| 1. |
- Afrasiabi, Roodabeh, et al.
(författare)
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Effect of microwave-assisted silanization on sensing properties of silicon nanoribbon FETs
- 2015
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Ingår i: Sensors and actuators. B, Chemical. - : Elsevier B.V.. - 0925-4005 .- 1873-3077. ; 209, s. 586-595
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Tidskriftsartikel (refereegranskat)abstract
- An important concern with using silicon nanoribbon field-effect transistors (SiNR FET) for ion-sensing is the pH-response of the gate oxide surface. Depending on the application of the FET sensor, this response has to be chemically manipulated. Thus in silicon oxide-gated pH-sensors with integrated sensor and reference FETS, a surface with high pH-sensitivity, compared to the bare gate oxide, is required in the sensor FETs (SEFET), whereas in the reference FETs (REFET) the surface has to be relatively pH-insensitive. In order to control the sensitivity and chemistry of the oxide surface of the nanoribbons, a silanization reagent with a functional group is often self-assembled on the SiNR surface. Choice of a silanization reaction that results in a self-assembled layer on a silicon oxide surface has been studied extensively over the past decades. However, the effect of various self-assembled layers such as monolayers or mixed layers on the electrical response of SiNR FETs in aqueous solution needs to be exploited further, especially for future integrated SEFET/REFET systems. In this work, we have performed a comprehensive study on 3-aminopropyltriethoxysilane (APTES) silanization of silicon oxide surfaces using microwave (MW) heating as a new biocompatible route to conventional methods. A set of complementary surface characterization techniques (ellipsometry, AFM and ATR-FTIR) was used to analyze the properties of the APTES layer deposited on the silicon surface. We have found that a uniform monolayer can be achieved within 10 min by heating the silanization solution to 75 °C using MW heating. Furthermore, electrical measurements suggest that little change in device performance is observed after exposure to MW irradiation. Real-time pH measurements indicate that a uniform APTES monolayer not only reduces the pH sensitivity of SiNR FET by passivating the surface silanol groups, but also makes the device less sensitive to cation concentration in the background electrolyte. Our silanization route proves promising for future chemical surface modification of on-chip REFETs.
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| 2. |
- Afrasiabi, Roodabeh, et al.
(författare)
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Integration of a droplet-based microfluidic system and silicon nanoribbon FET sensor
- 2016
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Ingår i: Micromachines. - : MDPI AG. - 2072-666X. ; 7:8
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Tidskriftsartikel (refereegranskat)abstract
- We present a novel microfluidic system that integrates droplet microfluidics with a silicon nanoribbon field-effect transistor (SiNR FET), and utilize this integrated system to sense differences in pH. The device allows for selective droplet transfer to a continuous water phase, actuated by dielectrophoresis, and subsequent detection of the pH level in the retrieved droplets by SiNR FETs on an electrical sensor chip. The integrated microfluidic system demonstrates a label-free detection method for droplet microfluidics, presenting an alternative to optical fluorescence detection. In this work, we were able to differentiate between droplet trains of one pH-unit difference. The pH-based detection method in our integrated system has the potential to be utilized in the detection of biochemical reactions that induce a pH-shift in the droplets.
