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This Letter introduces a novel, to the best of our knowledge, approach to estimate the power conversion efficiency (PCE) of a square luminescent solar concentrator (LSC) by point excitations on the "optical centers." Predicted by theoretical calculations, photoluminescence emissions from these optical centers experience almost the same average optical path as those from the whole device under uniform illumination. This is experimentally verified by a 20 × 20 cm

Fluorescent probes are vital to cell imaging by allowing specific parts of cells to be visualized and quantified. Color-switchable probes (CSPs), with tunable emission wavelength upon contact with specific targets, are particularly powerful because they not only eliminate the need to wash away all unbound probe but also allow for internal controls of probe concentrations, thereby facilitating quantification. Several such CSPs exist and have proven very useful, but not for all key cellular targets. Here we report a pioneering CSP for in situ cell imaging using aldehydefunctionalized silicon nanocrystals (SiNCs) that switch their intrinsic photoluminescence from red to blue quickly when interacting with amino acids in live cells. Though conventional probes often work better in cell-free extracts than in live cells, the SiNCs display the opposite behavior and function well and fast in universal cell lines at 37 ? while requiring much higher temperature in extracts. Furthermore, the SiNCs only disperse in cytoplasm not nucleus, and their fluorescence intensity correlated linearly with the concentration of fed amino acids. We believe these nanosilicon probes will be promising tools to visualize distribution of amino acids and potentially quantify amino acid related processes in live cells.

The optical response of hierarchical materials is convoluted, which hinders their direct study and property control. Transparent wood (TW) is an emerging biocomposite in this category, which adds optical function to the structural properties of wood. Nano- and microscale inhomogeneities in composition, structure and at interfaces strongly affect light transmission and haze. While interface manipulation can tailor TW properties, the realization of optically clear wood requires detailed understanding of light-TW interaction mechanisms. Here we show how material scattering and absorption coefficients can be extracted from a combination of experimental spectroscopic measurements and a photon diffusion model. Contributions from different length scales can thus be deciphered and quantified. It is shown that forward scattering dominates haze in TW, primarily caused by refractive index mismatch between the wood substrate and the polymer phase. Rayleigh scattering from the wood cell wall and absorption from residual lignin have minor effects on transmittance, but the former affects haze. Results provide guidance for material design of transparent hierarchical composites towards desired optical functionality; we demonstrate experimentally how transmittance and haze of TW can be controlled over a broad range. QC 20220125

A concept of transparent “quantum dot glass”(TQDG) is proposed for a combination of a quantum dot(QD)-based glass luminescent solar concentrator (LSC) and itsedge-attached solar cells, as a type of transparent photovoltaics(TPVs) for building-integrated photovoltaics (BIPVs). Differentfrom conventional LSCs, which typically serve as pure opticaldevices, TQDGs have to fulfill requirements as both powergeneratingcomponents and building construction materials. In thiswork, we demonstrate large-area (400 cm2) TQDGs based onsilicon QDs in a triplex glass configuration. An overall powerconversion efficiency (PCE) of 1.57% was obtained with back-reflection for a transparent TQDG (average visible transmittance of84% with a color rendering index of 88 and a low haze ≤3%), contributing to a light utilization efficiency (LUE) of 1.3%, which isamong the top reported TPVs based on the LSC technology with similar size. Most importantly, these TQDGs are shown to havebetter thermal and sound insulation properties compared to normal float glass, as well as improved mechanical performance andsafety, which significantly pushes the TPV technology toward practical building integration. TQDGs simultaneously exhibit favorablephotovoltaic, aesthetic, and building envelope characteristics and can serve as a multifunctional material for the realization of nearlyzero-energy building concepts. QC 20220906

Here we present a one-step synthesis that provides silicon nanocrystals with a thin shell composed of a ceramic-like carbonyl based compound, embedded in a porous organosilicon film. The silicon nanocrystals were synthesised from hydrogen silsesquioxane molecules, modified with organic molecules containing carbonyl groups, which were annealed at 1000 °C in a slightly reducing 5% H2 : 95% Ar atmosphere. The organic character of the shell was preserved after annealing due to trapping of organic molecules inside the HSQ-derived oxide matrix that forms during the annealing. The individual silicon nanocrystals, studied by single dot spectroscopy, exhibited a significantly narrower emission peak at room temperature (lowest linewidth ∼ 17 meV) compared to silicon nanocrystals embedded in a silicon oxide shell (150 meV). Their emission linewidths are even significantly narrower than those of single CdSe quantum dots (>50 meV). It is hypothesized that the Si-core–thin shell structure of the nanoparticle is responsible for the unique optical properties. Its formation within one synthesis step opens new opportunities for silicon-based quantum dots. The luminescence from the produced nanocrystals covers a broad spectral range from 530–720 nm (1.7–2.3 eV) suggesting strong application potential for solar cells and LEDs, following the development of a suitable mass-fabrication protocol.

We develop an empirical tight binding approach for the modeling of the electronic states and optical properties of Si nanocrystals embedded in a SiO2 matrix. To simulate the wide band gap SiO2 matrix we use the virtual crystal approximation. The tight-binding parameters of the material with the diamond crystal lattice are fitted to the band structure of β-cristobalite. This model of the SiO2 matrix allows us to reproduce the band structure of real Si nanocrystals embedded in a SiO2 matrix. In this model, we compute the absorption spectra of the system. The calculations are in an excellent agreement with experimental data. We find that an important part of the high-energy absorption is defined by the spatially indirect, but direct in k-space transitions between holes inside the nanocrystal and electrons in the matrix.

As a cost-effective batch synthesis method, Si quantum dots (QDs) with nearinfrared photoluminescence, high quantum yield (>50% in polymer nanocomposite), and nearunity internal quantum efficiency were fabricated from an inexpensive commercial precursor (triethoxysilane, TES), using optimized annealing and etching processes. The optical properties of such QDs are similar to those prepared from state-of-the-art precursors (hydrogen silsesquioxane, HSQ) yet featuring an order of magnitude lower cost. To understand the effect of synthesis parameters on QD optical properties, we conducted a thorough comparison study between common solid precursors: TES, HSQ, and silicon monoxide (SiO), including chemical, structural, and optical characterizations. We found that the structural nonuniformity and abundance of oxide inherent to SiO limited the resultant QD performance, while for TES-derived QDs this drawback can be avoided. The presented low-cost synthetic approach would significantly favor applications requiring high loading of good-quality Si QDs, such as light conversion for photovoltaics. QC 20211103

A concept of transparent “Quantum Dot Glass” (TQDG) is proposed for a combination of quantum dot (QD) based glass luminescent solar concentrator (LSC) and its edge-attached solar cells, as a type of transparent photovoltaics (TPV) for building-integrated photovoltaics (BIPV). Different from conventional LSCs, which typically serve as pure optical devices, TQDGs have to fulfill requirements both as power-generating components and building envelop construction materials. In this work, we demonstrate large-area (400 cm2) TQDGs based on environmentally benign silicon QDs in a triplex glass configuration. Balanced photovoltaic performance and aesthetic quality of the TQDGs were achieved by optimization of Si QDs/polymer interlayer thickness and QD loading in the devices. As a result, an overall electrical power conversion efficiency (PCE) of 1.57% was obtained with back-reflection for a highly transparent TQDG (average visible transmittance of 84%, with color rendering index of 94 and low haze ≤ 3%), contributing to a high light utilization efficiency (LUE) of 1.3%, which is among the top of reported TPVs based on LSC technology with similar size. Most importantly, these TQDGs are shown to have better thermal and sound insulation property compared to normal float glass, as well as improved mechanical performance and safety, which significantly pushes the TPV technology towards practical building integration and construction. TQDGs simultaneously exhibiting favorable photovoltaic, aesthetic and building-envelope characteristics, can serve as a multifunctional material for the realization of nearly zero-energy building concept.

Refractive index (RI) determination for delignified wood templates is vital for transparent wood composite fabrication. Reported RIs in the literature are based on either single plant fibers or wood powder, measured by the immersion liquid method (ILM) combined with mathematical fitting. However, wood structure complexity and the physical background of the fitting were not considered. In this work, RIs of delignified wood templates were measured by the ILM combined with a light transmission model developed from the Fresnel reflection/refraction theory for composite materials. The RIs of delignified balsa wood are 1.536 ± 0.006 and 1.525 ± 0.008 at the wavelength of 589 nm for light propagating perpendicular and parallel to the wood fiber direction, respectively. For delignified birch wood, corresponding values are 1.537 ± 0.005 and 1.529 ± 0.006, respectively. The RI data for delignified wood scaffolds are important for tailoring optical properties of transparent wood biocomposites, and also vital in optical properties investigations by theoretical modelling of complex light propagation in transparent wood and related composites. The developed light transmission model in combination with the immersion liquid method can be used to determine the RI of complex porous or layered solid materials and composites.

