microelectronic chip is one of the most challenging problems of materials research. Silicon is an indirect-bandgap semiconductor and so is an inefficient emitter of light. For this reason, integration of optically functional elements with silicon microelectronic circuitry has largely been achieved through the use of direct-bandgap compound semiconductors. For optoelectronic applications, the key device is the light source--a laser. Compound semiconductor lasers exploit low-dimensional electronic systems, such as quantum wells and quantum dots, as the active optical amplifying medium. Here we demonstrate that light amplification is possible using silicon itself, in the form of quantum dots dispersed in a silicon dioxide matrix. Net optical gain is seen in both waveguide and transmission configurations, with the material gain being of the same order as that of direct-bandgap quantum dots. We explain the observations using a model based on population inversion of radiative states associated with the Si/SiO2 interface. These findings open a route to the fabrication of a silicon laser.
2,204 citations
Cites background or methods from "Silicon quantum wire array fabricat..."
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...But light ampli®cation in silicon is dif®cult because (1) it has ef®cient free carrier absorption, which reduces the net gain available for laser action(14); (2) there is signi®cant Auger saturation of the luminescence intensity at high power(9); and (3) there is signi®cant size-dependence of the radiative energies in Si nanostructures, which yields large inhomogeneous broadening and signi®cant optical losses in the system(16)....
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...A ®t to the data with equation (1) is shown as the dashed line....
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1,762 citations
TL;DR: LPSiNPs are presented, a new type of multifunctional nanostructure with a low-toxicity degradation pathway for in vivo applications that can carry a drug payload and of which the intrinsic near-infrared photoluminescence enables monitoring of both accumulation and degradation in vivo.
Abstract: Nanomaterials that can cir culate in the body hold great potential to diagnose and treat disease 1‐4 . For such applications, it is important that the nanomaterials be harmlessly eliminated from the body in a reasonable period of time after they carry out their diagnostic or therapeutic function. Despite efforts to improve their targeting efficiency, significant quantities of systemically administered nanomaterials are cleared by the mononuclear phagocytic system before finding their targets, increasing the likelihood of unintended acute or chronic toxicity. However, there has been little effort to engineer the self-destruction of errant nanoparticles into non-toxic, systemically eliminated products. Here, we present luminescent porous silicon nanoparticles (LPSiNPs) that can carry a drug payload and of which the intrinsic near-infrared photoluminescence enables monitoring of both accumulation and degradation in vivo. Furthermore, in contrast to most optically active nanomaterials (carbon nanotubes, gold nanoparticles and quantum dots), LPSiNPs self-destruct in a mouse model into renally cleared components in a relatively short period of time with no evidence of toxicity. As a preliminary in vivo application, we demonstrate tumour imaging using dextran-coated LPSiNPs (D-LPSiNPs). These results demonstrate a new type of multifunctional nanostructure with a low-toxicity degradation pathway forinvivo applications. The in vivo use of nanomaterials as therapeutic and diagnostic agents is of intense interest owing to their unique properties such as large specific capacity for drug loading 2 , strong superparamagnetism 3 ,efficientphotoluminescence 1,5 ordistinctive Raman signatures 4 , among others. Materials with sizes in the range of 20200nm can avoid renal filtration, leading to prolonged resi
1,727 citations
TL;DR: In this paper, the structure of the porous layers that emit red light under photoexcitation was revealed, which constitutes direct evidence that highly porous silicon contains quantum-size crystalline structures responsible for the visible emission.
Abstract: LIGHT-emitting devices based on silicon would find many applications in both VLSI and display technologies, but silicon normally emits only extremely weak infrared photoluminescence because of its relatively small and indirect band gap1. The recent demonstration of very efficient and multicolour (red, orange, yellow and green) visible light emission from highly porous, electrochemically etched silicon2,3 has therefore generated much interest. On the basis of strong but indirect evidence, this phenomenon was initially attributed to quantum size effects within crystalline material2, but this interpretation has subsequently been extensively debated. Here we report results from a transmission electron microscopy study which reveals the structure of the porous layers that emit red light under photoexcitation. Our results constitute direct evidence that highly porous silicon contains quantum-size crystalline structures responsible for the visible emission. We show that arrays of linear quantum wires are present and obtain images of individual quantum wires of width <3 nm.
1,285 citations
TL;DR: The photoluminescence properties of porous silicon have attracted considerable research interest since their discovery in 1990 as discussed by the authors, which is due to excitonic recombination quantum confined in Si nanocrystals which remain after the partial electrochemical dissolution of silicon.
1,261 citations
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TL;DR: In this article, the properties of electrolyte-semiconductor barriers are described, with emphasis on germanium, and the use of these barriers in localizing electrolytic etching is discussed.
Abstract: Properties of electrolyte-semiconductor barriers are described, with emphasis on germanium. The use of these barriers in localizing electrolytic etching is discussed. Other localization techniques are mentioned. Electrolytes for etching germanium and silicon are given.
1,039 citations
TL;DR: It is found that a standard, widespread, chemical-preparation method for silicon, oxidation followed by an HF etch, results in a surface which from an electronic point of view is remarkably inactive, which has implications for the ultimate efficiency of silicon solar cells.
Abstract: We have found that a standard, widespread, chemical-preparation method for silicon, oxidation followed by an HF etch, results in a surface which from an electronic point of view is remarkably inactive. With preparation in this manner, the surface-recombination velocity on Si111g is only 0.25 cm/sec, which is the lowest value ever reported for any semiconductor. Multiple-internal-reflection infrared spectroscopy shows that the surface appears to be covered by covalent Si-H bonds, leaving virtually no surface dangling bonds to act as recombinatiuon centers. These results have implications for the ultimate efficiency of silicon solar cells.
910 citations
TL;DR: In this paper, multiple internal infrared reflection spectroscopy has been used to identify the chemical nature of chemically oxidized and subsequently HF stripped silicon surfaces, and these very inert surfaces are found to be almost completely covered by atomic hydrogen.
Abstract: Multiple internal infrared reflection spectroscopy has been used to identify the chemical nature of chemically oxidized and subsequently HF stripped silicon surfaces. These very inert surfaces are found to be almost completely covered by atomic hydrogen. Results using polarized radiation on both flat and stepped Si(111) and Si(100) surfaces reveal the presence of many chemisorption sites (hydrides) that indicate that the surfaces are microscopically rough, although locally ordered. In particular, the HF‐prepared Si(100) surface appears to have little in common with the smooth H‐saturated Si(100) surface prepared in ultrahigh vacuum.
588 citations
TL;DR: In this article, the authors measured hydrogen desorption from monohydride and dihydride species on crystalline-silicon surfaces using transmission Fourier-transform infrared (FTIR) spectroscopy.
Abstract: Hydrogen desorption kinetics from monohydride and dihydride species on crystalline-silicon surfaces were measured using transmission Fourier-transform infrared (FTIR) spectroscopy. The FTIR desorption measurements were performed in situ in an ultrahigh-vacuum chamber using high-surface-area porous-silicon samples. The kinetics for hydrogen desorption from the monohydride and dihydride species was monitored using the SiH stretch mode at 2102 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ and the ${\mathrm{SiH}}_{2}$ scissors mode at 910 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, respectively. Annealing studies revealed that hydrogen from the ${\mathrm{SiH}}_{2}$ species desorbed between 640 and 700 K, whereas hydrogen from the SiH species desorbed between 720 and 800 K. Isothermal studies revealed second-order hydrogen desorption kinetics for both the monohydride and dihydride surface species. Desorption activation barriers of 65 kcal/mol (2.82 eV) and 43 kcal/mol (1.86 eV) were measured for the monohydride and dihydride species, respectively. These desorption activation barriers yield upper limits of 84.6 kcal/mol (3.67 eV) and 73.6 kcal/mol (3.19 eV) for the Si-H chemical bond energies of the SiH and ${\mathrm{SiH}}_{2}$ surface species.
479 citations