Room Temperature Solution Synthesis of Alkyl-Capped Tetrahedral Shaped Silicon Nanocrystals

Baldwin, Richard K.; Pettigrew, Katherine A.; Garno, Jayne C.; Power, Phillip P.; Liu, Gang-yu; Kauzlarich, Susan M.

doi:10.1021/ja017170b

Cited by 186 publications

(148 citation statements)

References 19 publications

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“…Solution chemistry routes are attractive because particle size and surface chemistry can be controlled simultaneously. These strategies include sonochemical reduction of Si(OEt) 4 , reduction of SiCl 4 using Zintl salts [14], and other reductive routes [15][16][17][18][19].…”

Section: Introductionmentioning

confidence: 99%

A new solution route to hydrogen-terminated silicon nanoparticles: synthesis, functionalization and water stability

et al. 2007

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Hydrogen capped silicon nanoparticles with strong blue photoluminescence were synthesized by the metathesis reaction of sodium silicide, NaSi, with NH 4 Br. The hydrogen capped Si nanoparticles were further terminated with octyl groups and then coated with a polymer to render them water soluble. The nanoparticles were characterized by TEM, FT-IR, UV-VIS absorption, and photoluminescence. The Si nanoparticles were shown to have an average diameter of 3.9 ±1.3 nm and exhibited room-temperature photoluminescence with a peak maximum at 438 nm with a quantum efficiency of 32% in hexane and 18% in water; the emission was stable in ambient air for up to 2 months. These nanoparticles could hold great potential as a non-heavy element containing quantum dot for applications in biology.

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Section: Introductionmentioning

confidence: 99%

A new solution route to hydrogen-terminated silicon nanoparticles: synthesis, functionalization and water stability

et al. 2007

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“…Further development of this synthesis, using SiCl 4 as the only precursor, was initially reported by Kauzlarich and colleagues via Zintl salt metathesis [27][28][29] . Besides metathesis, other types of solution reactions were also used for Si nanocrystals via sodium naphthanide and hydride reagents 30,31 . However, unlike for Ge materials, solution synthesis of porous, crystalline Si materials has not yet been reported.…”

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confidence: 99%

Bottom-up synthesis of high surface area mesoporous crystalline silicon and evaluation of its hydrogen evolution performance

et al. 2014

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As an important material for many practical and research applications, porous silicon has attracted interest for decades. Conventional preparations suffer from high mass loss because of their etching nature. A few alternative routes have been reported, including magnesiothermic reduction; however, pre-formed porous precursors are still necessary, leading to complicated syntheses. Here we demonstrate a bottom-up synthesis of mesoporous crystalline silicon materials with high surface area and tunable primary particle/pore size via a self-templating pore formation process. The chemical synthesis utilizes salt by-products as internal self-forming templates that can be easily removed without any etchants. The advantages of these materials, such as their nanosized crystalline primary particles and high surface areas, enable increased photocatalytic hydrogen evolution rate and extended working life. These also make the mesoporous silicon a potential candidate for other applications, such as optoelectronics, drug delivery systems and even lithium-ion batteries.

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“…Recently, several groups, including ourselves, have prepared alkyl-passivated silicon nanocrystals. [5][6][7][8][9][10][11][12][13][14][15][16] These are SiNCs whose surface is capped by a monolayer of saturated hydrocarbon molecules and anchored to the Si core via covalent Si-C bonds. Although the particles contain a little oxide from their preparation, the alkyl monolayer protects the Si core and they are not oxidized further under ambient conditions.…”

mentioning

confidence: 99%

Optical luminescence from alkyl-passivated Si nanocrystals under vacuum ultraviolet excitation: Origin and temperature dependence of the blue and orange emissions

Chao

Houlton

Horrocks

et al. 2006

Applied Physics Letters

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The origin and stability of luminescence are critical issues for Si nanocrystals which are intended for use as biological probes. The optical luminescence of alkyl-monolayer-passivated silicon nanocrystals was studied under excitation with vacuum ultraviolet photons ͑5.1-23 eV͒. Blue and orange emission bands were observed simultaneously, but the blue band only appeared at low temperatures ͑Ͻ175 K͒ and with high excitation energies ͑Ͼ8.7 eV͒. At 8 K, the peak wavelengths of the emission bands were 430± 2 nm ͑blue͒ and 600± 2 nm ͑orange͒. The orange and blue emissions originate from unoxidized and oxidized Si atoms, respectively. © 2006 American Institute of Physics. ͓DOI: 10.1063/1.2216911͔Silicon nanostructures have attracted great interest since the observation of their efficient visible photoluminescence at room temperature in the early 1990s. 1-4 Silicon nanocrystals ͑SiNCs͒ are potential building blocks of future electronic and photonic devices. They also have promise as luminescent labels in biological applications, 5-9 because they show red-orange luminescence at small particle sizes ͑ca. 2 nm diam͒ and are not expected to show some aspects of the toxicity of cadmium-based semiconductors. However, the stability of SiNCs towards O 2 and H 2 O is a concern. Recently, several groups, including ourselves, have prepared alkyl-passivated silicon nanocrystals. [5][6][7][8][9][10][11][12][13][14][15][16] These are SiNCs whose surface is capped by a monolayer of saturated hydrocarbon molecules and anchored to the Si core via covalent Si-C bonds. Although the particles contain a little oxide from their preparation, the alkyl monolayer protects the Si core and they are not oxidized further under ambient conditions. 6 The reaction used to prepare the capping monolayer is sufficiently general to allow manipulation of the chemical functionality on the particle surface, e.g., for synthesis of DNA strands. 6 However, it is also important to characterize the physical properties, especially the luminescence, of these systems because the utility of the particles depends on their luminescence upon insertion into biological cells.Compared to the generally weak IR luminescence of bulk silicon ͑observed at low temperatures͒, the efficiency of photoluminescence ͑PL͒ from Si nanostructures is strongly increased due to the greater overlap of the electron and hole wave functions and the decrease in efficiency of nonradiative pathways. 17,18 A few electronic structure calculations on alkylated SiNCs have been made using density functional methods: these calculations include Si 29 clusters passivated with CH 3 or CH 2 ͑Ref. 19͒ and, more recently, alkyl monolayers up to C 4 H 9 on cluster sizes from Si 20 to Si 142 . 20 Theoretical work suggests that the band gap of SiNCs is little changed upon alkylation of the hydrogen-terminated particle surface, but the positions of the band edges are shifted significantly towards the vacuum level and the properties of the excited states are affected. 20 Experimental studies of the PL mechanism o...

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Room Temperature Solution Synthesis of Alkyl-Capped Tetrahedral Shaped Silicon Nanocrystals

Cited by 186 publications

References 19 publications

A new solution route to hydrogen-terminated silicon nanoparticles: synthesis, functionalization and water stability

A new solution route to hydrogen-terminated silicon nanoparticles: synthesis, functionalization and water stability

Bottom-up synthesis of high surface area mesoporous crystalline silicon and evaluation of its hydrogen evolution performance

Optical luminescence from alkyl-passivated Si nanocrystals under vacuum ultraviolet excitation: Origin and temperature dependence of the blue and orange emissions

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