TY - JOUR A1 - Wang, Cui A1 - Kitzmann, W.R. A1 - Weigert, Florian A1 - Förster, Ch. A1 - Wang, X. A1 - Heintze, K. A1 - Resch-Genger, Ute T1 - Matrix Effects on Photoluminescence and Oxygen Sensitivity of a Molecular Ruby N2 - The molecular ruby analogue [Cr(ddpd)2]3+ (ddpd=N,N’-dimethyl-N,N’-dipyridine-2-ylpyridine-2,6-diamine) exhibits near infrared (NIR) emission with a high photoluminescence (PL) quantum yield ΦPL of 11 % and a lifetime of 898 μs in deaerated water at room temperature. While ligand-based control of the photophysical properties has received much attention, influences of the counter anions and microenvironment are still underexplored. In this study, the luminescence properties of the molecular ruby were systematically examined for the counter anions Cl−, Br−, [BF4]−, [PF6]−, [BPh4]−, and [BArF24]− in acetonitrile (MeCN) solution, in crystals, and embedded into polystyrene nanoparticles (PSNP). Stern-Volmer analyses of the oxygen quenching studies in the intensity and lifetime domain showed the highest oxygen sensitivity of the complexes with the counter anions of [BF4]− and [BArF24]−, which also revealed the longest luminescence lifetimes. Embedding [Cr(ddpd)2][PF6]3 in PSNPs and shielding with poly(vinyl alcohol) yields a strongly NIR-emissive oxygen-insensitive material with a record ΦPL of 15.2 % under ambient conditions. KW - Fluorescence KW - Sensor KW - Oxygen KW - Quantum yield KW - Quality assurance KW - Complex KW - Cr(III) KW - Lifetime KW - Ligand KW - Solid state KW - X-Ray analysis KW - Structure-property relationship KW - Nano KW - Polymer KW - Particle PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-546057 DO - https://doi.org/10.1002/cptc.202100296 SN - 2367-0932 VL - 6 IS - 6 SP - 1 EP - 9 PB - Wiley-VCH CY - Weinheim AN - OPUS4-54605 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Wang, Z. A1 - Wegner, Karl David A1 - Stiegler, L. M. S. A1 - Zhou, X. A1 - Rezvani, A. A1 - Odungat, A. S. A1 - Zubiri, B. A. A1 - Wu, M. A1 - Spiecker, E. A1 - Walter, J. A1 - Resch-Genger, Ute A1 - Segets, D. T1 - Optimizing the Shelling Process of InP/ZnS Quantum Dots Using a Single-Source Shell Precursor: Implications for Lighting and Display Applications N2 - InP/ZnS core/shell quantum dots (QDs), recognized as highly promising heavy-metal-free emitters, are increasingly being utilized in lighting and display applications. Their synthesis in a tubular flow reactor enables production in a highly efficient, scalable, and reproducible manner, particularly when combined with a single-source shell precursor, such as zinc diethyldithiocarbamate (Zn(S2CNEt2)2). However, the photoluminescence quantum yield (PLQY) of QDs synthesized with this route remains significantly lower compared with those synthesized in batch reactors involving multiple steps for the shell growth. Our study identifies the formation of absorbing, yet nonemissive ZnS nanoparticles during the ZnS shell formation process as a main contributing factor to this discrepancy. By varying the shelling conditions, especially the shelling reaction temperature and InP core concentration, we investigated the formation of pure ZnS nanoparticles and their impact on the optical properties, particularly PLQY, of the resultant InP/ZnS QDs through ultraviolet−visible (UV−vis) absorption, steady-state and time-resolved photoluminescence (PL) spectroscopy, scanning transmission electron microscopy (STEM), and analytical ultracentrifugation (AUC) measurements. Our results suggest that process conditions, such as lower shelling temperatures or reduced InP core concentrations (resulting in a lower external surface area), encourage homogeneous nucleation of ZnS. This reduces the availability of shell precursors necessary for effective passivation of the InP core surfaces, ultimately resulting in lower PLQYs. These findings explain the origin of persistently underperforming PLQY of InP/ZnS QDs synthesized from this synthesis route and suggest further optimization strategies to improve their emission for lighting and display applications. KW - Nano KW - Particle KW - Synthesis KW - InP KW - Shell KW - Fluorescence KW - Quantum yield KW - ZnS KW - Semiconductor KW - Quantum dot KW - Flow reactor KW - Method KW - AUC KW - Size KW - Automation KW - Sensor PY - 2024 DO - https://doi.org/10.1021/acsanm.4c05265 SN - 2574-0970 VL - 7 IS - 20 SP - 24262 EP - 24273 PB - ACS Publications AN - OPUS4-61518 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Meng, M. A1 - Zhang, T. A1 - Wang, J. A1 - Cheng, Z. A1 - Liu, Y. A1 - Qiao, X. A1 - Wen, J. A1 - Resch-Genger, Ute A1 - Long, W. A1 - Ou, J. T1 - NaYF4:Yb3+/Tm3+@NaYF4:Yb3+ Upconversion Nanoparticles for Optical Temperature Monitoring and Self-Heating in Photothermal Therapy N2 - The core−shell NaYF4:Yb3+/Tm3+@NaYF4:Yb3+ upconversion nanoparticles were successfully prepared by a solvothermal method, and a layer of mesoporous silica (mSiO2) was successfully coated on the periphery of the core−shell nanoparticles to transform their surface from lipophilic to hydrophilic, further expanding their applications in biological tissues. The physical phase, morphology, structure, and fluorescence properties were characterized by X-ray diffraction (XRD), field emission transmission electron microscopy (TEM), Fourier infrared spectroscopy (FT-IR), ζ potential analysis, and fluorescence spectroscopy. It was found that the material has a hexagonal structure with good hydrophilicity and emits intense fluorescence under 980 nm pump laser excitation. The non-contact temperature sensing performance of nanoparticles was evaluated by analyzing the upconversion fluorescence of Tm3+ (1G4 → 3F4 and 3F3 → 3H6) in the temperature range of 284−344 K. The absolute and relative sensitivities were found to be 0.0067 K−1 and 1.08 % K−1, respectively, with high-temperature measurement reliability and good temperature cycling performance. More importantly, its temperature measurement in phosphate-buffered saline (PBS) solution is accurate. In addition, the temperature of the cells can be increased by adjusting the laser power density and laser irradiation time. Therefore, an optical temperature sensing platform was built to realize the application of real-time monitoring of cancer cell temperature and the dual function of photothermal therapy. KW - Sensor KW - Temperature KW - Lanthanide KW - Tag KW - Fluorescence KW - Nanoparticles KW - Synthesis KW - Environment KW - Monitoring KW - Sensing KW - Nano KW - Life sciences KW - Upconversion PY - 2023 DO - https://doi.org/10.1021/acsanm.2c05110 VL - 6 IS - 1 SP - 759 EP - 771 PB - ACS Publications AN - OPUS4-57081 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Meng, M. A1 - Zhang, T. A1 - Wang, J. A1 - Cheng, Z. A1 - Yang, J. A1 - Qiao, X. A1 - Wen, J. A1 - Resch-Genger, Ute A1 - Ou, J. T1 - Fluorescence temperature sensing of NaYF4:Yb3+/Tm3+@NaGdF4:Nd3+/Yb3+ nanoparticles at low and high temperatures N2 - NaYF4:Yb3+/Tm3+@NaGdF4:Nd3+/Yb3+ upconversion nanoparticles (UCNPs) were prepared using a solvothermal method, and the effects of key factors such as the content of sensitiser Nd 3+ and Yb3+ on their luminescence properties were investigated. The nanoparticles are homogeneous in size and well dispersed. Under 808 nm excitation, it can produce strong upconversion fluorescence. At the same time, the nanoparticles have good temperature-sensing properties at the thermally coupled energy levels of 700 nm and 646 nm for Tm3+. Using its fluorescence intensity ratio (FIR), accurate temperature measurements can be performed, and it has been found that it exhibits different temperature sensing properties in low and high-temperature regions. The maximum relative sensitivity was found to be 0.88% K-1 and 1.89% K-1 for the lowtemperature region of 285 K-345 K and the high-temperature region of 345 K-495 K. The nanoparticles were applied to the internal temperature measurement of lithium batteries and the actual high-temperature environment, respectively, and were found to have good temperature measurementt performance. KW - Fluorescence KW - Sensor KW - Temperature KW - Ratiometric KW - Lanthanide KW - Quantum yield KW - Integrating sphere spectroscopy KW - Absolute fluorescence KW - Quality assurance KW - Nano KW - Particle KW - Application KW - Upconversion nanoparticle PY - 2022 DO - https://doi.org/10.1088/1361-6528/ac84e4 SN - 1361-6528 VL - 33 IS - 34 SP - 1 EP - 15 PB - IOP Publishing CY - Bristol AN - OPUS4-55454 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -