TY - JOUR A1 - Napp, J. A1 - Behnke, Thomas A1 - Fischer, L. A1 - Würth, Christian A1 - Wottawa, M. A1 - Katschinski, D.M. A1 - Alves, F. A1 - Resch-Genger, Ute A1 - Schäferling, M. T1 - Targeted luminescent near-infrared polymer-nanoprobes for in vivo imaging of tumor hypoxia JF - Analytical chemistry N2 - Polystyrene nanoparticles (PS-NPs) were doped with an oxygen-sensitive near-infrared (NIR)-emissive palladium meso-tetraphenylporphyrin and an inert reference dye which are both excitable at 635 nm. The nanosensors were characterized with special emphasis on fundamental parameters such as absolute photoluminescence quantum yield and fluorescence lifetime. The PS-NPs were employed for ratiometric dual-wavelength and lifetime-based photoluminescent oxygen sensing. They were efficiently taken up by cultured murine alveolar macrophages, yielding a characteristic and reversible change in ratiometric response with decreasing oxygen concentration. This correlated with the cellular hypoxic status verified by analysis of hypoxia inducible factor-1α (HIF-1α) accumulation. In addition, the surface of PS-NPs was functionalized with polyethylene glycol (PEG) and the monoclonal antibody herceptin, and their binding to HER2/neu-overexpressing tumor cells was confirmed in vitro. First experiments with tumor-bearing mouse revealed a distinctive ratiometric response within the tumor upon hypoxic condition induced by animal sacrifice. These results demonstrate the potential of these referenced NIR nanosensors for in vitro and in vivo imaging that present a new generation of optical probes for oncology. KW - Fluorescence KW - NIR KW - Nanoparticles KW - Microparticles KW - Imaging KW - Cancer KW - Oxygene PY - 2011 DO - https://doi.org/10.1021/ac201870b SN - 0003-2700 SN - 1520-6882 VL - 83 IS - 23 SP - 9039 EP - 9046 PB - American Chemical Society CY - Washington, DC AN - OPUS4-24987 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Natte, Kishore A1 - Behnke, Thomas A1 - Orts Gil, Guillermo A1 - Würth, Christian A1 - Friedrich, Jörg Florian A1 - Österle, Werner A1 - Resch-Genger, Ute T1 - Synthesis and characterisation of highly fluorescent core-shell nanoparticles based on Alexa dyes JF - Journal of nanoparticle research N2 - Current and future developments in the emerging field of nanobiotechnology are closely linked to the rational design of novel fluorescent nanomaterials, e.g. for biosensing and imaging applications. Here, the synthesis of bright near infrared (NIR)-emissive nanoparticles based on the grafting of silica nanoparticles (SNPs) with 3-aminopropyl triethoxysilane (APTES) followed by covalent attachment of Alexa dyes and their subsequent shielding by an additional silica shell are presented. These nanoparticles were investigated by dynamic light scattering (DLS), transmission electron microscopy (TEM) and fluorescence spectroscopy. TEM studies revealed the monodispersity of the initially prepared and fluorophorelabelled silica particles and the subsequent formation of raspberry-like structures after addition of a silica precursor.Measurements of absolute fluorescence quantum yields of these scattering particle suspensions with an integrating sphere setup demonstrated the influence of dye labelling density-dependent fluorophore aggregation on the signaling behaviour of such nanoparticles. KW - Silica KW - Alexa dyes KW - Fluorescent particles KW - Quantum yields KW - Nanoparticles KW - Protective shell KW - Nanobiotechnology PY - 2012 DO - https://doi.org/10.1007/s11051-011-0680-9 SN - 1388-0764 SN - 1572-896X VL - 14 IS - 2 SP - 680-1 - 680-10 PB - Kluwer CY - Dordrecht AN - OPUS4-25872 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Würth, Christian A1 - Manley, P. A1 - Voigt, R. A1 - Ahiboz, D. A1 - Becker, C. A1 - Resch-Genger, Ute T1 - Metasurface Enhanced Sensitized Photon Upconversion: Toward Highly Efficient Low Power Upconversion Applications and Nanoscale E-Field Sensors JF - Nano Letters N2 - Large-scale nanoimprinted metasurfaces based on silicon photonic crystal slabs were produced and coated with a NaYF4:Yb3+/Er3+ upconversion nanoparticle (UCNP) layer. UCNPs on these metasurfaces yield a more than 500-fold enhanced upconversion emission compared to UCNPs on planar surfaces. It is also demonstrated how the optical response of the UCNPs can be used to estimate the local field energy in the coating layer. Optical simulations using the finite element method validate the experimental results and the calculated spatial three-dimensional field Energy distribution helps us to understand the emission enhancement mechanism of the UCNPs closely attached to the metasurface. In addition, we analyzed the spectral shifts of the resonances for uncoated and coated metasurfaces and metasurfaces submerged in water to enable a prediction of the optimum layer thicknesses for different excitation wavelengths, paving the way to applications such as electromagnetic field sensors or bioassays. KW - Nanoparticles KW - Upconversion KW - Metasurface KW - Field sensor KW - Emission enhancement KW - Photonic crystal PY - 2020 DO - https://doi.org/10.1021/acs.nanolett.0c02548 VL - 20 IS - 9 SP - 6682 EP - 6689 PB - ACS Publications AN - OPUS4-51427 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kaiser, M. A1 - Würth, Christian A1 - Kraft, Marco A1 - Hyppänen, I. A1 - Soukka, T. A1 - Resch-Genger, Ute T1 - Power-dependent upconversion quantum yield of NaYF4:Yb3+,Er3+ nano- and micrometer-sized particles – measurements and simulations JF - Nanoscale N2 - Photophysical studies of nonlinear lanthanide-doped photon upconverting nanoparticles (UCNPs) increasingly used in biophotonics and photovoltaics require absolute measurements of the excitation power density (P)-dependent upconversion luminescence (UCL) and luminescence quantum yields (ΦUC) for quantifying the material performance, UCL deactivation pathways, and possible enhancement factors. We present here the P-dependence of the UCL spectra, ΦUC, and slope factors of the different emission bands of representative 25 nm-sized oleate-capped β-NaYF4:17% Yb3+, 3% Er3+ UCNPs dispersed in toluene and as powder as well as ΦUC of 3 μm-sized upconversion particles (UCμP), all measured with a newly designed integrating sphere setup, enabling controlled variation of P over four orders of magnitude. This includes quantifying the influence of the beam shape on the measured ΦUC and comparison of experimental ΦUC with simulations utilizing the balancing power density model of the Andersson-Engels group and the simulated ΦUC of UCμP from the Berry group, underpinned by closely matching decay kinetics of our UC material. We obtained a maximum ΦUC of 10.5% for UCμP and a ΦUC of 0.6% and 2.1% for solid and dispersed UCNPs, respectively. Our results suggest an overestimation of the contribution of the purple and an underestimation of that of the red emission of β-NaYF4:Yb3+,Er3+: microparticles by the simulations of the Berry group. Moreover, our measurements can be used as a guideline to the absolute determination of UCL and ΦUC KW - Upconversion KW - Photophysics KW - Nanoparticles PY - 2017 DO - https://doi.org/10.1039/c7nr02449e VL - 9 IS - 28 SP - 10051 EP - 10058 PB - The Royal Society of Chemistry AN - OPUS4-41550 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Behnke, Thomas A1 - Würth, Christian A1 - Hoffmann, Katrin A1 - Hübner, Martin A1 - Panne, Ulrich A1 - Resch-Genger, Ute T1 - Encapsulation of hydrophobic dyes in polystyrene micro- and nanoparticles via swelling procedures JF - Journal of fluorescence N2 - Aiming at the derivation of a generalized procedure for the straightforward preparation of particles fluorescing in the visible and near-infrared (NIR) spectral region, different swelling procedures for the loading of the hydrophobic polarity-probe Nile Red into nano- and micrometer sized polystyrene particles were studied and compared with respect to the optical properties of the resulting particles. The effect of the amount of incorporated dye on the spectroscopic properties of the particles was investigated for differently sized beads with different surface chemistries, i.e., non-functionalized, aminomodified and PEG-grafted surfaces. Moreover, photostability and leaking studies were performed. The main criterion for the optimization of the dye loading procedures was a high and thermally and photochemically stable fluorescence output of the particles for the future application of these systems as fluorescent labels. KW - Fluorescence KW - Nile red KW - Polystyrene KW - Nanoparticles KW - Microparticles KW - Encapsulation KW - Swelling PY - 2011 DO - https://doi.org/10.1007/s10895-010-0632-2 SN - 1053-0509 SN - 1573-4994 VL - 21 IS - 3 SP - 937 EP - 944 PB - Plenum Publ. Corp. CY - New York, NY AN - OPUS4-22692 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Meng, M. A1 - Zhang, R. A1 - Zhenlong, F. A1 - Yang, J. A1 - Ansari, A. A1 - Ou, Jun A1 - Würth, Christian A1 - Resch-Genger, Ute T1 - Retracted article: Effect of Ca2+ doping on the upconversion luminescence properties of NaYF4:Yb3+/Tm3+ nanoparticles and study of its temperature measurement performance JF - CrystEngComm N2 - A solvothermal method was used to prepare a series of Yb3+/Tm3+/Ca2+ co-doped NaYF4 nanoparticles with different Ca2+ contents. Strong upconversion blue fluorescence could be observed under 980 nm laser excitation of the samples. The effect of different Ca2+ contents on the luminescence intensity was investigated, and it was found that the UV-vis upconversion luminescence increased and then decreased with an increasing Ca2+ concentration during the increase of the Ca2+ content from 0 mol% to 25 mol%, reaching the strongest fluorescence at 15 mol%, which was up to about 28 times stronger than that without Ca2+ doping. Furthermore, the mechanism was investigated, and it was found that the doping of Ca2+ disrupted the symmetry of the crystal field, resulting in a significant enhancement of the overall fluorescence. Applied to fluorescence intensity ratio thermometry, the absolute and relative sensitivities are as high as 0.0418 K−1 and 2.31% K−1, respectively, with a minimum temperature resolution of 0.0129 K. KW - Sensor KW - Temperature KW - Lanthanide KW - Luminescence KW - Nanoparticles KW - Upconversion KW - Advanced materials PY - 2022 DO - https://doi.org/10.1039/D2CE00562J SN - 1466-8033 VL - 24 IS - 27 SP - 4887 EP - 4898 PB - Royal Society of Chemistry CY - London AN - OPUS4-56952 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -