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Simultaneous enhancement of red upconversion luminescence and CT contrast of NaGdF <sub/>4</sub> :Yb,Er nanoparticles <i>via</i> Lu <sup>3+</sup> doping
摘要： To date, lanthanide-doped upconversion nanoparticles (UCNPs) have been widely reported as a promising CT contrast agent because they have high atomic numbers and big X-ray attenuation coefficient values. However, it is still a challenge to fabricate a simple multimodal imaging probe with improved image quality for early cancer diagnosis in clinical medicine. Herein, ultra-small, uniform and monodisperse β-NaGdF4:Yb,Er,X% Lu (X = 0, 1, 2.5, 4, 6, 7.5) UCNPs were prepared through a solvothermal method with high-level modulation of both the phase and morphology. Meanwhile, a remarkably enhanced red upconversion luminescence (UCL) in the β-NaGdF4:Yb,Er,X% Lu NPs was successfully realized via Lu3+ doping. It is found that as the content of Lu3+ increases from 0 to 7.5 mol%, the UCL intensity of the red emission first increases and then decreases, with the optimum doping content of Lu3+ ions of 2.5 mol%. The red UCL enhancement is ascribed to the change of the Yb–Er interionic distance controlling the Yb–Er energy transfer rate and the distortion of the local environment of Er3+ ions influencing the 4f–4f transition rates of Er3+ ions, which has been further confirmed by the experimental check of the crystallographic phase and by photoluminescence spectroscopy employing Eu3+ as the structural probe, respectively. More importantly, after being modified with the HS-PEG2000-NH2 ligand, the NH2-PEGylated-NaGdF4:Yb,Er,X% Lu NPs exhibited low cytotoxicity, high biocompatibility, and remarkably enhanced contrast performance in in vitro UCL and in vivo CT imaging. On the basis of our findings, the as-obtained functionalized UCNPs could be considered as a promising versatile dual-mode imaging probe for bioimaging, tumor diagnosis, and cancer therapy.
关键词： red luminescence enhancement,Lu3+ doping,upconversion nanoparticles,multimodal imaging,CT contrast
更新于2025-11-14 17:04:02
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A fluorescent probe for sequential sensing of MnO <sub/>4</sub><sup>?</sup> and Cr <sub/>2</sub> O <sub/>7</sub><sup>2?</sup> ions in aqueous medium based on a UCNS/TMB nanosystem
摘要： This paper reports the successful design of an UC fluorescence nanosystem for distinguishable and sequential detection of MnO4? and Cr2O72? based on the inner filter effect (IFE) between Gd2O3:Yb,Er upconversion nanospheres (UCNS) and 3,3’,5,5’-tetramethylbenzidine (TMB). The detection of MnO4? was realized by a stoichiometric oxidation reaction between TMB and Mn(VII), which resulted in quenching of the upconversion luminescence (UCL) by the blue product through IFE. The assay of Cr2O72?, in contrast, was based on the formation of complexes and the consumption of the oxidation product of the previous reaction. The sensing of MnO4? and Cr2O72? do not interfere with each other when Pb2+ was added as a masking agent. This provides a new strategy for sensitive and selective detection of MnO4? and Cr2O72?. The detection of MnO4? showed not only a low LOD of 0.243 μM but also high selectivity over other possible interfering ions. The sensitivity assay of MnO4? can be performed in the linear range of 1.85 to 69 μM. An excellent linear relationship was also found in the sensing of Cr2O72?, with a linear range of 18.3 to 250 μM and a LOD of 2.95 μM. The selectivity towards Cr2O72? was also proved to be good. Based on these properties, the UCNS–TMB nanoplatform is a potential chemosensor for both MnO4? and Cr2O72? ions in practical assays for waste water.
关键词： upconversion nanospheres,aqueous medium,UCNS/TMB nanosystem,Cr2O72?,MnO4?,TMB,fluorescent probe,inner filter effect,sequential sensing
更新于2025-11-14 17:03:37
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Role of Yb3+ ion on the evaluation of energy transfer and cross-relaxation processes in Gd2Ce2O7: Yb3+, Er3+ phosphors
摘要： Energy transfer (ET) and cross-relaxation (CR) processes play significant roles in regulating emitting colors and intensity of upconversion (UC) materials. Calculating the coefficients in ET and CR processes can provide visual descriptions for evaluating the UC luminescence properties. Here, we find that those ET and CR processes are responsible for the color-tunable properties in Gd2Ce2O7: Yb3+, Er3+ phosphors. By solving the rate equation, mathematical expressions are established to calculate the ET and CR coefficients based on the experimental UC spectra and lifetimes. The results are benefit to evaluate the efficiencies of ET and CR processes in quantization in different Yb3+ ion concentrations doped samples. The coefficients of ET process arise from 1.05 to 7.93 × 1017 cm3s?1 while those of CR process increase from 2.69 to 72.01 × 1017 cm3s?1 with increasing the Yb3+ ion concentration, which suggest that the CR and ET processes are efficient in Gd2Ce2O7 host. Furthermore, potential temperature sensing properties are also evaluated according to the fluorescence intensity ratio of 2H11/2 and 4S3/2 levels and the maximal sensitivity (S) is achieved about 0.00337 K?1 at 503 K. This work provides an insight into the evaluation of those UC processes and reveals the capacity in color-tunable and temperature sensing aspects.
关键词： Upconversion,Mathematical expression,Cross-relaxation,Temperature sensing,Energy transfer
更新于2025-11-14 17:03:37
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Improved negative thermal quenching effect via high sensitizer doping content in NaGdF4 based active-core/active-shell architecture
摘要： The strategies of introducing interior defects and reducing mean particle size have been applied to improve negative thermal quenching effect (TQE) in Yb3+ sensitized fluoride upconversion (UC) nanocrystals (NCs) recently. Herein, an active-core/active-shell structure with high total Yb3+ doping content is used to enhance the absorption intensity of Er3+ ions. Moreover, the Er3+ activators are doped into the shell to enable the energy migration process from activators to surface defects. In this scenario, with the rise of temperature, the suppression degree of this energy migration process is enlarged followed by an improved negative TQE. Specifically, with rising the temperature from 293 K to 413 K, the integral upconversion emission intensity of 40Yb: NaGdF4@60Yb/2Er: NaGdF4 NCs increases by ~ 8.24 times, while that of NaGdF4@20Yb/2Er: NaGdF4 NCs with a similar mean particle size only enhances ~ 3.44 times.
关键词： Yb3+ concentration,upconversion,temperature sensing,negative thermal quenching
更新于2025-11-14 17:03:37
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Reversible luminescence modulation and temperature sensing properties of Pr <sup>3+</sup> /Yb <sup>3+</sup> codoped K <sub/>0.5</sub> Na <sub/>0.5</sub> NbO <sub/>3</sub> ceramics
摘要： In this work, we have prepared a novel (K0.5Na0.5)0.99-xPrxYb0.01NbO3 (abbreviated as KNN:xPr3+/0.01Yb3+, x=0.0006, 0.0008, 0.001, 0.002, 0.003 and 0.004) ceramic, which possess visible UC emissions, photochromic (PC) and optical thermometric properties. Under the excitation of a 980-nm diode laser, all the samples show the featured emissions of Pr3+ ions and the UC emission intensity is greatly dependent on the Pr3+ doping content. The optimal UC luminescence intensity is obtained at x=0.001. All the prepared samples show a strong PC reaction, and a large luminescence quenching degree (ΔRt) of 74.94% is found. The optical thermometric properties of both the irradiated and unirradiated KNN:0.001Pr3+/0.01Yb3+ ceramics in the temperature range of 123-573 K have been investigated via measuring the temperature-dependent UC emission spectra of green emissions, which originate from the two 3P1 and 3P0 thermally coupled levels. It has been found that the prepared samples have both excellent PC behaviors and temperature sensing performances. These results suggest that the KNN:xPr3+/0.01Yb3+ ceramics are promising candidates for the applications in PC reaction and thermometers.
