Aqueous red-emitting silicon nanoparticles for cellular imaging: Consequences of protecting against surface passivation by hydroxide and water for stable red emission

Chiu, Shen; Manhat, Beth A.; DeBenedetti, William J. I.; Brown, Anna L.; Fichter, Katye M.; Vu, Tania Q.; Eastman, Micah; Jiao, Jun; Goforth, Andrea M.

doi:10.1557/jmr.2012.377

Cited by 18 publications

(33 citation statements)

References 74 publications

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“…[10][11][12][13]44 Difficulties involved with integration of nanocrystalline Si into commercial devices arise in stabilizing the PL intensity and energy in aqueous or aerobic environments. 23,41,45 Changes in the PL of nanocrystalline Si over time, presumably alongside alterations in the surface chemistry or size of the particles, have been reported consistently across the literature. 23,30,46 However, the promise of robust, inorganic fluorophores with size-dependent optical properties continues to motivate researchers to develop strategies to mitigate the changing PL energy and intensity.…”

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 69%

“…23,41,45 Changes in the PL of nanocrystalline Si over time, presumably alongside alterations in the surface chemistry or size of the particles, have been reported consistently across the literature. 23,30,46 However, the promise of robust, inorganic fluorophores with size-dependent optical properties continues to motivate researchers to develop strategies to mitigate the changing PL energy and intensity. bandgap to occur, they must be coupled with phonons (i.e., lattice vibrations), which have enough momentum to elicit the transition.…”

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 69%

“…Since that first report of visible PL from nanoscale Si domains, the field of Si nanomaterials has grown exponentially and now includes studies of ultra-small, colloidal Si nanoparticles (Si NPs) in variety of applications. Solid-, [20][21][22][23] solution-, [24][25][26][27][28][29] and gas-phase [30][31][32][33] reductions of Si precursors are methods currently used to synthesize Si NPs. Extensive descriptions of the synthesis methodologies published to date have been reviewed elsewhere.…”

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 99%

“…[36][37][38][39] In addition, Si NPs have been envisioned as replacements for traditional organic dyes in a variety of sensing and tracking applications owing to their strong visible PL and superior resistance to photobleaching and photodegredation. 22,23,[40][41][42] For biomedical imaging and sensing applications, red-to-NIR-fluorescence is desired, since these wavelengths penetrate tissue, and do not damage cells. While the number of red-to-NIR-emitting molecular organic dyes is limited (e.g., to…”

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 99%

“…21,23,43 Another intended application for emissive Si NPs is in optoelectronic devices. Currently, modern optoelectronic devices use III-V semiconductor nanoparticles as the light-emitting diodes, which are then interfaced to the electronic silicon-based circuitry.…”

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 99%

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Investigation into Effects of Instability and Reactivity of Hydride-Passivated Silicon Nanoparticles on Interband Photoluminescence

