首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
Multifunctional NaGdF4:Yb3+,Er3+,Nd3+@NaGdF4:Nd3+ core–shell nanoparticles (called Gd:Yb3+,Er3+,Nd3+@Gd:Nd3+ NPs) with simultaneously enhanced near‐infrared (NIR)‐visible (Vis) and NIR‐NIR dual‐conversion (up and down) luminescence (UCL/DCL) properties were successfully synthesized. The resulting core–shell NPs simultaneously emitted enhanced UCL at 522, 540, and 660 nm and DCL at 980 and 1060 nm under the excitation of a 793 nm laser. The enhanced UCL and DCL can be explained by complex energy‐transfer processes, Nd3+→Yb3+→Er3+ and Nd3+→Yb3+, respectively. The effects of Nd3+ concentration and shell thickness on the UCL/DCL properties were systematically investigated. The UCL and DCL properties of NPs were observed under the optimal conditions: a shell Nd3+ content of 20 % and a shell thickness of approximately 5 nm. Moreover, the Gd:Yb3+,Er3+,Nd3+@Gd:20 % Nd3+ NPs exhibited remarkable magnetic resonance imaging (MRI) properties similar to that of a clinical agent, Omniscan. Thus, the core–shell NPs with excellent UCL/DCL/magnetic resonance imaging (MRI) properties have great potential for both in vitro and in vivo multimodal bioimaging.  相似文献   

2.
A family of monodisperse YF3, YF3:Ce3+ and YF3:Ce3+/Ln3+ (Ln=Tb, Eu) mesocrystals with a morphology of a hollow spindle can be synthesized by a solvothermal process using yttrium nitrate and NH4F as precursors. The effects of reaction time, fluorine source, solvents, and reaction temperature on the synthesis of these mesocrystals have been studied in detail. The results demonstrate that the formation of a hollow spindle‐like YF3 can be ascribed to a nonclassical crystallization process by means of a particle‐based reaction route in ethanol. It has been shown that the fluorine sources selected have a remarkable effect on the morphologies and crystalline phases of the final products. Moreover, the luminescent properties of Ln3+‐doped and Ce3+/Ln3+‐co‐doped spindle‐like YF3 mesocrystals were also investigated. It turns out that Ce3+ is an efficient sensitizer for Ln3+ in the spindle‐like YF3 mesocrystals. Remarkable fluorescence enhancement was observed in Ce3+/Ln3+‐co‐doped YF3 mesocrystals. The mechanism of the energy transfer and electronic transition between Ce3+ and Ln3+ in the host material of YF3 mesocrystals was also explored. The cytotoxicity study revealed that these YF3‐based nanocrystals are biocompatible for applications, such as cellular imaging.  相似文献   

3.
A new class of lanthanide‐doped upconversion nanoparticles are presented that are without Yb3+ or Nd3+ sensitizers in the host lattice. In erbium‐enriched core–shell NaErF4:Tm (0.5 mol %)@NaYF4 nanoparticles, a high degree of energy migration between Er3+ ions occurs to suppress the effect of concentration quenching upon surface coating. Unlike the conventional Yb3+‐Er3+ system, the Er3+ ion can serve as both the sensitizer and activator to enable an effective upconversion process. Importantly, an appropriate doping of Tm3+ has been demonstrated to further enhance upconversion luminescence through energy trapping. This endows the resultant nanoparticles with bright red (about 700‐fold enhancement) and near‐infrared luminescence that is achievable under multiple excitation wavelengths. This is a fundamental new pathway to mitigate the concentration quenching effect, thus offering a convenient method for red‐emitting upconversion nanoprobes for biological applications.  相似文献   

4.
Herein, we report the preparation of zeolite NIR luminescence materials with a remarkable increase of luminescence intensity by attaching stopper molecule (an imidazolium salt) to the channel entrances of zeolite L loading with NIR lanthanide (Er3+ or Nd3+) β‐diketonate complexes. This results from the formation of Ln3+β‐diketonate complexes (Ln=Er or Nd) with high coordination numbers through the decreasing of the proton strength in the zeolite channels. The obtained materials were characterized with SEM and photoluminescence spectroscopy. We believe that this hybrid material will be an appealing candidate for the applications of optical fiber, telecommunications and bio‐imaging.  相似文献   

5.
The synthesis of hydrophilic lanthanide‐doped nanocrystals (Ln3+‐NCs) with molecular recognition ability for bioimaging currently remains a challenge. Herein, we present an effective strategy to circumvent this bottleneck by encapsulating Ln3+‐NCs in graphene oxide (NCs@GO). Monodisperse NCs@GO was prepared by optimizing GO size and core–shell structure of NaYF4:Yb,Er@NaYF4, thus combining the intense visible/near‐infrared II (NIR‐II) luminescence of NCs and the unique surface properties and biomedical functions of GO. Such nanostructures not only feature broad solvent dispersibility, efficient cell uptake, and excellent biocompatibility but also enable further modifications with various agents such as DNA, proteins, or nanoparticles without tedious procedures. Moreover, we demonstrate in proof‐of‐concept experiments that NCs@GO can realize simultaneous intracellular tracking and microRNA‐21 visualization, as well as highly sensitive in vivo tumor‐targeted NIR‐II imaging at 1525 nm.  相似文献   

6.
A unique example of discrete molecular entity NdyErxYb3?(x+y)Q9 ( 1 ) (Q=quinolinolato) containing three different lanthanides simultaneously emitting in three different spectral regions in the NIR, ranging from 900 to 1600 nm, has been synthesized and fully chararacterized. A simple molecular strategy based on tuning metal composition in the Ln3Q9 framework, which contains inequivalent central and terminal coordination sites, has allowed a satisfactory ion‐size‐driven control of molecular speciation close to 90 %. In 1 the central position of the larger Nd ion is well distinguished from the terminal ones of the smaller Yb3+ and Er3+, which are almost “vicariants” as found in the heterobimetallic ErxYb3?xQ9 ( 2 ). The Ln3Q9 molecular architecture, which allows communication between the ions, has proved to afford multiple NIR emission in 1 and 2 , and is promising to develop a variety of multifunctional materials through the variation of the Ln composition.  相似文献   

7.
Small (2–28 nm) NaREF4 (rare earth (RE)=Nd–Lu, Y) nanoparticles (NPs) were prepared by an oil/water two‐phase approach. Meanwhile, hydrophilic NPs can be obtained through a successful phase‐transition process by introducing the amphiphilic surfactant sodium dodecylsulfate (SDS) into the same reaction system. Hollow‐structured NaREF4 (RE=Y, Yb, Lu) NPs can be fabricated in situ by electron‐beam lithography on solid NPs. The MTT assay indicates that these hydrophilic NPs with hollow structures exhibit good biocompatibility. The as‐prepared hollow‐structured NPs can be used as anti‐cancer drug carriers for drug storage/release investigations. Doxorubicin hydrochloride (DOX) was taken as model drug. The release of DOX from hollow α‐NaLuF4:20 % Yb3+, 2 % Er3+ exhibits a pH‐sensitive release patterns. Confocal microscopy observations indicate that the NPs can be taken up by HeLa cells and show obvious anti‐cancer efficacy. Furthermore, α‐NaLuF4:20 % Yb3+, 2 % Er3+ NPs show bright‐red emission under IR excitation, making both the excitation and emission light fall within the “optical window” of biological tissues. The application of α‐NaLuF4:20 % Yb3+, 2 % Er3+ in the luminescence imaging of cells was also investigated, which shows a bright‐red emission without background noise.  相似文献   

8.
An intense single‐band blue emission at λ=450 nm is observed from Tm3+ ions through Ce3+ sensitization, for the first time, in colloidal Ce3+/Tm3+‐doped NaYF4 nanocrystals. The intense Tm3+ emission through broad‐band excitation is advantageous for developing luminescent nanocomposites because they can be easily incorporated into polymers. The composites can easily be coated over UV light‐emitting diodes (LEDs) to develop phosphor‐based blue LEDs.  相似文献   

9.
Two heterobimetallic Zn‐Nd phenylene‐bridged Schiff‐base ligands complexes [ZnNd L1 (Py)(NO3)3] ( 1 ) and [Zn L2 Nd(Py)(NO3)3]·MeCN ( 2 ) (Py = pyridine, H2L1 = N,N′‐bis‐ (3‐methoxy‐salicylidene)phenylene‐1,2‐diamine, H2L2 = N,N′‐bis‐5‐bromo‐3‐methoxy‐salicylidene)phenylene‐1,2‐diamine) were obtained. Both 1 and 2 were structurally characterized by X‐ray crystallography, and their near‐infrared (NIR) luminescent properties were determined. For the two complexes, the occupation of pyridine at the axial position of 3d Zn2+ ions could effectively prevent luminescent quenching arising from OH‐, NH‐ or CH oscillators of the solvates around the 4f Nd3+ ions, and the heavy‐atom (Br) effect of the Schiff‐base ligands on their NIR luminescent properties is also discussed.  相似文献   

10.
The design and preparation of luminescent drug carriers has been a prosperous area of research for many years. However, the excitation and/or emission wavelength of such luminescent drug carriers haven′t been optimized in the so‐called human “near infrared (NIR) optical window”, thus restricting their practical applications. Herein, we report the synthesis of electrospun porous YAG:Nd3+ (neodymium‐doped yttrium aluminum garnet) fibers with both excitation and emission in the “NIR optical window” as luminescent drug carriers. The YAG:Nd3+ porous fibers were characterized by SEM, TEM, XRD, scanning transmission electron microscopy–energy‐dispersive X‐ray spectroscopy (STEM‐EDX), and photoluminescence (PL). Ibuprofen (IBU) was used as a model drug to evaluate the drug‐loading capacities and release profiles of the samples. BMSCs (bone mesenchymal stem cells) were used as model human cells to investigate cytotoxicity. Our results indicated that the YAG:Nd3+ fibers possessed a fine, irregularly porous fibrous morphology with an average diameter of 378 nm. The florescence of the sample (1064 nm) could be excited over a wide wavelength range in the NIR region. During the release process of IBU in simulated body fluid (SBF), along with the dissolving of the drug, the solvent entered into the pores, and the emission intensity of the YAG:Nd3+ fibers at 1064 nm decreased gradually, owing to a quenching effect of the hydroxy groups, thus provided an approach to track and monitor drug release. In addition, cytotoxicity investigations revealed that these YAG:Nd3+ fibers were biocompatible with human cells. Consequently, the porous YAG:Nd3+ fibers are a promising material for applications as advanced drug carriers.  相似文献   

11.
Wide-coverage near infrared (NIR) phosphor-converted LEDs possess promising potential for practical applications, but little is developed towards the efficient and wide-coverage NIR phosphors. Here, we report the single-component lanthanide (Ln3+) ions doped Cs2M(In0.95Sb0.05)Cl6 (M=alkali metal) nanocrystals (NCs), exhibiting emission from 850 to 1650 nm with high photoluminescence quantum yield of 20.3 %, which is accomplished by shaping the multiple metal halide octahedra of double perovskite via the simple alkali metal substitution. From Judd-Ofelt theoretical calculation and spectroscopic investigations, the shaping of metal halide octahedra in Cs2M(In1−xSbx)Cl6 NCs can break the forbidden of f-f transition of Ln3+, thus increasing their radiative transition rates and simultaneously boosting the energy transfer efficiency from host to Ln3+. Finally, the wide-coverage NIR LEDs based on Sm3+, Nd3+, Er3+-tridoped Cs2K0.5Rb0.5(In0.95Sb0.05)Cl6 NCs are fabricated and employed in the multiplex gas sensing and night-vision application.  相似文献   

12.
Lanthanide triflates have been used to incorporate NdIII and SmIII ions into the 2.2.2‐cryptand ligand (crypt) to explore their reductive chemistry. The Ln(OTf)3 complexes (Ln=Nd, Sm; OTf=SO3CF3) react with crypt in THF to form the THF‐soluble complexes [LnIII(crypt)(OTf)2][OTf] with two triflates bound to the metal encapsulated in the crypt. Reduction of these LnIII‐in‐crypt complexes using KC8 in THF forms the neutral LnII‐in‐crypt triflate complexes [LnII(crypt)(OTf)2]. DFT calculations on [NdII(crypt)]2+], the first NdII cryptand complex, assign a 4f4 electron configuration to this ion.  相似文献   

13.
A series of upconversion luminescent erbium‐doped SrTiO3 (ABO3‐type) photocatalysts with different initial molar ratios of Sr/Ti have been prepared by a facile polymerized complex method. Er3+ ions, which were gradually transferred from the A to the B site with increasing Sr/Ti, enabled the absorption of visible light and the generation of high‐energy excited states populated by upconversion processes. The local internal fields arising from the dipole moments of the distorted BO6 octahedra promoted energy transfer from the high‐energy excited states of Er3+ with B‐site occupancy to the host SrTiO3 and thus enhanced the band‐to‐band transition of the host SrTiO3. Consequently, the erbium‐doped SrTiO3 species with B‐site occupancy showed higher photocatalytic activity than those with A‐site occupancy for visible‐light‐driven H2 or O2 evolution in the presence of the corresponding sacrificial reagents. The results generally suggest that the introduction of upconversion luminescent agents into host semiconductors is a promising approach to simultaneously harnessing low‐energy photons and maintaining redox ability for photocatalytic H2 and O2 evolution and that the site occupancy of doped elements in ABO3‐type perovskite oxides greatly determines the photocatalytic activity.  相似文献   

14.
We have investigated the self‐assembly of three luminescent species in CH3CN/CH2Cl2, namely: 1) a polylysin dendrimer ( D ) composed of 21 aliphatic amide units and 24 green luminescent dansyl chromophores at the periphery, 2) a molecular clip ( C ) with two blue luminescent anthracene sidewalls and a benzene bridging unit that bears two sulfate groups in the para position, and 3) a near infrared (NIR)‐emitting Nd3+ ion. For purposes of comparison, analogous systems have also been investigated in which Gd3+ replaced Nd3+. The dendrimer and the clip can bind Nd3+ ions with formation of [ D? 2 Nd3+] and [ C? Nd3+] complexes, in which energy transfer from dansyl and, respectively, anthracene to Nd3+ ion takes place with 65 and 8 % efficiency, in air‐equilibrated solution. In the case of [ C? Nd3+], the energy‐transfer efficiency is quenched by dioxygen, thereby showing that the energy donor is the lowest triplet excited state of anthracene. In [ D? 2 Nd3+] the intrinsic emission efficiency of Nd3+ is much higher (ca. 5 times) than in [ C? Nd3+] because of a better protection of the excited lanthanide ion towards nonradiative deactivation caused by interaction with solvent molecules. By mixing solutions of D , Nd3+, and C with proper concentrations, a supramolecular structure with five components of three different species, [ D? 2 Nd3+ ? 2 C ], is formed. The excitation light absorbed by the clips is transferred with 100 % efficiency to the dansyl units of the dendrimer and then to the Nd3+ ions with 65 % efficiency either in the presence or absence of dioxygen. These results show that the [ D? 2 Nd3+ ? 2 C ] complex is able to efficiently harvest UV light by the 24 dansyl units of the dendrimer and the four anthracene chromophores of the two clips, and efficiently transfer it to the encapsulated Nd3+ ions that emit in the NIR spectral region.  相似文献   

15.
Bi3+ and lanthanide ions have been codoped in metal oxides as optical sensitizers and emitters. But such codoping is not known in typical semiconductors such as Si, GaAs, and CdSe. Metal halide perovskite with coordination number 6 provides an opportunity to codope Bi3+ and lanthanide ions. Codoping of Bi3+ and Ln3+ (Ln=Er and Yb) in Cs2AgInCl6 double perovskite is presented. Bi3+‐Er3+ codoped Cs2AgInCl6 shows Er3+ f‐electron emission at 1540 nm (suitable for low‐loss optical communication). Bi3+ codoping decreases the excitation (absorption) energy, such that the samples can be excited with ca. 370 nm light. At that excitation, Bi3+‐Er3+ codoped Cs2AgInCl6 shows ca. 45 times higher emission intensity compared to the Er3+ doped Cs2AgInCl6. Similar results are also observed in Bi3+‐Yb3+ codoped sample emitting at 994 nm. A combination of temperature‐dependent (5.7 K to 423 K) photoluminescence and calculations is used to understand the optical sensitization and emission processes.  相似文献   

16.
Two zwitterionic‐type ligands featuring π–π* and intraligand charge‐transfer (ILCT) excited states, namely 1,1′‐(2,3,5,6‐tetramethyl‐1,4‐phenylene)bis(methylene)dipyridinium‐4‐olate (TMPBPO) and 1‐dodecylpyridin‐4(1 H)‐one (DOPO), have been prepared and applied to the assembly of lanthanide coordination complexes in an effort to understand the ligand‐direction effect on the structure of the Ln complexes and the ligand sensitization effect on the luminescence of the Ln complexes. Due to the wide‐band triplet states plus additional ILCT excitation states extending into lower energy levels, broadly and strongly sensitized photoluminescence of f→f transitions from various Ln3+ ions were observed to cover the visible to near‐infrared (NIR) regions. Among which, the Pr, Sm, Dy, and Tm complexes simultaneously display both strong visible and NIR emissions. Based on the isostructural feature of the Ln complexes, color tuning and single‐component white light was achieved by preparation of solid solutions of the ternary systems Gd‐Eu‐Tb (for TMPBPO) and La‐Eu‐Tb and La‐Dy‐Sm (for DOPO). Moreover, the visible and NIR luminescence lifetimes of the Ln complexes with the TMPBPO ligand were investigated from 77 to 298 K, revealing a strong temperature dependence of the Tm3+ (3H4) and Yb3+ (2F5/2) decay dynamics, which has not been explored before for their coordination complexes.  相似文献   