关键词： Ferroelectrics,Thermometer,Upconversion,Rare-earth ions,Photochromism
更新于2025-11-14 15:28:36
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Near-infrared-light-triggered photoelectrochemical biosensor for detection of alpha-fetoprotein based on upconversion nanophosphors
摘要： A novel photoelectrochemical (PEC) biosensor based on hybrids of NaYF4:Yb, Tm， zinc oxide (ZnO) and cadmium sulfide (CdS) was constructed to detect alpha-fetoprotein (AFP), which possesses the advantages of low background noise and non-damage to the biological substance. Herein, we prepared NaYF4:Yb,Tm/ZnO/CdS composite film electrode by pulsed laser deposition. The selected materials of ZnO and CdS can make full use of the upconversion luminescence (~360nm, ~480nm) of NaYF4:Yb,Tm nanophosphors under 980nm laser excitation. Meanwhile, an effective matching of energy levels between the conduction bands of CdS and ZnO can prompt photoelectrochemical performance of the electrode. The biosensor shows ultrasensitive detection of AFP with a wide linear range from 0.01 ng mL-1 to 200 ng mL-1 and a low detection limit of 5 pg mL-1. Therefore, the proposed PEC biosensor based on upconversion nanophosphors is potentially attractive for achieving excellent photoelectrochemical biosensor for detection of other cancer markers in clinical analysis.
关键词： photoelectrochemical,pulsed laser deposition,upconversion luminescence,near-infrared light-triggered biosensor
更新于2025-11-14 15:27:09
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Photo-physical properties of substituted 2,3-distyryl indoles: Spectroscopic, computational and biological insights
摘要： The structural dependence of the photo-physical properties of substituted 2,3-distyryl (23DSI) indoles were studied using several spectroscopic techniques including steady-state UV-VIS spectroscopy, steady-state fluorescence spectroscopy, steady-state excitation spectroscopy, time correlated single photon counting (TCSPC) spectroscopy, and time-resolved fluorescence upconversion spectroscopy (TRFLS). Each of 23DSI derivatives investigated showed distinct fluorescence emission and UV-VIS spectra, indicating strong structural dependence of the emission and the excitation. The UV-VIS spectra of the 23DSI derivatives showed three main identical absorption bands with minor deviations in the absorbance caused by substituent groups on the distyryl rings. The time-resolved fluorescence up-conversion studies indicated that the fluorescence undergoes a mono-exponential decay whereas the calculated fluorescence lifetime showed relatively short fluorescence lifetimes of approximately 1 ns. All of the 23DSI derivatives showed two-photon absorption upon direct excitation of 1.6 W laser pulses at 800 nm. These studies suggest that the substituents, attached to distyryl core, are capable of boosting or hindering fluorescence intensities by distorting the π-conjugation of the 23DSI molecule. Our studies showed that 23DSI (p-F) has the highest fluorescence emission quantum yield. Theoretical calculations for the ground state of 23DSI derivatives confirmed differences in electron densities in 23DSI derivatives in the presence of different substituent attachments. The excellent fluorescence emission, high fluorescence quantum yield and two-photon absorption properties of these 23DSI molecules make them attractive candidates for potential applications in the fields of biological imaging, biomedicine, fluorescent probes, and photodynamic inactivation (PDI). B. subtilis samples, treated with micro molar solutions of 23DSI (p-OCH3) and 23DSI (p-CH3), showed very effective photodynamic inactivation (PDI) upon irradiation with white light.
