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Lanthanide-doped up-converting nanoparticles (UCNPs) are promising reporters for medical diagnostics and bioimaging, which are excited in the near infrared (NIR) by multiphoton absorption processes, and show multiple narrow emission bands in the visible (vis) and NIR, long luminescence lifetimes in the μs range, and excellent photostability. 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.
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.
Due to their unique physical properties, particularly their electronic and luminescent properties, graphene quantum dots (GQDs) are expected to be suitable for a wide range of applications in bioimaging, electro-optical and photonic materials or energy harvesting among others.1 Tuning the surface chemistry provides an efficient approach to modulate the fluorescence and distinct electronic properties of GQDs.2 Nevertheless, the role of surface chemistry on the electronic structure of GQDs remains poorly understood. In this presentation, we will compare systematically the electronic and chemical structures of GQDs functionalized with carboxylic and aminated groups to those of non-functionalized GQDs, combining theoretical and experimental approaches, here various photon-based spectroscopies. First, the electronic structure of GQDs was characterized by soft X-ray absorption (XA) and X-ray emission (XE) spectroscopies, probing unoccupied and occupied electronic states, respectively, at the carbon K edge for the first time. The interpretation of the XA/XE spectra was done based on theoretical calculations. Then, the chemical structure of the GQDs was characterized in situ by ATR-FTIR in water, thereby accounting for the importance of the interface between GQDs and water believed to play a central role in the chemical reactivity and the optical properties. We previously demonstrated that monitoring the OH vibrations of water molecules during exposure to humid air was a powerful method to probe H-bonding environment around carbon nanomaterials.3 For GQDs, clear surface-dependent water adsorption profiles are observed and discussed. Finally, UV/Vis absorption and photoluminescence measurements were done to characterize the optical properties of these GQDs. Our results suggest that the surface chemistry of the GQDs affects significantly their electronic structure and optical properties. These findings will contribute to an improved understanding of the structure–activity relationship of GQDs and other carbon nanomaterials with surface modifications.
The overall objective of project Improved traceability chain of nanoparticle size measurements is to improve the traceability chain for nanoparticle size measurements. The main impact will be achieved by manifold contributions to standard documents for CEN/TC 352 “Nanotechnologies”, which directly addresses the research needs of CEN, CENELEC and ETSI mandated by EC to develop standards for methods and reference materials to accurately measure the size and size distribution of nanoparticles. This will take place in collaboration with ISO/TC229 ‘Nanotechnologies’, ISO/TC24/SC4 ‘Particle characterization’ and ISO/TC201 ‘Surface analysis’/ SC9 ‘Scanning probe microscopy’.
There is an increasing interest in optical reporters like semiconductor and lanthanide-based nanocrystals with emission > 800 nm and recently also > 1000 nm for bioanalysis, medical diagnostics, and safety barcodes. Mandatory for the comparison of different emitter classes and the rational design of the next generation of reporters for the short wavelength infrared (SWIR) region are reliable and quantitative photoluminescence measurements in this challenging wavelength region. This is of special relevance for nanocrystalline emitters like semiconductor quantum dots and rods as well as for upconversion and downconversion nanocrystals, where surface states and the accessibility of emissive states by quenchers largely control accomplishable quantum yields and hence, signal sizes and detection sensitivities from the reporter side. Such measurements are currently hampered by the lack of suitable methods and standards for instrument calibration and validation as well as by the lack of quantum yield standards with emission > 800 nm and especially > 1000 nm.
In this respect, we present the design of integrating sphere setups for absolute and excitation power densitydependent measurements of emission spectra and quantum yields in the wavelength region of 650 to 1650 nm
including calibration strategies and first candidates for potential fluorescence standards. Subsequently, the photoluminescence properties of different types of nanocrystals are presented and discussed including absolute photoluminescence measurements of upconversion and down conversion emission in different solvents.