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| 3. |
- Afrasiabi, Roodabeh
(författare)
-
Silicon Nanoribbon FET Sensors : Fabrication, Surface Modification and Microfluidic Integration
- 2016
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Over the past decade, the field of medical diagnostics has seen an incredible amount of research towards the integration of one-dimensional nanostructures such as carbon nanotubes, metallic and semiconducting nanowires and nanoribbons for a variety of bio-applications. Among the mentioned one-dimensional structures, silicon nanoribbon (SiNR) field-effect transistors (FET) as electro-chemical nanosensors hold particular promise for label-free, real-time and sensitive detection of biomolecules using affinity-based detection. In SiNR FET sensors, electrical transport is primarily along the nanoribbon axis in a thin sheet (< 30 nm) serving as the channel. High sensitivity is achieved because of the large surface-to-volume ratio which allows analytes to bind anywhere along the NR affecting the entire conductivity by their surface charge. Unfortunately, sensitivity without selectivity is still an ongoing issue and this thesis aims at addressing the detection challenges and further proposing effective developments, such as parallel and multiple detection through using individually functionalized SiNRs.We present here a comprehensive study on design, fabrication, operation and device performance parameters for the next generation of SiNR FET sensors towards multiplexed, label-free detection of biomolecules using an on-chip microfluidic layer which is based on a highly cross-linked epoxy. We first study the sensitivity of different NR dimensions followed by analysis of the drift and hysteresis effects. We have also addressed two types of gate oxides (namely SiO2 and Al2O3) which are commonly used in standard CMOS fabrication of ISFETs (Ion sensitive FET). Not only have we studied and compared the hysteresis and response-time effects in the mentioned two types of oxides but we have also suggested a new integrated on-chip reference nanoribbon/microfluidics combination to monitor the long-term drift in the SiNR FET nanosensors. Our results show that compared to Al2O3, silicon-oxide gated SiNR FET sensors show high hysteresis and slow-response which limit their performance only to background electrolytes with low ionic strength. Al2O3 on the other hand proves more promising as the gate-oxide of choice for use in nanosensors. We have also illustrated that the new integrated sensor NR/Reference NR can be utilized for real-time monitoring of the above studied sources of error during pH-sensing. Furthermore, we have introduced a new surface silanization (using 3-aminopropyltriethoxysilane) method utilizing microwave-assisted heating which compared to conventional heating, yields an amino-terminated monolayer with high surface coverage on the oxide surface of the nanoribbons. A highly uniform and dense monolayer not only reduces the pH sensitivity of the bare-silicon oxide surface in a physiological media but also allows for more receptors to be immobilized on the surface. Protocols for surface functionalization and biomolecule immobilization were evaluated using model systems. Selective spotting of receptor molecules can be used to achieve localized functionalization of individual SiNRs, opening up opportunities for multiplexed detection of analytes.Additionally, we present here a novel approach by integrating droplet-based microfluidics with the SiNR FET sensors. Using the new system we are able to successfully detect trains of droplets with various pH values. The integrated system enables a wide range of label-free biochemical and macromolecule sensing applications based on detection of biological events such as enzyme-substrate interactions within the droplets.
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| 4. |
- Cavallaro, Sara, et al.
(författare)
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Label-Free Surface Protein Profiling of Extracellular Vesicles by an Electrokinetic Sensor
- 2019
-
Ingår i: ACS Sensors. - : AMER CHEMICAL SOC. - 2379-3694. ; 4:5, s. 1399-1408
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Tidskriftsartikel (refereegranskat)abstract
- Small extracellular vesicles (sEVs) generated from the endolysosomal system, often referred to as exosomes, have attracted interest as a suitable biomarker for cancer diagnostics, as they carry valuable biological information and reflect their cells of origin. Herein, we propose a simple and inexpensive electrical method for label-free detection and profiling of sEVs in the size range of exosomes. The detection method is based on the electrokinetic principle, where the change in the streaming current is monitored as the surface markers of the sEVs interact with the affinity reagents immobilized on the inner surface of a silica microcapillary. As a proof-of-concept, we detected sEVs derived from the non-small-cell lung cancer (NSCLC) cell line H1975 for a set of representative surface markers, such as epidermal growth factor receptor (EGFR), CD9, and CD63. The detection sensitivity was estimated to be similar to 175000 sEVs, which represents a sensor surface coverage of only 0.04%. We further validated the ability of the sensor to measure the expression level of a membrane protein by using sEVs displaying artificially altered expressions of EGFR and CD63, which were derived from NSCLC and human embryonic kidney (HEK) 293T cells, respectively. The analysis revealed that the changes in EGFR and CD63 expressions in sEVs can be detected with a sensitivity in the order of 10% and 3%, respectively, of their parental cell expressions. The method can be easily parallelized and combined with existing microfluidic-based EV isolation technologies, allowing for rapid detection and monitoring of sEVs for cancer diagnosis.
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| 5. |
- Chulapakorn, Thawatchart, 1988-, et al.