Luminescence solar concentrators act as semitransparent photovoltaic cells of interest for modern urban environments. Here, their efficiencies were analytically derived for different regular unit shapes as simple, integral-free expressions. This allowed analysis of the shape and size effect on the device performance. All regular shapes appear to have a similar efficiency as revealed by optical path distribution formulas, despite differences in the perimeter length. Rectangles of the same area feature higher efficiency due to reduced average optical path. It comes with the cost of a longer perimeter, and the relation between these two is provided. An explicit formula for the critical size of an LSC unit, above which its inner part becomes inactive, has been obtained. For square geometry with matrix absorption coefficient

The treatment of time-resolved (TR) photoluminescence (PL) decay kinetics is analysed in details and illustrated by experiments on semiconductor quantum dots, namely silicon nanocrystals (Si NCs). ...

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 MAPbX3 (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.

For biomolecule sensing purposes a solid-state nanopore platform based on silicon has certain advantages as compared to nanopores on other substrates such as graphene, silicon nitride, silicon oxide etc Capitalizing on the developed CMOS technology, nanopores on silicon are scalable without any requirement for additional processing, the devices are low cost and the process can be repeatable with a high yield. One of the essential requirements in biomolecule sensing is the ability of the nanopore to interact with the analyte. In this work, we present a method for processing high aspect ratio, single nanopores in the range of 10-30 nm in diameter and approximately 700 nm in length on a silicon-on-insulator (SOI) wafer. The presented method of manufacturing the high aspect ratio individual nanopores combines optical lithography and anisotropic KOH etching with a final electrochemical etching step to form the nanopores and is repeatable and can be processed in batches. We demonstrate electrical detection of dsDNA translocation, where the characteristic time of the process is in the millisecond range. We also analyse the translocation parameters and correlate the enhanced length of the nanopore to a longer translocation time as compared to other substrates.

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 ...

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/detra...

Thiol-ene polymer/Si nanocrystal bulk hybrids were synthesized from alkyl-passivated Si nanocrystal (Si NC) toluene solutions. Radicals in the polymer provided a copassivation 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.

Luminescent solar concentrator (LSC) is a promising technology to integrate semitransparent photovoltaic (PV) systems into modern buildings and vehicles. Silicon quantum dots (QDs) are good candidates as fluorophores in LSCs, due to the absence of overlap between absorption and emission spectra, high photoluminescence quantum yield (PLQY), good stability, nontoxicity, and element abundance. Herein, LSCs based on Si QDs/polymer nanocomposites are fabricated in a triplex glass configuration. A special polymer matrix (off-stoichiometric thiol-ene, OSTE) is used, which improves Si nanocrystal quantum yield. Herein, a comprehensive investigation to improve the performance of LSCs by exploring different strategies under the guidance of a theoretical description is conducted. Among these strategies, the systematical enhancement of PLQY of the nanocomposite is achieved by tuning the thiol/allyl group ratio in the OSTE matrix. In addition, ligand selection and loading optimization for QDs reduce the total scattering loss in the device. Finally, an optical power efficiency of 7.9% is achieved for an optimized LSC prototype (9 x 9 x 0.6 cm(3), transmittance approximate to 62% at 500 nm) based on Si QDs/OSTE nanocomposite, which shows good potential of this material system in LSC fabrication. QC 20210119

The complex structure of halide and oxide perovskites strongly affects their physical properties. Here, the effect of dimensions reduced to the nanoscale has been investigated by a combination of single-dot optical experiments with a phase transition theory. Methylammonium lead bromide (CH

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 wavelengt ...

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 ∼30–40% for yellow-red nanocomposites.

Polymer materials offer process compatibility, design flexibility, and low cost technology as a multi-functional platform for optical communication and photonics applications. Design and thermal reflowing technology of low loss polymer waveguides, as well as demonstration of transparent wood laser are presented in this paper.

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 CCDdevice, 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-rayimages 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.

The aim of this study was to synthesise new luminescent small molecular weight benzo- and naphthoquinoline derivatives (based on already known synthons) with different substituents (chlorine, tetrazole, iminophosphorane and amine), to characterize them by ultraviolet photoelectron spectroscopy in air (UPS), luminescence and absorption photospectrometry and to investigate the changes in these properties resulted by differences of molecular structure. Measured values of the HOMO, the LUMO energy levels and optical band gap (Eg_opt) were in range E HOMO = [ − 5 , 9 ; − 5 , 5 ] eV , E LUMO = [ − 3 , 6 ; − 3 ] eV , E g _ opt = [ 2 ; 2 , 8 ] eV . Most of the examined materials showed high intensity fluorescence reaching quantum yields of 49%. Fluorescence peaks of thermally evaporated layers distributed in range of λLayer=[477; 596] nm – from blue to orange colour while in chloroform solution remained in blue-green interval λSolution=[471;537] nm. Primary study results of electroluminescence indicate that the materials have a potential to be used in organic optoelectronics.

Bulk silicon as an indirect bandgap semiconductor is a poor light emitter. In contrast, silicon nanocrystals (Si NCs) exhibit strong emission even at room temperature, discovered initially at 1990 for porous silicon by Leigh Canham. This can be explained by the indirect to quasi-direct bandgap modification of nano-sized silicon according to the already well-established model of quantum confinement.In the absence of deep understanding of numerous fundamental optical properties of Si NCs, it is essential to study their photoluminescence (PL) characteristics at the single-dot level. This thesis presents new experimental results on various photoluminescence mechanisms in single silicon quantum dots (Si QDs).The visible and near infrared emission of Si NCs are believed to originate from the band-to-band recombination of quantum confined excitons. However, the mechanism of such process is not well understood yet. Through time-resolved PL decay spectroscopy of well-separated single Si QDs, we first quantitatively established that the PL decay character varies from dot-to-dot and the individual lifetime dispersion results in the stretched exponential decays of ensembles. We then explained the possible origin of such variations by studying radiative and non-radiative decay channels in single Si QDs. For this aim the temperature dependence of the PL decay were studied. We further demonstrated a model based on resonance tunneling of the excited carriers to adjacent trap sites in single Si QDs which explains the well-known thermal quenching effect.Despite the long PL lifetime of Si NCs, which limits them for optoelectronics applications, they are ideal candidates for biomedical imaging, diagnostic purposes, and phosphorescence applications, due to the non-toxicity, biocompability and material abundance of silicon. Therefore, measuring quantum efficiency of Si NCs is of great importance, while a consistency in the reported values is still missing. By direct measurements of the optical absorption cross-section for single Si QDs, we estimated a more precise value of internal quantum efficiency (IQE) for single dots in the current study. Moreover, we verified IQE of ligand-passivated Si NCs to be close to 100%, due to the results obtained from spectrally-resolved PL decay studies. Thus, ligand-passivated silicon nanocrystals appear to differ substantially from oxide-encapsulated particles, where any value from 0 % to 100 % could be measured. Therefore, further investigation on passivation parameters is strongly suggested to optimize the efficiency of silicon nanocrystals systems.

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 ...

The role of surface species in the optical properties of silicon nanocrystals (SiNCs) is the subject of intense debate. Changes in photoluminescence (PL) energy following hydrosilylation of SiNCs with alkyl-terminated surfaces are most often ascribed to enhanced quantum confinement in the smaller cores of oxidized NCs or to oxygen-induced defect emission. We have investigated the PL properties of alkyl-functionalized SiNCs prepared using two related methods: thermal and photochemical hydrosilylation. Photochemically functionalized SiNCs exhibit higher emission energies than the thermally functionalized equivalent. While microsecond lifetime emission attributed to carrier recombination within the NC core was observed from all samples, much faster, size-independent nanosecond lifetime components were only observed in samples prepared using photochemical hydrosilylation that possessed substantial surface oxidation. In addition, photochemically modified SiNCs exhibit higher absolute photoluminescent quantum y...

Transparent wood (TW) is a biocomposite material with hierarchical structure, which exhibits high optical transmittance and anisotropic light scattering. Here, the relation between anisotropic scattering and the internal structure of transparent wood is experimentally studied and the dependence of scattering anisotropy on material thickness, which characterizes the fraction of ballistic photons in the propagating light, is shown. The limitations of the conven-tional haze, as it is implemented to isotropic materials, are discussed, and a modified characteristic parameter of light scattering—the degree of aniso-tropic scattering is defined. This parameter together with the transport mean free path value is more practical and convenient for characterization of the material scattering properties. It is believed that the generic routine described in this paper can be applied for scattering characterization and comparison of other TW materials of either different thickness, optical quality or based on various wood species. QC 20181126

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.

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.

The influence of swift heavy ion (SHI) irradiation on the photoluminescence (PL) of silicon nanoparticles (SiNPs) and defects in SiO

The luminescence linewidth of individual silicon nanocrystals was characterized by single-dot spectroscopy, and an ultranarrow linewidth of similar to 200 mu eV at 10 K was found. This value is, in fact, limited by system resolution and represents only the upper limit of the homogeneous linewidth. In addition, the effect of the matrix was investigated for nanocrystals coated with organic ligands, embedded in silicon dioxide, as well as for nanocrystals with only a thin passivating layer. It was found that, depending on the matrix, the room-temperature bandwidth may vary by an order of magnitude, where values as small as similar to 12 meV (similar to 5 nm) at 300 K were detected for nanocrystals with a thin passivation. The observed values for silicon nanocrystals are similar and even surpass some of those for direct-band-gap quantum dots. The narrow linewidth at room temperature enables the use of silicon nanocrystals for nontoxic narrow-band labeling of biomolecules and for application as phosphors in white-light-emitting devices. QC 20141114

We report two orders of magnitude stronger absorption in silicon nanorods relative to bulk in a wide energy range. The local field enhancement and dipole matrix element contributions were disentangled experimentally by single-dot absorption measurements on differently shaped particles as a function of excitation polarization and photon energy. Both factors substantially contribute to the observed effect as supported by simulations of the light-matter interaction and atomistic calculations of the transition matrix elements. The results indicate strong shape dependence of the quasidirect transitions in silicon nanocrystals, suggesting nanostructure shape engineering as an efficient tool for overcoming limitations of indirect band gap materials in optoelectronic applications, such as solar cells.

Epitaxial lateral overgrowth (ELOG) of GaInP on GaAs by hydride vapor phase epitaxy (HVPE) is carried out as a pre-study to obtain GaInP/Si heterointerface. We present first results on the growth of GaInP/Si by a modified ELOG technique, corrugated epitaxial lateral overgrowth (CELOG).

We study the effect of X-ray irradiation on the photoluminescence (PL) efficiency and intermittency (blinking) of single Si/SiO2 and CdSe/CdZnS quantum dots (QDs). Our results show that the PL efficiency of Si nanocrystals is not significantly altered up to a cumulative fluence of 10(20) photons/m(2) (corresponding to similar to 300 kGy of absorbed dose in SiO2), while CdSe particles become completely dark already after a 17 times lower fluence. In both types of QDs, the statistical nature of blinking ON- and OFF-times remains unaltered: mono-exponential for Si and power-law for CdSe QDs. However, the evolution of the blinking parameters with absorbed dose depends on the choice of material. On average, both ON- and OFF-time constants do not vary in Si nanocrystals, highlighting their radiation hardness. Instead, the ON-time exponent increases while the OFF-time exponent decreases with the increasing dose for CdSe dots, confirming their efficiency quenching. Ensemble measurements did not show PL spectral changes neither indicated removal of surface ligands in irradiated CdSe dots. Thus, ionization-generated non-radiative centers in the core-shell system modify blinking of CdSe dots and eventually rapidly quench their emission, in contrast to robust Si/SiO2 nanocrystals. Our study is important for the future use of luminescent QDs in harsh environments, such as space, and the engineering of their blinking properties via ionizing radiation. Credit for the Accepted Manuscript: AIP PublishingReference: Federico Pevere, Carl von Treskow, Emanuele Marino, Monib Anwar, Benjamin Bruhn, Ilya Sychugov and Jan Linnros, "X-ray radiation hardness and influence on blinking in Si and CdSe quantum dots," Applied Physics Letters, Volume 113, Issue 25, pp. 25310, Year 2018.QC 20190115

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.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.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.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.

