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Eingeladener Vortrag
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Lanthanide-doped photon-upconversion nanoparticles (UCNPs) have been the Focus of many Research activities in materials and life sciences in the last 15 years because of their potential to convert light between different spectral regions and their unique photophysical properties. To fully exploit the application potential of These facinating nanomaterials, a number of challenges have to be overcome, such as the low brightness, particularly of small UCNPs, and the reliable quantification of the excitation-power-density-dependent upconversion luminescence. In this series of critical Reviews, recent developments in the design, Synthesis, optical-spectroscopic characterization, and application of UCNPs are presented with Special Focus on bioanalysis and the life sciences. Here we guide the reader from the Synthesis of UCNPs to different concepts to enhance their luminescence, including the required optical-spectroscopic assessment to quantify material Performance; surface modification strategies and bioanalytical applications as well as selected examples of the use of UCNPs as reporters in different Assay formats are addressed in part II. Future Trends and challenges in the field of upconversion are discussed with Special emphasis on UCNP Synthesis and material characterization, particularly quantitative luminescence studies.
The rational design of functional nanomaterials for optical applications in the material and life sciences requires optical-spectroscopic methods for the quantitative characterization of their signal-relevant optical properties. Additionally, methods for the simple and quantitative analysis of the surface chemistry are desired as the chemical nature and number of the surface groups and ligands can affect the optical features and controls the interaction of these nanomaterials with their environment. Here, we present quantitative photoluminescenvce studies of different types of vis/NIR-emissive nanomaterials like semiconductor quantum dots and upconversion nanocrystals will be presented and their relevance for the mechanistic understanding of nonradiative decay channels and the rational design of new nanomaterials will be underpinned. In this respect, also validation concepts for such measurements and absolute fluorometry will be introduced. In addition, the potential of optical spectroscopy for surface group and ligand analysis surface chemistry will be demonstrated exemplarily for semiconductor quantum dots
Lanthanide-doped photon-upconversion nanoparticles (UCNPs) have been in the focus of many research activities in the material and life sciences over the last 15 years because of their potential to convert light between different spectral regions and their unique photophysical properties. In order to fully exploit the application potential of these fascinating nanomaterials, a number of challenges has to be overcome such as the low brightness particularly of small UCNPs and the reliable quantification of the excitation power density (P)-dependent upconversion luminescence (UCL). Here, the need and requirements on the characterization of the optical properties of UCNPs are discussed with special focus on the reliabiliy and comparability of relative and quantitative luminescence measurements and prerequisites for their standardization.
At the core of luminescence color and lifetime tuning of rare earth doped upconverting nanoparticles (UCNPs) is the understanding of the impact of the particle architecture for commonly used sensitizer (S) and activator (A) ions. In this respect, we present here a series of core@shell NaYF4 UCNPs doped with Yb3+ and Ho3+ ions, where the same dopant concentrations were distributed in different particle architectures following the scheme: YbHo core and YbHo@..., …@YbHo, Yb@Ho, Ho@Yb, YbHo@Yb, and Yb@YbHo core-shell NPs. As revealed by quantitative steady state and time-resolved luminescence studies, the relative spatial distribution of the A and S ions in the UCNPs and their protection from surface quenching has critical impact on their luminescent characteristics. Interestingly, although the increased amount of Yb3+ ions boosts UCNP performance by increasing the absorption, the Yb3+ ions can also dissipate the energy stored in the material through energy migration to surface, thereby reducing the overall energy transfer efficiency to the activator ions.
Functional Nanomaterials with VIS/NIR Emission-Spectroscopic Properties And Surface Group Analysis
(2017)
Optical-spectroscopic methods for the quantitative characterization of the optical properties of different types of vis/NIR-emissive nanomaterials like semiconductor quantum dots and upconversion nanocrystals will be presented and their relevance for the mechanistic understanding of nonradiative decay channels and the rational design of new nanomaterials will be underpinned. In this respect, also validation concepts for such measurements and absolute fluorometry will be introduced. In addition, the potential of optical spectroscopy for surface group and ligand analysis surface chemistry will be demonstrated exemplarily for semiconductor quantum dots.
The excitation wavelength (lexc) dependence of the photoluminescence (PL) quantum yield (FPL) and decay behavior (tPL) of a series of CdSe/CdS quantum dot/Quantum rods (QDQRs), consisting of the same spherical CdSe core and rod-shaped CdS shells, with aspect ratios ranging from 2 to 20 was characterized. lexc between 400–565 nm were chosen to cover the first excitonic absorption band of the CdSe core material, the onset of absorption of the CDs shell, and the region of predominant shell absorption. A strong lexc dependence of relative and absolutely measured FPL and tPL was found particularly for the longer QDQRs with higher aspect ratios. This is attributed to combined contributions from a length-dependent shell-to-core exciton localization efficiency, an increasing number of defect states within the shell for the longest QDQRs, and probably also the presence of absorbing, yet non-emitting shell material. Although the FPL values of the QDQRs decrease at shorter wavelength, the extremely high extinction coefficients introduced by the shell outweigh this effect, leading to significantly higher brightness values at wavelengths below the absorption onset of the CdS Shell compared with direct excitation of the CdSe cores. Moreover, our results present also an interesting example for the comparability of absolutely measured FPL using an integrating sphere setup and FPL values measured relative to common FPL standards, and underline the Need for a correction for particle scattering for QDQRs with high aspect ratios.
The rational design of brighter upconversion nanoparticles (UCNPs) requires a better understanding of the radiationless deactivation pathways in these materials. Here, we demonstrate the potential of excitation power density (P)-dependent studies of upconversion (UC) luminescence intensities, slope factors, and absolute quantum yields (ΦUC) of popular β-NaYF4:20% Yb3+,2% Er3+ UCNPs of different surface chemistries in organic solvents, D2O, and water as a tool to gain deeper insight into the UC mechanism including population and deactivation pathways particularly of the red emission. Our measurements, covering a P regime of three orders of magnitude, reveal a strong difference of the P-dependence of the ratio of the green and red luminescence bands (Ig/r) in water and organic solvents and P-dependent population pathways of the different emissive energy levels of Er3+. In summary, we provide experimental evidence for three photon processes in UCNPs, particularly for the red emission. Moreover, we demonstrate changes in the excited population dynamics via bi- and triphotonic processes dependent on the environment, surface chemistry, and P, and validate our findings theoretically
Quality control requirements imposed on assays used in clinical diagnostics and point-of-care-diagnostic testing (POCT), utilizing amplification reactions performed at elevated temperatures of 35 to 95 °C are very stringent. As the temperature of a reaction vessel has a large impact on the specificity and sensitivity of the amplification reaction, simple tools for local in situ temperature sensing and monitoring are required for reaction and assay control. We describe here a platform of stem-and-loop structured DNA hairpins (molecular beacons, MBs), absorbing and emitting in the visible and red spectral region, rationally designed for precise temperature measurements in microfluidic assays for POCT, and their ap-plication for temperature measurements in a common DNA-based molecular biological assay utilizing thermophilic helicase-dependent amplification (tHDA). Spectroscopic studies of these MBs, rationally designed from DNA se-quences of different thermal stabilities, chosen not to interact with the DNA probes applied in the nucleic acid amplification assay, and temperature-dependent fluorescence measurements of MB-assay mixtures revealed the suitability of these MBs for temperature measurements directly in such an assay with a temperature resolution of about 0.5 °C without interferences from assay components. Combining two spectrally distinguishable MBs provides a broader response range and an increase in temperature sensitivity up to 0.1 °C. This approach will find future application for temperature monitoring and quality control in commercialized diagnostics assays using dried reagents and microfluidic chips as well as assays read out with tube and microplate readers and PCR detection systems for temperature measurements in the range of 35 to 95 °C.
3-Aminovinylquinoxalines are readily accessible from (hetero)aryl glyoxylic acids or heterocyclic π-nucleophiles by consecutive four- and fivecomponent syntheses in the sense of an activation-alkynylation-cyclocondensation-addition sequence or glyoxylation-alkynylation-cyclocondensation-addition sequence in good yields. The title compounds are highly fluorescent with pronounced emission solvatochromicity and protochromic fluorescence quenching. Time-resolved fluorescence spectroscopy furnishes radiative and nonradiative fluorescence decay rates in various solvent polarities. The electronic structure is corroborated by DFT and TD-DFT calculations rationalizing the observed spectroscopic effects.
Lanthanide-doped up-converting nanoparticles (UCNPs) are promising reporters for medical diagnostics and bioimaging. Current limitations present their relative low absorption cross sections and low fluorescence efficiencies, with the latter being affected by particle size, surface chemistry, and microenvironment, particularly water.
Here, we present results from systematic studies of the excitation power density dependent upconversion luminescence spectra, intensities/intensity ratios of the individual emission bands, slope factors, and quantum yields of UCNPs of varying size, dopant concentration, and surface chemistry in different microenvironments as well as the up- and downconversion luminescence decay kinetics of the different emission bands. Moreover, first studies of the energy transfer from UCNPs to surface-bound organic dyes acting as fluorescence acceptors are shown. Based upon these measurements, fluorescence deactivation channels are identified and spectroscopic parameters for the screening of material performance are derived.