(författare)
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Impact of H-uptake by forming gas annealing and ion implantation on photoluminescence of Si-nanoparticles
- 2018
-
Ingår i: Physica Status Solidi (a) applications and materials science. - : John Wiley & Sons. - 1862-6300 .- 1862-6319. ; 215:3
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Tidskriftsartikel (refereegranskat)abstract
- Silicon nanoparticles (SiNPs) are formed by implanting 70 keV Si+ into a SiO2-film and subsequent thermal annealing. SiNP samples are further annealed in forming gas. Another group of samples containing SiNP is implanted by 7.5 keV H+ and subsequently annealed in N2-atmosphere at 450 °C to reduce implantation damage. Nuclear reaction analysis (NRA) is employed to establish depth profiles of the H-concentration. Enhanced hydrogen concentrations are found close to the SiO2surface, with particularly high concentrations for the as-implanted SiO2. However, no detectable uptake of hydrogen is observed by NRA for samples treated by forming gas annealing (FGA). H-concentrations detected after H-implantation follow calculated implantation profiles. Photoluminescence (PL) spectroscopy is performed at room temperature to observe the SiNP PL. Whereas FGA is found to increase PL under certain conditions, i.e., annealing at high temperatures, increasing implantation fluence of H reduces the SiNP PL. Hydrogen implantation also introduces additional defect PL. After low-temperature annealing, the SiNP PL is found to improve, but the process is not found equivalently efficient as conventional FGA.
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| 6. |
- Chulapakorn, Thawatchart, 1988-, et al.
(författare)
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Influence of Swift Heavy Ion Irradiation on the Photoluminescence of Si-nanoparticles and Defects in SiO2
- 2017
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Ingår i: Nanotechnology. - : IOP PUBLISHING LTD. - 0957-4484 .- 1361-6528. ; 28:37
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Tidskriftsartikel (refereegranskat)abstract
- The influence of swift heavy ion (SHI) irradiation on the photoluminescence (PL) of silicon nanoparticles (SiNPs) and defects in SiO2-film is investigated. SiNPs were formed by implantation of 70 keV Si+ and subsequent thermal annealing to produce optically active SiNPs and to remove implantation-induced defects. Seven different ion species with energy between 3-36 MeV and fluence from 10(11)-10(14) cm(-2) were employed for irradiation of the implanted samples prior to the thermal annealing. Induced changes in defect and SiNP PL were characterized and correlated with the specific energy loss of the employed SHIs. We find that SHI irradiation, performed before the thermal annealing process, affects both defect and SiNP PL. The change of defect and SiNP PL due to SHI irradiation is found to show a threshold-like behaviour with respect to the electronic stopping power, where a decrease in defect PL and an anticorrelated increase in SiNP PL after the subsequent thermal annealing are observed for electronic stopping exceeding 3-5 keV nm(-1). PL intensities are also compared as a function of total energy deposition and nuclear energy loss. The observed effects can be explained by ion track formation as well as a different type of annealing mechanisms active for SHI irradiation compared to the thermal annealing.
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| 7. |
- Chulapakorn, Thawatchart, 1988-, et al.
(författare)
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Luminescence of silicon nanoparticles from oxygen implanted silicon
- 2018
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Ingår i: Materials Science in Semiconductor Processing. - : Elsevier. - 1369-8001 .- 1873-4081. ; 86, s. 18-22
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Tidskriftsartikel (refereegranskat)abstract
- Oxygen with a kinetic energy of 20 keV is implanted in a silicon wafer (100) at different fluences, followed by post-implantation thermal annealing (PIA) performed at temperatures ranging from 1000 to 1200 degrees C, in order to form luminescent silicon nanoparticles (SiNPs) and also to reduce the damage induced by the implantation. As a result of this procedure, a surface SiOx layer (with 0 < x < 2) with embedded crystalline Si nanoparticles has been created. The samples yield similar luminescence in terms of peak wavelength, lifetime, and absorption as recorded from SiNPs obtained by the more conventional method of implanting silicon into silicon dioxide. The oxygen implantation profile is characterized by elastic recoil detection (ERD) technique to obtain the excess concentration of Si in a presumed SiO2 environment. The physical structure of the implanted Si wafer is examined by grazing incidence X-ray diffraction (GIXRD). Photoluminescence (PL) techniques, including PL spectroscopy, time-resolved PL (TRPL), and photoluminescence excitation (PLE) spectroscopy are carried out in order to identify the PL origin. The results show that luminescent SiNPs are formed in a Si sample implanted by oxygen with a fluence of 2 x 10(17) atoms cm(-2) and PIA at 1000 degrees C. These SiNPs have a broad size range of 6-24 nm, as evaluated from the GIXRD result. Samples implanted at a lower fluence and/or annealed at higher temperature show only weak defect-related PL. With further optimization of the SiNP luminescence, the method may offer a simple route for integration of luminescent Si in mainstream semiconductor fabrication.
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| 8. |
- Chulapakorn, Thawatchart, 1988-, et al.
(författare)
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MeV ion irradiation effects on the luminescence properties of Si-implanted SiO2-thin films
- 2016
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Ingår i: Physica Status Solidi (C) Current Topics in Solid State Physics. - : Wiley-VCH Verlagsgesellschaft. - 1862-6351 .- 1610-1634 .- 1610-1642. ; 13:10-12, s. 921-926
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Tidskriftsartikel (refereegranskat)abstract
- The effects of MeV heavy ion irradiation at varying fluence and flux on excess Si, introduced in SiO2 by keV ion implantation, are investigated by photoluminescence (PL). From the PL peak wavelength (λ) and decay lifetime (τ), two PL sources are distinguished: i) quasi-direct recombination of excitons of Si-nanoparticles (SiNPs), appearing after thermal annealing (λ > 720 nm, τ ∼ μs), and ii) fast-decay PL, possibly due to oxide-related defects (λ ∼ 575-690 nm, τ ∼ ns). The fast-decay PL (ii) observed before and after ion irradiation is induced by ion implantation. It is found that this fast-decay luminescence decreases for higher irradiation fluence of MeV heavy ions. After thermal annealing (forming SiNPs), the SiNP PL is reduced for samples irradiated by MeV heavy ions but found to stabilize at higher level for higher irradiation flux; the (ii) band vanishes as a result of annealing. The results are discussed in terms of the influence of electronic and nuclear stopping powers.
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| 9. |
- Chulapakorn, Thawatchart, 1988-, et al.
(författare)
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Si-nanoparticle synthesis using ion implantation and MeV ion irradiation
- 2015
-
Ingår i: Physica Status Solidi (C) Current Topics in Solid State Physics. - : Wiley-VCH Verlagsgesellschaft. - 1862-6351.
-
Tidskriftsartikel (refereegranskat)abstract
- A dielectric matrix with embedded Si-nanoparticles may show strong luminescence depending on nanoparticles size, surface properties, Si-excess concentration and matrix type. Ion implantation of Si ions with energies of a few tens to hundreds of keV in a SiO2 matrix followed by thermal annealing was identified as a powerful method to form such nanoparticles. The aim of the present work is to optimize the synthesis of Si-nanoparticles produced by ion implantation in SiO2 by employing MeV ion irradiation as an additional annealing process. The luminescence properties are measured by spectrally resolved photoluminescence including PL lifetime measurement, while X-ray reflectometry, atomic force microscopy and ion beam analysis are used to characterize the nanoparticle formation process. The results show that the samples implanted at 20%-Si excess atomic concentration display the highest luminescence and that irradiation of 36 MeV 127I ions affects the luminosity in terms of wavelength and intensity. It is also demonstrated that the nanoparticle luminescence lifetime decreases as a function of irradiation fluence.
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| 10. |
- Dev, Apurba, et al.
(författare)
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Electrokinetic effect for molecular recognition : A label-free approach for real-time biosensing
- 2016
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Ingår i: Biosensors & bioelectronics. - : Elsevier. - 0956-5663 .- 1873-4235. ; 82, s. 55-63
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Tidskriftsartikel (refereegranskat)abstract
- We present a simple and inexpensive method for label-free detection of biomolecules. The method monitors the changes in streaming current in a fused silica capillary as target biomolecules bind to immobilized receptors on the inner surface of the capillary. To validate the concept, we show detection and time response of different protein-ligand and protein-protein systems: biotin-avidin and biotin-streptavidin, barstar-dibarnase and Z domain-immunoglobulin G (IgG). We show that specific binding of these biomolecules can be reliably monitored using a very simple setup. Using sequential injections of various proteins at a diverse concentration range and as well as diluted human serum we further investigate the capacity of the proposed technique to perform specific target detection from a complex sample. We also investigate the time for the signal to reach equilibrium and its dependence on analyte concentration and demonstrate that the current setup can be used to detect biomolecules at a concentration as low as 100 pM without requiring any advanced device fabrication procedures. Finally, an analytical model based on diffusion theory has been presented to explain the dependence of the saturation time on the analyte concentration and capillary dimensions and how reducing length and inner diameter of the capillary is predicted to give faster detection and in practice also lower limit of detection.
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| 11. |
- Horak, Josef, et al.
(författare)
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Recombinant Spider Silk as Mediator for One-Step, Chemical-Free Surface Biofunctionalization
- 2018
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Ingår i: Advanced Functional Materials. - : Wiley. - 1616-301X .- 1616-3028. ; 28:21
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Tidskriftsartikel (refereegranskat)abstract
- A unique strategy for effective, versatile, and facile surface biofunctionalization employing a recombinant spider silk protein genetically functionalized with the antibody-binding Z domain (Z-4RepCT) is reported. It is demonstrated that Z-silk can be applied to a variety of materials and platform designs as a truly one-step and chemical-free surface modification that site specifically captures antibodies while simultaneously reducing nonspecific adsorption. As a model surface, SiO2 is used to optimize and characterize Z-silk performance compared to the Z domain immobilized by a standard silanization method. First, Z-silk adsorption is investigated and verified its biofunctionality in a long-term stability experiment. To assess the binding capacity and protein-protein interaction stability of Z-silk, the coating is used to capture human antibodies in various assay formats. An eightfold higher binding capacity and 40-fold lower detection limit are obtained in the immunofluorescence assay, and the complex stability of captured antibodies is shown to be improved by a factor of 20. Applicability of Z-silk to functionalize microfluidic devices is demonstrated by antibody detection in an electrokinetic microcapillary biosensor. To test Z-silk for biomarker applications, real-time detection and quantification of human immunoglobulin G are performed in a plasma sample and C1q capture from human serum using an anti-C1q antibody.
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| 12. |
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| 13. |
- Hormozan, Yashar, et al.
(författare)
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High-resolution x-ray imaging using a structured scintillator
- 2016
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Ingår i: Medical physics (Lancaster). - : American Association of Physicists in Medicine. - 0094-2405. ; 43:2, s. 696-701
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Tidskriftsartikel (refereegranskat)abstract
- Purpose: In this study, the authors introduce a new generation of finely structured scintillators with a very high spatial resolution (a few micrometers) compared to conventional scintillators, yet maintaining a thick absorbing layer for improved detectivity. Methods: Their concept is based on a 2D array of high aspect ratio pores which are fabricated by ICP etching, with spacings (pitches) of a few micrometers, on silicon and oxidation of the pore walls. The pores were subsequently filled by melting of powdered CsI(Tl), as the scintillating agent. In order to couple the secondary emitted photons of the back of the scintillator array to a CCD device, having a larger pixel size than the pore pitch, an open optical microscope with adjustable magnification was designed and implemented. By imaging a sharp edge, the authors were able to calculate the modulation transfer function (MTF) of this finely structured scintillator. Results: The x-ray images of individually resolved pores suggest that they have been almost uniformly filled, and the MTF measurements show the feasibility of a few microns spatial resolution imaging, as set by the scintillator pore size. Compared to existing techniques utilizing CsI needles as a structured scintillator, their results imply an almost sevenfold improvement in resolution. Finally, high resolution images, taken by their detector, are presented. Conclusions: The presented work successfully shows the functionality of their detector concept for high resolution imaging and further fabrication developments are most likely to result in higher quantum efficiencies.
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| 14. |
- Li, Yuanyuan, et al.
(författare)
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Luminescent Transparent Wood
- 2017
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Ingår i: Advanced Optical Materials. - : John Wiley & Sons. - 2195-1071. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- Luminescent transparent wood is prepared by combining the complementary properties of naturally grown anisotropic porous wood and luminescent quantum dots. The wood structure introduces strong diffused luminescence and waveguiding, which can potentially be exploited for optoelectronic and photovoltaic applications, such as for planar illumination sources and luminescent buildings/furniture. Images below show the transparency, haze, and luminescence of quantum dot wood.
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| 15. |
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| 16. |
- Liu, Lige, et al.
(författare)
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Photodegradation of Organometal Hybrid Perovskite Nanocrystals : Clarifying the Role of Oxygen by Single-Dot Photoluminescence
- 2019
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Ingår i: The Journal of Physical Chemistry Letters. - : AMER CHEMICAL SOC. - 1948-7185. ; 10:4, s. 864-869
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Tidskriftsartikel (refereegranskat)abstract
- Photostability has been a major issue for perovskite materials. Understanding the photodegradation mechanism and suppressing it are of central importance for applications. By investigating single-dot photoluminescence spectra and the lifetime of MAPbX(3) (MA = CH3NH3+, X = Br, I) nanocrystals with quantum confinement under different conditions, we identified two separate pathways in the photodegradation process. The first is the oxygen-assisted light-induced etching process (photochemistry). The second is the light-driven slow charge-trapping process (photophysics), taking place even in oxygen-free environment. We clarified the role of oxygen in the photodegradation process and show how the photoinduced etching can be successfully suppressed by OSTE polymer, preventing an oxygen-assisted reaction.
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| 17. |
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| 18. |
- Marinins, Aleksandrs, et al.
(författare)
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All-optical intensity modulation in polymer waveguides doped with si quantum dots
- 2018
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Ingår i: Optics InfoBase Conference Papers. - : Optical Society of America. - 9781557528209
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Konferensbidrag (refereegranskat)abstract
- We demonstrate all-optical intensity modulation in integrated PMMA optical waveguides doped with silicon quantum dots. The 1550 nm probe signal is absorbed by free carriers excited in silicon quantum dots with 405 nm pump light.
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| 19. |
- Marinins, Aleksandrs, et al.
(författare)
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Light Converting Polymer/Si Nanocrystal Composites with Stable 60-70% Quantum Efficiency and their Glass Laminates
- 2017
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 9:36, s. 30267-30272
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Tidskriftsartikel (refereegranskat)abstract
- Thiol-ene polymer/Si nanocrystal bulk hybrids were synthesized from alkyl-passivated Si nanocrystal (Si NC) toluene solutions. Radicals in the polymer provided a co-passivation of “dark” Si NCs, making them optically active and leading to a substantial ensemble quantum yield increase. Optical stability over several months was confirmed. The presented materials exhibit the highest photoluminescence quantum yield (~65%) of any solid-state Si NC hybrid reported to date. The broad tunability of thiol-ene polymer reactivity provides facile glass integration, as demonstrated by a laminated structure. This, together with extremely fast polymerization, makes the demonstrated hybrid material a promising candidate for light converting applications.
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| 20. |
- Marinins, Aleksandrs, et al.
(författare)
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Photostable Polymer/Si Nanocrystal Bulk Hybrids with Tunable Photoluminescence
- 2016
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Ingår i: ACS Photonics. - : American Chemical Society (ACS). - 2330-4022. ; 3:9, s. 1575-1580
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Tidskriftsartikel (refereegranskat)abstract
- Solid polymer/Si nanocrystal bulk nanocomposites were fabricated from solutions of alkene- and hydride-terminated silicon nanocrystals (NCs) in toluene. The photoluminescence peak position of hydride-terminated SiNCs before polymerization was tuned by photoassisted hydrofluoric acid etching. Optical properties of obtained PMMA/NC hybrids, such as quantum yield, luminescence lifetime, and dispersion factor, were evaluated over time. Photostability of these transparent bulk polymer/SiNC hybrids over months was confirmed. The emission covers the visible to near-infrared range with a quantum yield of similar to 30-40% for yellow-red nanocomposites.
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| 21. |
- Parmeggiani, Matteo, et al.
(författare)
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Electrokinetic-assisted gating in a microfluidic integrated Si nanoribbon ion sensor for enhanced sensitivity
- 2018
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Ingår i: Sensors and actuators. B, Chemical. - : Elsevier BV. - 0925-4005 .- 1873-3077. ; 262, s. 974-981
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Tidskriftsartikel (refereegranskat)abstract
- Using the electrokinetic principle, we demonstrate a novel approach to modulate the response of an ion sensitive silicon-nanoribbon field-effect-transistor, effectively manipulating the device sensitivity to a change in surface potential. By using the streaming potential effect we show that the changes in the surface potential induced by e.g. a pH change can be accurately manipulated in a microfluidic-integrated chip leading to an enhanced response. By varying the flow velocity and the biasing condition along the microfluidic channel, we further demonstrate that the pH response from such a device can also be suppressed or even reversed as a function of the flow velocity and the biasing configuration. Experiments performed with different pH buffer shows that the sensor response can be enhanced/suppressed by several times in magnitude simply by using the streaming potential effects. A mathematical description is also presented for qualitative assessment of the electrokinetic influence on the gate terminal under different biasing condition. The approach presented here shows the prospect to exploit the electrokinetic modulation for developing highly sensitive nanoscale biosensors.
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| 22. |
- Pevere, Federico, et al.
(författare)
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Biexciton Emission as a Probe of Auger Recombination in Individual Silicon Nanocrystals
- 2015
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 119:13, s. 7499-7505
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Tidskriftsartikel (refereegranskat)abstract
- Biexciton emission from individual silicon nanocrystals was detected at room temperature by time-resolved, single-particle luminescence measurements. The efficiency of this process, however, was found to be very low, about 10-20 times less than the single exciton emission efficiency. It decreases even further at low temperature, explaining the lack of biexciton emission line observations in silicon nanocrystal single-dot spectroscopy under high excitation. The poor efficiency of the biexciton emission is attributed to the dominant nonradiative Auger process. Corresponding measured biexciton decay times then represent Auger lifetimes, and the values obtained here, from tens to hundreds of nanoseconds, reveal strong dot-to-dot variations, while the range compares well with recent calculations taking into account the resonant nature of the Auger process in semiconductor nanocrystals.
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| 23. |
- Pevere, Federico, et al.
(författare)
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Effect of X-ray irradiation on the blinking of single silicon nanocrystals
- 2015
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Ingår i: Physica Status Solidi (a) applications and materials science. - : Wiley-VCH Verlagsgesellschaft. - 1862-6300 .- 1862-6319. ; 212:12
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Tidskriftsartikel (refereegranskat)abstract
- Photoluminescence (PL) intermittency (blinking) observed for single silicon nanocrystals (Si-NCs) embedded in oxide is usually attributed to trapping/de-trapping of carriers in the vicinity of the NC. Following this model, we propose that blinking could be modified by introducing new trap sites, for example, via X-rays. In this work, we present a study of the effect of X-ray irradiation (up to 65 kGy in SiO) on the blinking of single Si-NCs embedded in oxide nanowalls. We show that the luminescence characteristics, such as spectrum and life-time, are unaffected by X-rays. However, substantial changes in ON-state PL intensity, switching frequency, and duty cycle emerge from the blinking traces, while the ON- and OFF- time distributions remain of mono-exponential character. Although we do not observe a clear monotonic dependence of the blinking parameters on the absorbed dose, our study suggests that, in the future, Si-NCs could be blinking-engineered via X-ray irradiation.
