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Lanthanide-doped NaYF4 upconversion nano- and microcrystals were synthesized via a facile solvothermal approach. Thereby, the influence of volume ratios of ethylene glycol (EG)/H2O, molar ratios of NH4F/RE3+ (RE3+ represents the total amount of Y3+ and rare-earth dopant ions), Gd3+ ion contents, types of activator dopant ions, and different organic co-solvents on the crystal phase, size, and morphology of the resulting particles were studied systematically. A possible formation mechanism for the growth of crystals of different morphology is discussed. Our results show that the transition from the α- to the β-phase mainly depends on the volume ratio of EG/H2O and the molar ratio of NH4F/RE3+, while the morphology and size could be controlled by the type of organic co-solvent and Gd3+ dopant ions. Furthermore, the reaction time has to be long enough to convert α-NaYF4 into β-NaYF4 during the growth process to optimize the upconversion luminescence. The formation of larger β-NaYF4 crystals, which possess a higher upconversion luminescence than smaller particles, proceeds via intermediates of smaller crystals of cubic structure. In summary, our synthetic approach presents a facile route to tailor the size, Crystal phase, morphology, and luminescence features of upconversion
materials.
Solovyev, N. ; El-Khatib, Ahmed ; Costas-Rodrigues, M. ; Schwab, K. ; Griffin, E. ; Raab, A. ; Platt, B. ; Theuring, F. ; Vogl, Jochen ; Vanhaecke, F.
Alzheimer’s disease (AD) is characterized by accumulation of tau and amyloid-beta in the brain, and recent evidence suggests a correlation between associated protein aggregates and trace elements, such as copper, iron and zinc. In AD, distorted brain redox homeostasis and complexation by amyloid-beta and hyperphosphorylated tau May alter the isotopic composition of essential mineral elements. Therefore, high-precision isotopic analysis may reveal changes in the homeostasis of these elements. We used inductively coupled plasma-mass spectrometry (ICP-MS)-based techniques to determine the total Cu, Fe and Zn contents in the brain, as well as their isotopic compositions in both mouse brain and serum.
Results for male transgenic tau (Line 66, L66) and amyloid/presenilin (5xFAD) mice were compared to those for the corresponding age- and gendermatched wild-type control mice (WT). Our data show that L66 brains showed significantly higher Fe levels than the corresponding WT. Significantly less Cu, but more Zn was found in 5xFAD brains. We observed significantly lighter isotopic compositions of Fe (enrichment in the lighter isotopes) in the brain, and in serum of L66 mice compared to WT. For 5xFAD mice, Zn exhibited a trend towards a lighter isotopic composition in brain and a heavier isotopic composition in serum compared to WT. Neither mouse model yielded differences in the isotopic composition of Cu. Our findings indicate significant pathology-specific alterations of Fe and Zn brain homeostasis in mouse models of AD. The associated changes in isotopic composition May serve as a marker for proteinopathies Underlying AD and other types of dementia.
Kader, A. ; Brangsch, J. ; Kaufmann, Jan Ole ; Zhao, J. ; Mangarova, D. B. ; Moeckel, J. ; Adams, L. C. ; Sack, I. ; Taupitz, M. ; Hamm, B. ; Makowski, M. R.
This review summarizes recent developments regarding molecular imaging markers for magnetic resonance imaging (MRI) of prostate cancer (PCa). Currently, the clinical standard includes MR imaging using unspecific gadolinium-based contrast agents. Specific molecular probes for the diagnosis of PCa could improve the molecular characterization of the tumor in a non-invasive examination. Furthermore, molecular probes could enable targeted therapies to suppress tumor growth or reduce the tumor size.
Climent Terol, Estela ; Biyikal, Mustafa ; Gröninger, Delia ; Weller, Michael G. ; Martínez Mánez, R. ; Rurack, Knut
Vor dem Hintergrund der einzigartigen Modularität, hohen Empfindlichkeit und Selektivität von Antikörper‐gesteuerten Indikatorfreisetzungssystemen (gAID‐Systemen) wurde hier ein Multiplex‐Assay für drei organische Explosivstoffmoleküle (TATP, TNT, PETN) entwickelt, der es erlaubt, die Analyten gleichzeitig in flüssiger Phase mit einem einzelnen Teststreifen und einem Fluoreszenzlesegerät bzw. Smartphone als Detektor in Konzentrationen bis in den unteren ppb‐Bereich in <5 min nachzuweisen. Alle drei Systeme, darunter die hier neu entwickelten Systeme für TNT und PETN, tolerieren zudem nicht nur gepufferte wässrige Modelllösungen, sondern auch komplexere Matrices. Neben einem konventionellen Teststreifen mit einem Kanal erlaubte uns die Anwendung von Wachsdrucktechnologie das Herstellen von mehrkanaligen Streifen mit vergleichbarer analytischer Leistungsfähigkeit, was das enorme Potenzial der modular aufgebauten, hybriden Biosensormaterialien im Hinblick auf eine für den Endanwender maßgeschneiderte Vor‐Ort‐Analytik unterstreicht.
Climent Terol, Estela ; Biyikal, Mustafa ; Gröninger, Delia ; Weller, Michael G. ; Martínez Mánez, R. ; Rurack, Knut
Rapid testing methods for the use directly at apointof need are expected to unfold their true potential especiallywhen offering adequate capabilities for the simultaneousmeasurement of multiple analytes of interest. Considering theunique modularity,high sensitivity,and selectivity of antibody-gated indicator delivery (gAID) systems,amultiplexed assayfor three small-molecule explosives (TATP, TNT,PETN) wasthus developed, allowing to detect the analytes simultaneouslywith asingle test strip at lower ppb concentrations in the liquidphase in < 5min using afluorescence reader or asmartphonefor readout. While the TNT and PETN systems were newlydeveloped here,all the three systems also tolerated harshermatrices than buffered aqueous model solutions.Besidesasingle-track strip,the outstanding modularity of the hybridbiosensor materials in combination with strip-patterningtechnologies allowed us to obtain amultichannel strip inastraightforwardmanner,offering comparable analyticalperformance while allowing to be tailored even more to theusersneed.
Pharmacologically active compounds are often detected in wastewater and surface waters. The nonsteroidal anti-inflammatory drug diclofenac (DCF) was included in the European watch list of substances that requires its environmental monitoring in the member states. DCF may harmfully influence the ecosystem already at concentrations ≤ 1 μg L−1. The fast and easy quantification of DCF is becoming a subject of global importance. Fluorescence polarization immunoassay (FPIA) is a homogeneous mix-and-read method which does not require the immobilization of reagents. FPIA can be performed in one phase within 20–30 min, making it possible to analyse wastewater without any complicated pre-treatment. In this study, new tracermolecules with different structures, linking fluorophores to derivatives of the analyte, were synthesized, three homologous tracers based on DCF, two including a C6 spacer, and one heterologous tracer derived from 5-hydroxy-DCF. The tracer molecules were thoroughly assessed for performance. Regarding sensitivity of the FPIA, the lowest limit of detection reached was 2.0 μg L−1 with a working range up to 870 μg L−1. The method was validated for real wastewater samples against LC-MS/MS as reference method with good agreement of both methods.
Santos, C.I.L. ; Machado, W.S. ; Wegner, Karl David ; Gontijo, L.A.P. ; Bettini, J. ; Schiavon, M.A. ; Reiss, P. ; Aldakov, D.
facile hydrothermal method to synthesize water-soluble copper indium sulfide (CIS) nanocrystals (NCs) at 150 degrees C is presented. The obtained samples exhibited three distinct photoluminescence peaks in the red, green and blue spectral regions, corresponding to three size fractions, which could be separated by means of size-selective precipitation. While the red and green emitting fractions consist of 4.5 and 2.5 nm CIS NCs, the blue fraction was identified as in situ formed carbon nanodots showing excitation wavelength dependent emission. When used as light absorbers in quantum dot sensitized solar cells, the individual green and red fractions yielded power conversion efficiencies of 2.9% and 2.6%, respectively. With the unfractionated samples, the efficiency values approaching 5% were obtained. This improvement was mainly due to a significantly enhanced photocurrent arising from complementary panchromatic absorption.
Weigert, Florian ; Müller, A. ; Häusler, I. ; Geißler, Daniel ; Skroblin, D. ; Unger, Wolfgang ; Radnik, Jörg ; Resch-Genger, Ute
Controlling thickness and tightness of surface passivation shells is crucial for many applications of core–shell nanoparticles (NP). Usually, to determine shell thickness, core and core/shell particle are measured individually requiring the availability of both nanoobjects. This is often not fulfilled for functional nanomaterials such as many photoluminescent semiconductor quantum dots (QD) used for bioimaging, solid state lighting, and display technologies as the core does not show the applicationrelevant functionality like a high photoluminescence (PL) quantum yield, calling for a whole nanoobject approach. By combining high-resolution transmission electron microscopy (HR-TEM) and X-ray photoelectron spectroscopy (XPS), a novel whole nanoobject approach is developed representatively for an ultrabright oleic acid-stabilized, thick shell CdSe/CdS QD with a PL quantum yield close to unity. The size of this spectroscopically assessed QD, is in the range of the information depth of usual laboratory XPS. Information on particle size and monodispersity were validated with dynamic light scattering (DLS) and small angle X-ray scattering (SAXS) and compared to data derived from optical measurements. In addition to demonstrating the potential of this novel whole nanoobject approach for determining architectures of small nanoparticles, the presented results also highlight challenges faced by different sizing and structural analysis methods and method-inherent uncertainties.
The growth of ultrathin layers of VOx (<12 monolayers) on Pt(111) and the activity of these layers in catalytic methanol oxidation at 10−4 mbar have been studied with low-energy electron difraction, Auger electron spectroscopy, rate measurements, and with photoemission electron microscopy. Reactive deposition of V in O2 at 670 K obeys a Stranski–Krastanov growth mode with a (√3 × √3)R30° structure representing the limiting case for epitaxial growth of 3D-VOx. The activity of VOx/Pt(111) in catalytic methanol oxidation is very low and no redistribution dynamics is observed lifting the initial spatial homogeneity of the VOx layer. Under reaction conditions, part of the surface vanadium difuses into the Pt subsurface region.
Exposure to O2 causes part of the V to difuse back to the surface, but only up to one monolayer of VOx can be stabilized in this way at 10−4 mbar.
Keller, S. ; Borde, T. ; Brangsch, J. ; Reimann, C. ; Kader, A. ; Schulze, D. ; Buchholz, R. ; Kaufmann, Jan Ole ; Karst, U. ; Schellenberger, E. ; Hamm, B. ; Makowski, M. R.
To investigate the imaging performance of an elastin-specific molecular magnetic resonance imaging (MRI) probe with respect to the extracellular matrix (ECM) in an experimental hepatic cancer model. Twelve rabbits with hepatic VX2 tumors were examined using 3 T MRI 14, 21, and 28 days after tumor implantation for two subsequent days (gadobutrol, day 1; elastin-specific probe, day 2). The relative enhancement (RE) of segmented tumor regions (central and margin) and the peritumoral matrix was calculated using pre-contrast and delayed-phase T1w sequences. MRI measurements were correlated to histopathology and element-specific and spatially resolved mass spectrometry (MS). Mixed-model analysis was performed to assess the performance of the elastin-specific probe. In comparison to gadobutrol, the elastin probe showed significantly stronger RE, which was pronounced in the tumor margin (day 14–28: P ≤ 0.007). In addition, the elastin probe was superior in discriminating between tumor regions (χ2(4) = 65.87; P < 0.001). MRI-based measurements of the elastin probe significantly correlated with the ex vivo elastinstain (R = .84; P <0 .001) and absolute gadolinium concentrations (ICP-MS: R = .73, P <0 .01). LA-ICP-MS imaging confirmed the colocalization of the elastin-specific probe with elastic fibers. Elastin-specific molecular MRI is superior to non-specific gadolinium-based contrast agents in imaging the ECM of hepatic tumors and the peritumoral tissue.