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Eingeladener Vortrag
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Yb,Nd,Er-doped upconversion nanoparticles (UCNPs) have attracted considerable interest as luminescent reporters for bioimaging, sensing, energy conversion/shaping, and anticounterfeiting due to their capability to convert multiple near-infrared (NIR) photons into shorter wavelength ultraviolet, visible or NIR luminescence by successive absorption of two or more NIR photons. This enables optical measurements in complex media with very little background and high penetration depths for bioimaging. The use of Nd3+ as substitute for the commonly employed sensitizer Yb3+ or in combination with Yb3+ shifts the excitation wavelength from about 980 nm, where the absorption of water can weaken upconversion luminescence, to about 800 nm, and laser-induced local overheating effects in cells, tissue, and live animal studies can be minimized. To systematically investigate the potential of Nd3+ doping, we assessed the performance of a set of similarly sized Yb3+,Nd3+,Er3+-doped core- and core–shell UCNPs of different particle architecture in water at broadly varied excitation power densities (P) with steady state and time-resolved fluorometry for excitation at 980 nm and 808 nm. As a measure for UCNPs performance, the P-dependent upconversion quantum yield (Φ) and its saturation behavior were used as well as particle brightness (B). Based upon spectroscopic measurements at both excitation wavelengths in water and in a lipid phantom and B-based calculations of signal size at different penetration depths, conditions under which excitation at 808 nm is advantageous are derived and parameters for the further optimization of triple-doped UCNPs are given.
Non-linear optical emitters are promising materials for energy applications and biotechnologies. Solid-state multi-band emitters like lanthanide doped up-conversion nanoparticles (UCNPs) show excellent photostability, are excitable in the near infrared (NIR), and show emission bands from the UV to SWIR spectral regions. The optical properties of these materials strongly depend on the excitation power density, i.e., the number of photons absorbed per time interval. The upconversion (ΦUC) and downshifting quantum efficiencies (ΦDS) of these materials, the excitation power dependent population, and the deactivation dynamics are influenced by nanoparticle architecture, doping concentration, and the microenvironment. We studied the fundamental changes of the luminescence properties of ß-NaYF4 UCNPs doped with Yb3+ and Er3+ depending on size, different surroundings such as aqueous and organic media, and different surface chemistries. We obtained further insights into shelling procedures, FRET optimization, influence of doping concentration, and advantages of different sensitizer ions.
In contrast to microplastics, little is known about nanoplastics (1 to 100 nm). In order to make the dectecability of nanoplasics more reliable, we started to develop nanoplastic reference materials. This project also aims to anser the question of how the single chain conformation of bio(polymers) changes in contact with nanoplastics. Small-angle X-ray and neutron scattering methods are suitable methods for studing this topic. Recently the soft and hard interactions between polystyrene nanoplasics and human serum albumin corona was investigated with small-angle neutron scattering. Here we concentrate on small-angle X-ray scattering as our favorite method to study how (bio)polymers change their conformation in contact with nanoplastics. The scattering of bovine serum albumin in its native state can be detected easily. The scattering pattern of this biopolymer changes dramatically when its globular stucture changes to a coil structure. Modeling of chain conformations and the calculation of the scattering pattern is relatively easy to perform. Numerous model calculations will be provided to predict the changes of conformation of single bio(polymer) chains when in conatact with nanoplastics. These predictions will be compared with recent experimenal results from in situ measurments of bio(polymers) in contact with nanoplastics. The impact of temperature, polymer concentration and salt on the single-chain conformation changes will be discussed.
Single-particle inductively coupled plasma mass spectrometry (sp-ICP-MS) has become an effective tool for the detection and quantification of inorganic nanoparticles (NPs). While sizing of NPs suspended in water is relatively straightforward by sp-ICP-MS, accurate mass quantification of NPs in complex media, such as consumer products and natural systems still remains a challenge. When NPs are suspended in a complex medium, the matrix may affect the analyte sensitivity and lead to inaccurate NP sizing. Here, we investigate the use of an online microdroplet calibration system to size NPs in a single step. In this setup, microdroplets—which are used as the calibrant to determine elemental sensitivities—and nebulized NP-containing solutions are introduced concurrently into the ICP via a dual-inlet sample introduction system. Because calibrant microdroplets and analyte NPs experience the same plasma conditions, both the microdroplets and the NPs are subjected to the same matrix-related signal enhancement or suppression. In this way, the microdroplet calibration standards are automatically matrix matched with the NP-containing solution. The online microdroplet calibration system is combined with an ICP-TOFMS instrument for simultaneous measurement of multiple elements in microdroplets and NPs. We investigate the ability of online microdroplet calibration to compensate for matrix effects through a series of experiments, in which Ag and Au NPs are measured with variable plasma-sampling positions, varying concentrations of HCl and HNO3, varying concentrations of single element solutions, and high concentrations of a salt matrix, i.e. phosphate buffered saline (PBS). Through these experiments, we demonstrate that the online microdroplet calibration strategy provides a matrix-independent mass quantification of analyte NPs in the presence of several established types of matrix effects, including acid effects, space-charge effects, and ionisation suppression. In results presented here, we focus on the size determination of the NPs.
Simulational tools are applied to investigate the physical properties of nanoparticles.
For the description of radioactive gold nanoparticles, particles scattering simulations are performed with the Geant4 monte carlo simulation toolkit.
The temperature dependent behaviour of the magnetization dynamics of different magnetic nanoparticles are simulated with the object oriented micormagnetic framework (OOMMF).
Nowadays, different nanoparticles have been developed for commercial applications. However, since data on toxicity are barely available, their increasing application in cosmetic products, food and their release in the environment might cause severe problems. Since a range of physical, chemical, and biological characteristics of NPs are closely related to particle size and surface functionalization, precise separation and surface groups quantification is essential to acquire an in-depth understanding of their properties.
In this work, the performance of asymmetrical flow field flow fractionation (AF4) and capillary electrophoresis (CE) for the separation of nanoparticles (NPs) with different sizes, coatings, and coating densities was investigated and optimized.
For the first time, a two-dimensional off-line hyphenation of both techniques (AF4-CE) was developed. The results clearly demonstrated, that AF4-CE hyphenation can significantly improve the separation resolution and reduce the peak broadening in CE. Also, for the first time, CE was employed to determine the coating density of NPs and the results were in good agreement with the values acquired with conductometric titration.
Relative and Absolute Methods for Measuring Photoluminescence Quantum Yields of UV/vis/NIR Emitters
(2019)
One of the key spectroscopic performance parameters of molecular and particulate emitters is the photoluminescence quantum yield (PL QY) that provides a direct measure for the number of emitted per absorbed photons. This triggered the interest in methods suitable for measuring this property for emitters in various environments in the UV/vis/NIR and above 1000 nm as well as on the ensemble and single emitter level. Moreover, for nonlinear emitters like lanthanide-based upconversion nanocrystals methods including instrumentation for power density-dependent PL QY studies are required.
An overview of the research activities in Division Biophotonics of BAM is given and suitable relative and absolute methods for the deter-mination of PL QY of organic dyes and different types of application-relevant nanomaterials in dispersion and in the solid state are presen-ted. This covers also the design and calibration of integrating sphere setups, achievable uncertainties, and candidates for PL QY reference materials.
Two nanosensors for simultaneous optical measurements of temperature (“T”), oxygen (“O”), and pH (“P”) have been designed. These “TOP” nanosensors are based on 100 nm-sized silica-coated polystyrene nanoparticles (PS-NPs) doped with the near infrared emissive oxygen- and temperature-sensitive chromium(III) complex ([Cr(ddpd)2][BPh4]3 CrBPh4)[1][2] and an inert reference fluorescence dye (Nile Red NR or 5,10,15,20-tetrakis-(pentafluorophenyl) porphyrin TFPP) and are covalently labeled with the pH-sensitive fluorophore fluorescein isothiocyanate (FITC). These emitters can be excited at the same wavelength and reveal distinguishable emission spectra suitable for ratiometric intensity-based and time-resolved studies in the visible and near infrared spectral region. The core-shell nanostructure of these sensors reveals high colloidal stability in various aqueous media. Studies in PBS buffer solutions and in a model body liquid demonstrate the applicability of the TOP nanosensors for optically detecting the three bioanalytically and biologically relevant analytes temperature, oxygen and pH simultaneously at the same position.
Dose enhancement by gold nanoparticles (AuNP) was shown to increase the biological effectiveness of radiation damage in biomolecules and tissue. Most of the current studies focus on external beam therapy on combination with AuNP. Here we present a Monte-Carlo study (Geant4) to characterise radioactive AuNP. Radioactive ¹⁹⁸Au emits beta and gamma rays and is considered for applications with solid tumours. To effectively apply ¹⁹⁸AuNP their energy deposit characteristics have to be determined in terms of intrinsic and extrinsic properties e.g. AuNP diameter, AuNP density, and their clustering behaviour. After each decay process, the energy deposit, inelastic scattering events, kinetic energy spectrum of secondary particles within the AuNP themselves and in a spherical target volume of water up to 1 μm radius were determined. Simulations were performed for AuNP radii ranging from 2.5 nm to 20 nm radius, different cluster sizes and densities. The results show an increase of the energy deposit in the vicinity of the AuNP up to 150 nm. This effect nearly vanishes for distances up to one micron. For the case of AuNP clusters and the same activity, the enhancement of the energy deposit increases with the relative gold mass percentage and therefore can be adjusted by changing AuNP radius or clustering behaviour.
Dose enhancement by gold nanoparticles (AuNP) was shown to increase the biological effectiveness of radiation damage in biomolecules and tissue. Most of the current studies focus on external beam therapy on combination with AuNP. Here we present a Monte-Carlo study (Geant4) to characterise radioactive AuNP. Radioactive 198 Au emits beta and gamma rays and is considered for applications with solid tumours. To effectively apply 198 AuNP their energy deposit characteristics have to be determined in terms of intrinsic and extrinsic properties e.g. AuNP diameter, AuNP density, and their clustering behaviour. After each decay process, the energy deposit, inelastic scattering events, kinetic energy spectrum of secondary particles within the AuNP themselves and in a spherical target volume of water up to 1 μm radius were determined. Simulations were performed for AuNP radii ranging from 2.5 nm to 20 nm radius, different cluster sizes and densities. The results show an increase of the energy deposit in the vicinity of the AuNP up to 150 nm. This effect nearly vanishes for distances up to one micron. For the case of AuNP clusters and the same activity, the enhancement of the energy deposit increases with the relative gold mass percentage and therefore can be adjusted by changing AuNP radius or clustering behaviour.