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| 24. |
- Pevere, Federico
(författare)
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Optical Properties of Single Silicon Quantum Dots
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- For over 60 years silicon (Si) has dominated the semiconductor microelectronics industry mainly due to its abundance and good electrical and material properties. The advanced processing technology of Si has made it the workhorse for photovoltaics industry as well. However, this material has also a big drawback: it is an indirect-bandgap semiconductor in its bulk form, hence an inefficient light emitter. This has hindered the silicon photonics revolution envisioned in 1980s, where photons were thought to replace electrons inside computer chips.In parallel with the exponential scaling of Si transistor's size over the years, the discovery of quantum phenomena at the nanoscale raised new hopes for this semiconductor. In the 1990s bright luminescence from nanostructured porous Si was demonstrated claiming the quantum confinement effect as origin of the emission. Since then, an intense research activity has been focused on Si quantum dots (Si-QDs) due to their potential use as abundant and non-toxic light emitters. More precisely, they could be used as fluorescent biolabels in biomedicine, as light-emitting phosphors in e.g. TV screens or as down-converters in luminescent solar concentrators. Nevertheless, in order to realize such applications, it is necessary not only to improve the fabrication of Si-QDs but also to gain a better understanding of their photo-physics. Among different types of optical measurements, those performed at the single-dot level are free of sample inhomogeneities, hence more accurate for a correct physical description.This doctoral thesis presents a study of the optical properties of single Si-QDs of different type: encapsulated in an oxide matrix, capped with ligands or covered by a thin passivation layer. The homogeneous photoluminescence (PL) linewidth is found to strongly depend on the type of embedding matrix, being narrower for less rigid ones. A record resolution-limited linewidth of ~200 μeV is measured at low temperatures whereas room-temperature values can even compete with direct-bandgap QDs like CdSe. Such narrow PL lines exhibit intensity saturation at high excitation fluxes without any indication of emission from multiexciton states, suggesting the presence of fast non-radiative Auger recombination. Characteristic Auger-related lifetimes extracted from power-dependent decays show a variation from dot-to-dot and confirm the low biexciton quantum efficiency.For the first time, the absorption curve of single Si-QDs is probed by means of photoluminescence excitation in the range 2.0-3.5 eV. A step-like structure is found which depends on the nanocrystal shape considered and agrees well with simulations of the exciton level structure. Rod-like Si-QDs can exhibit ~50 times higher absorption than spherical-like ones due to local field effects and enhanced optical transitions. In contrast with previous studies, evidence of a direct-bandgap red-shift for small Si-QDs is missing at the single dot level, in agreement with atomistic calculations.Low-temperature PL decay measurements reveal no triplet-like emission lines, but two ~μs decay constants appearing at low temperatures. They suggest presence of a temperature-dependent fast blinking process based on trapping/detrapping of carriers in the oxide matrix, leading to delayed emission. The proposed model allows to extract characteristic trapping/de-trapping rates for Si-QDs featuring mono-exponential blinking statistics. From PL saturation curves, ligand-passivated Si-QDs do not exhibit such detrimental phenomenon, in agreement with the proposed model.Last, Si-QDs demonstrate to be very hard against ~10 keV X-ray radiation, in contrast with CdSe-QDs whose PL quenching is correlated with a change in the blinking parameters. This property could be exploited for example in space applications, where radiation-hard materials are required.To conclude, the results achieved in this thesis will help to understand and engineer the properties of Si-QDs whose application potential has increased after several years of research both at the ensemble and at the single-dot level.
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- Pevere, Federico, et al.
(författare)
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Rapid Trapping as the Origin of Nonradiative Recombination in Semiconductor Nanocrystals
- 2018
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Ingår i: ACS Photonics. - : American Chemical Society (ACS). - 2330-4022. ; 5:8, s. 2990-2996
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Tidskriftsartikel (refereegranskat)abstract
- We demonstrate that nonradiative recombination in semiconductor nanocrystals can be described by a rapid luminescence intermittency, based on carrier tunneling to resonant traps. Such process, we call it "rapid trapping (blinking)", leads to delayed luminescence and promotes Auger recombination, thus lowering the quantum efficiency. To prove our model, we probed oxide- (containing static traps) and ligand- (trap-free) passivated silicon nanocrystals emitting at similar energies and featuring monoexponential blinking statistics. This allowed us to find analytical formulas and to extract characteristic trapping/detrapping rates, and quantum efficiency as a function of temperature and excitation power. Experimental single-dot temperature-dependent decays, supporting the presence of one or few resonant static traps, and ensemble saturation curves were found to be very well described by this effect. The model can be generalized to other semiconductor nanocrystals, although the exact interplay of trapping/detrapping, radiative, and Auger processes may be different, considering the typical times of the processes involved.
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