17.
A crystal design strategy is described that generates hexagonal‐phased NaYF4:Nd/Yb@NaYF4:Yb/Tm luminescent nanocrystals with the ability to emit light at 803 nm when illuminated at 745 nm. This is accomplished by taking advantage of the large absorption cross‐section of Nd3+ between 720 and 760 nm plus efficient spatial energy transfer and migration through Nd3+→Yb3+→Yb3+→Tm3+. Mechanistic investigations suggest that a cascaded two‐photon energy transfer upconversion process underlies the emission mechanism. This protocol enables deep‐tissue imaging to be achieved while mitigating the attenuation effect associated with the visible emission and the overheating constraint imposed by conventional 980 nm excitation.  相似文献   

18.
Lanthanide‐doped upconversion nanoparticles (UCNPs) have shown great promise in bioapplications. Exploring new host materials to realize efficient upconversion luminescence (UCL) output is a goal of general concern. Herein, we develop a unique strategy for the synthesis of novel LiLuF4:Ln3+ core/shell UCNPs with typically high absolute upconversion quantum yields of 5.0 % and 7.6 % for Er3+ and Tm3+, respectively. Based on our customized UCL biodetection system, we demonstrate for the first time the application of LiLuF4:Ln3+ core/shell UCNPs as sensitive UCL bioprobes for the detection of an important disease marker β subunit of human chorionic gonadotropin (β‐hCG) with a detection limit of 3.8 ng mL−1, which is comparable to the β‐hCG level in the serum of normal humans. Furthermore, we use these UCNPs in proof‐of‐concept computed tomography imaging and UCL imaging of cancer cells, thus revealing the great potential of LiLuF4:Ln3+ UCNPs as efficient nano‐bioprobes in disease diagnosis.  相似文献   

19.
The two oxidation states of ceria nanoparticles, Ce3+ and Ce4+, play a pivotal role in scavenging reactive oxygen species (ROS). In particular, Ce3+ is largely responsible for removing O2 and .OH that are associated with inflammatory response and cell death. The synthesis is reported of 2 nm ceria–zirconia nanoparticles (CZ NPs) that possess a higher Ce3+/Ce4+ ratio and faster conversion from Ce4+ to Ce3+ than those exhibited by ceria nanoparticles. The obtained Ce0.7Zr0.3O2 (7CZ) NPs greatly improve ROS scavenging performance, thus regulating inflammatory cells in a very low dose. Moreover, 7CZ NPs are demonstrated to be effective in reducing mortality and systemic inflammation in two representative sepsis models. These findings suggest that 7CZ NPs have the potential as a therapeutic nanomedicine for treating ROS‐related inflammatory diseases.  相似文献   

20.
In order to create near-infrared (NIR) luminescent lanthanide complexes suitable for DNA-interaction, novel lanthanide dppz complexes with general formula [Ln(NO3)3(dppz)2] (Ln = Nd3+, Er3+ and Yb3+; dppz = dipyrido[3,2-a:2′,3′-c]phenazine) were synthesized, characterized and their luminescence properties were investigated. In addition, analogous compounds with other lanthanide ions (Ln = Ce3+, Pr3+, Sm3+, Eu3+, Tb3+, Dy3+, Ho3+, Tm3+, Lu3+) were prepared. All complexes were characterized by IR spectroscopy and elemental analysis. Single-crystal X-ray diffraction analysis of the complexes (Ln = La3+, Ce3+, Pr3+, Nd3+, Eu3+, Er3+, Yb3+, Lu3+) showed that the lanthanide’s first coordination sphere can be described as a bicapped dodecahedron, made up of two bidentate dppz ligands and three bidentate-coordinating nitrate anions. Efficient energy transfer was observed from the dppz ligand to the lanthanide ion (Nd3+, Er3+ and Yb3+), while relatively high luminescence lifetimes were detected for these complexes. In their excitation spectra, the maximum of the strong broad band is located at around 385 nm and this wavelength was further used for excitation of the chosen complexes. In their emission spectra, the following characteristic NIR emission peaks were observed: for a) Nd3+: 4F3/24I9/2 (870.8 nm), 4F3/24I11/2 (1052.7 nm) and 4F3/24I13/2 (1334.5 nm); b) Er3+: 4I13/24I15/2 (1529.0 nm) c) Yb3+: 2F5/22F7/2 (977.6 nm). While its low triplet energy level is ideally suited for efficient sensitization of Nd3+ and Er3+, the dppz ligand is considered not favorable as a sensitizer for most of the visible emitting lanthanide ions, due to its low-lying triplet level, which is too low for the accepting levels of most visible emitting lanthanides. Furthermore, the DNA intercalation ability of the [Nd(NO3)3(dppz)2] complex with calf thymus DNA (CT-DNA) was confirmed using fluorescence spectroscopy.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号