Radlinger¹

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While silicon has long been utilized for its electronic properties, its use as an optical material has largely been limited due to the poor efficiency of interband transitions. However, discovery of visible photoluminescence (PL) from nanocrystalline silicon in 1990 triggered many ensuing research efforts to optimize PL from nanocrystalline silicon for optical applications. Currently, use of photoluminescent silicon nanoparticles (Si NPs) is commercially limited by: 1) the instability of the energy and intensity of the PL, and 2) the low quantum yield of interband PL from Si NPs.Herein, red-emitting, hydrogen-passivated silicon nanoparticles (H-Si NPs) were synthesized by thermally-induced disproportionation of a HSiCl 3 -derived (HSiO 1.5 )n polymer. The H-Si NPs produced by this method were then subjected to various chemical and physical environments to assess the long-term stability of the optical properties as a function of changing surface composition. This dissertation is intended to elucidate correlations between the reported PL instability and the observed changes in the Si NP surface chemistry over time and as a function of environment.First, the stability of the H-Si NP surface at slightly elevated temperatures towards reactivity with a simple alkane was probed. The H-Si NPs were observed by FT-IR spectroscopy to undergo partial hydrosilylation upon heating in refluxing hexane, in addition to varying degrees of surface oxidation. The unexpected reactivity of the Si surface in n-hexane supports the unstable nature of the H-Si NP surface, and furthermore implicates the presence of highly-reactive Si radicals on the surfaces of the Si NPs. We propose that reaction of alkene impurities with the Si surface radicals is largely responsible for the observed surface alkylation. However, we also present an alternate ii mechanism by which Si surface radicals could react with alkanes to result in alkylation of the surface.Next, the energy and intensity stability of the interband PL from H-Si NPs in the presence of a radical trap was probed. Upon addition of (2,2,6,6,-tetramethyl-piperidin-1-yl)oxyl (TEMPO), the energy and intensity of the interband transition was observed to change over time, dependent on the reaction conditions. First, when the reaction occurred at 4ºC with minimal light exposure, the interband transition exhibited a gradual hypsochromic shift to between 595 nm and 655 nm, versus the λ max of the original low energy emission peak at 700 nm, depending on the amount of TEMPO in the sample.Second, when the reaction proceeded at room temperature with frequent exposure to 360 nm irradiation, the original interband transition at 660 nm was quenched while a new peak at 575 nm developed. Based on all the data collected and analyzed, we assign the 595 -655 nm transition as due to interband exciton recombination from Si NPs with reduced diameters relative to the original Si NPs. We furthermore assign the 575 nm transition as due to an oxide-related defect state resulting from rapid oxidation of pho...

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Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 69%

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 69%

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 99%

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 99%

Section: Technological Developments Leading To Photoluminescent Siliconmentioning

confidence: 99%

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Investigation into Effects of Instability and Reactivity of Hydride-Passivated Silicon Nanoparticles on Interband Photoluminescence

Radlinger¹

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Unlocking the potential of carbon dots in agriculture using data-driven approaches

Li,

Kah

et al. 2024

Science of The Total Environment

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Simple Preparation of Fluorescent Silicon Nanoparticles from Used Si Wafers

Hwang

Jeong

Lee

et al. 2015

Ind. Eng. Chem. Res.

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A simple way of preparing fluorescent silicon nanoparticles (SiNPs) with a mean diameter of ∼5 nm was demonstrated from used silicon wafers. Anodic etching of used wafers performed in a customized electrochemical cell produced H-terminated, nano- and micropores on the wafer surface, and SiNPs were attained by mechanically crumbling the nano-/microporous Si surface structures on the etched wafers in an ultrasonic bath. The obtained SiNPs were then re-etched in different ratios of HF/HNO3 acid mixture to produce different PL intensities, sizes, and yields. When the particle sizes were decreased by adjusting the experimental conditions (e.g., strength of the acid mixture, reaction time), the PL spectra from etched SiNPs were also shifted from red to blue, indicating the quantum confinement effect from the nanoparticles. Typically, blue-emitting SiNPs were observed with an average diameter of 2.7 nm and a yield of 0.3 mg/cm2 of used wafers. Re-etched SiNPs were dialyzed by a 1K-dialysis membrane for purification and for potential use in bioapplications. The efficient method of preparing fluorescent nanoparticles from used monocrystalline Si wafers was demonstrated with a high production yield. The produced particles showed outstanding physical and chemical properties, indicating the applicability of these materials in semiconductor research and bioapplications.

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Aqueous red-emitting silicon nanoparticles for cellular imaging: Consequences of protecting against surface passivation by hydroxide and water for stable red emission

Abstract: Abstract

Cited by 18 publications

References 74 publications

Investigation into Effects of Instability and Reactivity of Hydride-Passivated Silicon Nanoparticles on Interband Photoluminescence

Investigation into Effects of Instability and Reactivity of Hydride-Passivated Silicon Nanoparticles on Interband Photoluminescence

Unlocking the potential of carbon dots in agriculture using data-driven approaches

Simple Preparation of Fluorescent Silicon Nanoparticles from Used Si Wafers

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