关键词： Two photon absorption,Time-resolved fluorescence upconversion laser spectroscopy,Photodynamic inactivation,Gaussian calculations,Photo-physical properties,Light-activation
更新于2025-11-14 15:26:12
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Upconversion fluorescent nanoparticles based-sensor array for discrimination of the same variety red grape wines
摘要： In this research, a novel fluorescent sensor array based on upconversion nanomaterials (UCNPs) for the discrimination of the same variety red grape wines from different manufacturers was developed. The sensor array was composed of six elements: one positively charged UCNPs modified with guanidine groups (UCNPs@GDN), two negatively charged UCNPs modified with sulfonic acid groups (UCNPs@SO3H) and phosphonic acid groups (UCNPs@PO(OH)2), respectively, and their mixture 1 (UCNPs@GDN + UCNPs@SO3H), mixture 2 (UCNPs@GDN + UCNPs@PO(OH)2) and mixture 3 {UCNPs@GDN + UCNPs@SO3H + UCNPs@PO(OH)2}. The discrimination mechanism is mainly attributed to the emission of those upconversion fluorescent nanoparticles being quenched by organic ingredients that usually exist in red grape wines. The discrimination of red grape wines was carried out by employing UCNPs@GDN, UCNPs@SO3H and UCNPs@PO(OH)2 in pH = 7.0 HEPES buffer, the mixture 1 and mixture 2 in pH = 9.0 PBS buffer, and mixture 3 in pH = 6.0 Tris–HCl buffer. Principal component analysis (PCA) of the data obtained from our established array showed obvious distinction among the nine red grape wines from different manufacturers. The present work is expected to inspire more marvellous research in the fields of UCNPs and red grape wines identification.
关键词： red grape wines,fluorescence quenching,sensor array,upconversion nanoparticles,discrimination
更新于2025-11-14 15:18:02
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Large enhancement in upconverted green emission intensity from Ho3+/Yb3+ co-doped Y2Ti2O7 phosphor in the presence of Zn2+
摘要： The Ho3+, Yb3+ co-doped Y2Ti2O7 phosphor samples have been synthesized through solid state reaction method in the absence and presence of Zn2+ ions. The X-ray diffraction (XRD) analysis show that the phase of the crystal is face centered cubic. The zinc free phosphor shows weak upconversion emission in green region due to 5S2, 5F4 →5I8 transition of Ho3+ ion on excitation with 980 nm radiation. The emission intensity is enhanced significantly in the presence of Zn2+ ions due to increase in crystallinity, particle size and asymmetry in the crystal field. We are reporting ~92 times enhancement in the green emission intensity for 30 mol% co-doping of Zn2+ ions. The lifetime of 5S2 level of Ho3+ ion increases by increasing the concentration of Zn2+ ions. The intense green emission in this material may be suitable for display and other fluorescence based devices.
关键词： Upconversion,Y2Ti2O7 phosphor,Zn2+,Green emission,Ho3+ /Yb3+
更新于2025-11-14 14:48:53
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Remarkable laser-driven upconverting photothermal effect of Cs3LnF6@glass nanocomposites for anti-counterfeiting
摘要： Currently, advanced security strategies have aroused widely interest in anti-counterfeiting field to ensure the authentic items difficult to be replicated. Herein, cubic Cs3LnF6 (Ln = Y, Yb, Lu, Sc) nanocrystals embedded glasses are successfully prepared via an in-situ glass crystallization strategy. Emitting centers, such as Eu3+, Er3+, Ho3+ and Tm3+, can be incorporated into the precipitated Cs3YF6, Cs3YbF6 and Cs3LuF6 crystal lattices but remain in glass matrix rather than in Cs3ScF6 crystals for large ionic radius mismatch between lanthanide activators and Sc3+ host ions. It is demonstrated that upconverting quantum yields of all the Yb/Er: Cs3LnF6@glass samples are higher than those of well-known cubic/hexagonal Yb/Er: α/β-NaYF4@glass samples. Specifically, Yb/Er: Cs3LuF6@glass exhibits a maximal quantum yield of ~0.30%, which is superior to Yb/Er: β-NaYF4 @glass (~0.19%). Impressively, Er: Cs3YbF6@glass shows a remarkable 980 nm laser-induced photothermal effect, leading to significant alteration of upconversion emissive color from red to green with increase of incident laser power. As a prototype of the concept for practical application, a series of luminescent patterns using Er: Cs3YbF6@glass upconverting inks are constructed by a screen-printing technique and show distinct laser-power-sensitive emissive colors, being feasible for high-level anti-counterfeiting. The present work exploits a new anti-counterfeiting strategy by developing highly efficient laser-induced upconverting photothermal materials.
关键词： Anticounterfeit,Nanocomposites,Upconversion,Lanthanide ions,Photothermal effect,Luminescent glasses
更新于2025-10-22 19:38:57