We report a high-yield, low cost synthesis route to colloidal Cu 1-x InS 2 nanocrystals with a tunable amount of Cu vacancies in the crystal lattice. These are then converted into quaternary Cu−In−Zn−S (CIZS) nanocrystals by partial exchange of Cu + and In 3+ cations with Zn 2+ cations. The photoluminescence quantum yield of these CIZS nanocrystals could be tuned up to a record 80%, depending on the amount of copper vacancies.
Great control over size, shape and optical properties is now possible in colloidal Cd-based nanocrystals, which has paved the way for many fundamental studies and applications. One popular example of such class of nanocrystals is represented by CdSe(spherical core)/CdS(rod shell) nanorods. These can be nearly monodisperse in size and shape and have strong and stable photoluminescence that is tunable in the visible range (mainly by varying the size of the CdSe core). The corresponding Zn-based core/shell nanorods would be good candidates for tunable emission in the blue-UV region. However, while the synthesis of ZnS nanocrystals with elongated shapes has been demonstrated based on the oriented-attachment mechanism, elongated ZnS shells are difficult to fabricate because the more common cubic phase of ZnS has a highly symmetric crystal structure. We report here a procedure based on a sequence of two cation exchange reactions, namely, Cd(2+)⇒Cu(+) and then Cu(+)⇒Zn(2+), by which we transform colloidal CdSe(core)/CdS(shell) nanorods first into into Cu(2)Se/Cu(2)S nanorods, which are then converted into blue-UV fluorescent ZnSe(core)/ZnS(shell) nanorods. The procedure transfers the morphological and structural information of the initial Cd-based nanorods to the Zn-based nanorods. Therefore, the final nanoparticles are made by a ZnSe dot embedded in a rod-shaped shell of wurtzite ZnS. Since in the starting Cd-based nanorods the size of the CdSe core and the length of the CdS shell can be well controlled, the same holds for the final Zn-based rods. In the second step of the exchange reaction (Cu(+)⇒Zn(2+)), a large excess of Zn(2+) ions added over the Cu(+) ions present in the Cu(2)Se/Cu(2)S nanorods is the key requisite to obtain bright, band-edge emission (with quantum yields approaching 15%) with narrow line widths (approaching 75 meV). In these ZnSe/ZnS nanorods, photogenerated carriers appear to be more confined in the core region compared to their parent CdSe/CdS nanorods.
Fluorescence lifetime imaging is a rather new and effective tool that can be used to study complex biological samples, either at microscopic or macroscopic levels. The map of the fluorescence lifetime allows one to discriminate amongst different fluorophores and to achieve valuable insights into the behaviour of emitting molecules, leading to information like local pH, oxygen concentration in cells, etc. Moreover, the distribution in space of any fluorescent marker achievable with this technique can be exploited for diagnostic purposes in medicine. After a brief introduction on the motivations for applying fluorescence lifetime imaging in biology and medicine, the basic principles of this technique will be addressed. Then, the two possible implementations of fluorescence lifetime imaging (i.e. the frequency domain and the time domain methods) will be presented. For this purpose, special attention will be devoted to practical aspects of image acquisition and processing, especially for what concerns the time domain method. Then, the analysis of the state-of-the-art systems will include a brief discussion on new concepts that have recently been introduced in this research field. Finally, two interesting applications of fluorescence lifetime imaging will be presented. The former refers to skin tumour detection and has been successfully applied in a preliminary clinical trial, the latter regards DNA chips reading and has been tested only at laboratory level, yet it has produced promising results for its future implementation in commercial systems.
Aiming at discerning the role of fluorine from that of nitrogen as a dopant in N,F-codoped TiO 2 , a series of HF-doped TiO 2 photocatalysts were investigated in the decomposition of formic and acetic acid in aqueous suspensions, also as a function of the irradiation wavelength (action spectra analysis), in comparison with recent results obtained with an analogous series of NH 4 F-doped TiO 2 photocatalysts. Visible light absorption around 420 nm, which was found to be inactive in acetic acid decomposition, is definitely shown to be associated with nitrogen doping, whereas the enhanced absorption at ca. 365 nm, increasing with increasing calcination temperature, can be unambiguously attributed to structural modifications induced by fluorine doping. Action spectra analysis confirms that this absorption is active in acetic acid decomposition, in both HF-and NH 4 F-doped TiO 2 photocatalysts. From time-resolved photoluminescence (PL) spectroscopy analysis, a clear correlation is outlined between the photoactivity of the materials and the long-lasting component of the PL signal, which increases with the calcination temperature and is related to the formation of surface defects. Thus, fluorine doping, followed by calcination at high temperature, increases the amount of surface traps originating the long-lasting PL signal, which are beneficial in photoactivity by ensuring long-living photoproduced charge couples.
We study the exciton valley relaxation dynamics in single-layer MoS 2 by a combination of two nonequilibrium optical techniques: time-resolved Faraday rotation and time-resolved circular dichroism. The depolarization dynamics, measured at 77 K, exhibits a peculiar biexponential decay, characterized by two distinct time scales of 200 fs and 5 ps. The fast relaxation of the valley polarization is in good agreement with a model including the intervalley electron-hole Coulomb exchange as the dominating mechanism. The valley relaxation dynamics is further investigated as a function of temperature and photoinduced exciton density. We measure a strong exciton density dependence of the transient Faraday rotation signal. This indicates the key role of exciton-exciton interactions in MoS 2 valley relaxation dynamics.
Time-resolved reflectance spectroscopy can be used to assess nondestructively the bulk (rather than the superficial) optical properties of highly diffusive media. A fully automated system for time-resolved reflectance spectroscopy was used to evaluate the absorption and the transport scattering spectra of fruits in the red and the near-infrared regions. In particular, data were collected in the range 650-1000 nm from three varieties of apples and from peaches, kiwifruits, and tomatoes. The absorption spectra were usually dominated by the water peak near 970 nm, whereas chlorophyll was detected at 675 nm. For ail species the scattering decreased progressively with increasing wavelength. A best fit to water and chlorophyll absorption line shapes and to Mie theory permitted the estimation of water and chlorophyll content and the average size of scattering centers in the bulls; of intact fruits.
Single pixel camera imaging is an emerging paradigm that allows high-quality images to be provided by a device only equipped with a single point detector. A single pixel camera is an experimental setup able to measure the inner product of the scene under view-the image-with any user-defined pattern. Post-processing a sequence of point measurements obtained with different patterns permits to recover spatial information, as it has been demonstrated by state-of-theart approaches belonging to the compressed sensing framework. In this paper, a new framework for the choice of the patterns is proposed together with a simple and efficient image recovery scheme. Our goal is to overcome the computationally demanding 1-minimization of compressed sensing. We propose to choose patterns among a wavelet basis in an adaptive fashion, which essentially relies onto the prediction of the significant wavelet coefficients' location. More precisely, we adopt a multiresolution strategy that exploits the set of measurements acquired at coarse scales to predict the set of measurements to be performed at a finer scale. Prediction is based on a fast cubic interpolation in the image domain. A general formalism is given so that any kind of wavelets can be used, which enables one to adjust the wavelet to the type of images related to the desired application. Both simulated and experimental results demonstrate the ability of our technique to reconstruct biomedical images with improved quality compared to CS-based recovery. Application to real-time fluorescence imaging of biological tissues could benefit from the proposed method.
In oxygenic photosynthetic eukaryotes, the hydroxylated carotenoid zeaxanthin is produced from preexisting violaxanthin upon exposure to excess light conditions. Zeaxanthin binding to components of the photosystem II (PSII) antenna system has been investigated thoroughly and shown to help in the dissipation of excess chlorophyll-excited states and scavenging of oxygen radicals. However, the functional consequences of the accumulation of the light-harvesting complex I (LHCI) proteins in the photosystem I (PSI) antenna have remained unclarified so far. In this work we investigated the effect of zeaxanthin binding on photoprotection of PSI-LHCI by comparing preparations isolated from wild-type Arabidopsis thaliana (i.e., with violaxanthin) and those isolated from the A. thaliana nonphotochemical quenching 2 mutant, in which violaxanthin is replaced by zeaxanthin. Time-resolved fluorescence measurements showed that zeaxanthin binding leads to a previously unrecognized quenching effect on PSI-LHCI fluorescence. The efficiency of energy transfer from the LHCI moiety of the complex to the PSI reaction center was down-regulated, and an enhanced PSI resistance to photoinhibition was observed both in vitro and in vivo. Thus, zeaxanthin was shown to be effective in inducing dissipative states in PSI, similar to its well-known effect on PSII. We propose that, upon acclimation to high light, PSI-LHCI changes its light-harvesting efficiency by a zeaxanthin-dependent quenching of the absorbed excitation energy, whereas in PSII the stoichiometry of LHC antenna proteins per reaction center is reduced directly.photosynthesis | xanthophylls | violaxanthin de-epoxidase | photobleaching
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