Photoluminescence excitation measurements have been performed on single, unstrained oxide-embedded Si nanocrystals. Having overcome the challenge of detecting weak emission, we observe four broad peaks in the absorption curve above the optically emitting state. Atomistic calculations of the Si nanocrystal energy levels agree well with the experimental results and allow identification of some of the observed transitions. An analysis of their physical nature reveals that they largely retain the indirect band-gap structure of the bulk material with some intermixing of direct band- gap character at higher energies. QC 20160512

We apply Gans theory to fit the absorption spectra of gold nanorods with aspect ratios R ≤ 2.5 in solution using both the longitudinal and transversal surface plasmon resonance absorption peaks and the dielectric constant of the medium, em, as a fitting parameter. By fitting the broadened absorption peaks using the absorption spectra of a set of nanorods with a range of aspect ratios, we determine the size distribution of the nanorods in solution. The optimum value of em = 2.1 ± 0.1 is substantially higher than the dielectric constant of the solvent (em,water = 1.77), which is most likely due to a change in the effective dielectric constant in the vicinity of the nanorods. The validity of our method is confirmed by comparing the calculated size distributions with transmission electron microscope images, and we obtain a good agreement between the experiments and our calculations. Furthermore, several other recent experimental results are compared with our fitting method, and we find that the discrepancy be...

Optical nanopore sensing offers great potential in single-molecule detection, genotyping, or DNA sequencing for high-throughput applications. However, one of the bottle-necks for fluorophore-based biomolecule sensing is the lack of an optically optimized membrane with a large array of nanopores, which has large pore-to-pore distance, small variation in pore size and low background photoluminescence (PL). Here, we demonstrate parallel detection of single-fluorophore-labeled DNA strands (450 bps) translocating through an array of silicon nanopores that fulfills the above-mentioned requirements for optical sensing. The nanopore array was fabricated using electron beam lithography and anisotropic etching followed by electrochemical etching resulting in pore diameters down to ∼7 nm. The DNA translocation measurements were performed in a conventional wide-field microscope tailored for effective background PL control. The individual nanopore diameter was found to have a substantial effect on the translocation velocity, where smaller openings slow the translocation enough for the event to be clearly detectable in the fluorescence. Our results demonstrate that a uniform silicon nanopore array combined with wide-field optical detection is a promising alternative with which to realize massively-parallel single-molecule detection.

Spectrally resolved photoluminescence (PL) decays were measured for samples of colloidal, ligand-passivated silicon nanocrystals. These samples have PL emission energies with peak positions in the range ∼1.4-1.8 eV and quantum yields of ∼30-70%. Their ensemble PL decays are characterized by a stretched-exponential decay with a dispersion factor of ∼0.8, which changes to an almost monoexponential character at fixed detection energies. The dispersion factors and decay rates for various detection energies were extracted from spectrally resolved curves using a mathematical approach that excluded the effect of homogeneous line width broadening. Since nonradiative recombination would introduce a random lifetime variation, leading to a stretched-exponential decay for an ensemble, we conclude that the observed monoexponential decay in size-selected ensembles signifies negligible nonradiative transitions of a similar strength to the radiative one. This conjecture is further supported as extracted decay rates agree with radiative rates reported in the literature, suggesting 100% internal quantum efficiency over a broad range of emission wavelengths. The apparent differences in the quantum yields can then be explained by a varying fraction of "dark" or blinking nanocrystals.

A simple schematic on parallel optical detection of two-fluorophore barcode for single-molecule nanopore sensing is presented. The chosen two fluorophores, ATTO-532 and DY-521-XL, emitting in well-separated spectrum range can be excited at the same wavelength. A beam splitter was employed to separate signals from the two fluorophores and guide them to the same CCD camera. Based on a conventional microscope, sources of background in the nanopore sensing system, including membranes, compounds in buffer solution, and a detection cell was characterized. By photoluminescence excitation measurements, it turned out that silicon membrane has a negligible photoluminescence under the examined excitation from 440 nm to 560 nm, in comparison with a silicon nitrite membrane. Further, background signals from the detection cell were suppressed. Brownian motion of 450 bps DNA labelled with single ATTO-532 or DY-521-XL was successfully recorded by our optical system.

Single dot spectroscopy allows studying properties of a single nanocrystal avoiding inhomogeneous broadening of the emission band. Here, data obtained by this technique for Si nanocrystals fabricat ...

Silicon nanoparticles (SiNPs) are formed by implanting 70keV Si+ into a SiO2-film and subsequent thermal annealing. SiNP samples are further annealed in forming gas. Another group of samples contai ...