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Multicolor upconversion (UC) luminescence of NaYF4:Yb3+/Er3+ nanoparticles (NPs) was successfully tuned by simply controlling the NaF dosage. Unlike UC nanocrystals previously reported in the literature with multicolor emission obtained by varying the rare‐earth dopants, the current work developed a new approach to tune the UC emission color by controlling the NaF concentration without changing the ratio and dosage of rare‐earth ions. TEM and powder XRD were used to characterize the shape, size, and composition of the UC luminescent nanocrystals. The luminescence images, emission spectra, and multicolor emission mechanism of the NPs have also been demonstrated. As a result of the excellent ability of this new method to manipulate color emission, this will open up new avenues in the areas of bioprobes, light‐emitting devices, color displays, lasers, and so forth. To demonstrate their biological applications, the water‐stable, biocompatible, and bioconjugatable NaYF4:Yb3+/Er3+@poly(acrylic acid) NPs were synthesized by this developed strategy and applied in targeted‐cell UC luminescence imaging. 相似文献
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Tuning the Upconversion Luminescence Lifetimes of KYb2F7:Ho3+ Nanocrystals for Optical Multiplexing 下载免费PDF全文
Dr. Mingye Ding Prof. Daqin Chen Danyang Ma Peng Liu Dr. Kaixin Song Dr. Hongwei Lu Prof. Zhenguo Ji 《Chemphyschem》2015,16(18):3784-3789
Conventional luminescent color coding is limited by spectral overlap and the interference of background fluorescence, thus restricting the number of distinguishable identities that can be used in practice. Here, we demonstrate the possibility of generating diverse time‐domain codes, specially designed for a single emission band, using lanthanide‐doped upconversion nanocrystals. Based on the knowledge of concentration quenching, the upconversion luminescence kinetics of KYb2F7: Ho3+ nanocrystals can be precisely controlled by modifying the dopant concentration of Ho3+ ions, resulting in a tunable emission lifetime from 75.8 to 1944.5 μs, which suggests the practicality of these time‐domain codes for optical multiplexing. 相似文献
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Ln12‐Containing 60‐Tungstogermanates: Synthesis,Structure, Luminescence,and Magnetic Studies 下载免费PDF全文
Kai‐Yao Wang Dr. Bassem S. Bassil Dr. Zhengguo Lin Isabella Römer Stef Vanhaecht Prof. Tatjana N. Parac‐Vogt Dr. Cristina Sáenz de Pipaón Prof. José Ramón Galán‐Mascarós Linyuan Fan Prof. Jie Cao Prof. Ulrich Kortz 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(50):18168-18176
A new class of hexameric Ln12‐containing 60‐tungstogermanates, [Na(H2O)6?Eu12(OH)12(H2O)18Ge2(GeW10O38)6]39? ( Eu12 ), [Na(H2O)6?Gd12(OH)6(H2O)24Ge(GeW10O38)6]37? ( Gd12 ), and [(H2O)6?Dy12(H2O)24(GeW10O38)6]36? ( Dy12 ), comprising six di‐Ln‐embedded {β(4,11)‐GeW10} subunits was prepared by reaction of [α‐GeW9O34]10? with LnIII ions in weakly acidic (pH 5) aqueous medium. Depending on the size of the LnIII ion, the assemblies feature selective capture of two (for Eu12 ), one (for Gd12 ), or zero (for Dy12 ) extra GeIV ions. The selective encapsulation of a cationic sodium hexaaqua complex [Na(H2O)6]+ was observed for Eu12 and Gd12 , whereas Dy12 incorporates a neutral, distorted‐octahedral (H2O)6 cluster. The three compounds were characterized by single‐crystal XRD, ESI‐MS, photoluminescence, and magnetic studies. Dy12 was shown to be a single‐molecule magnet. 相似文献
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Filtration Shell Mediated Power Density Independent Orthogonal Excitations–Emissions Upconversion Luminescence 下载免费PDF全文
Dr. Xiaomin Li Zhenzhen Guo Tiancong Zhao Yang Lu Lei Zhou Prof. Dongyuan Zhao Prof. Fan Zhang 《Angewandte Chemie (International ed. in English)》2016,55(7):2464-2469
Lanthanide doped core–multishell structured NaGdF4:Yb,Er@NaYF4:Yb@NaGdF4:Yb,Nd@NaYF4@NaGdF4:Yb,Tm@NaYF4 nanoparticles with power‐density independent orthogonal excitations‐emissions upconversion luminescence (UCL) were fabricated for the first time. The optical properties of these core–multishell structured nanoparticles were related to the absorption filtration effect of the NaGdF4:Yb,Tm layer. By tuning the thickness of the filtration layer, the nanoparticles can exhibit unique two independent groups of UCL: Tm3+ prominent UV/blue (UV=ultraviolet) UCL under the excitation at 980 nm and Er3+ prominent green/red UCL under the excitation at 796 nm. The filtration‐shell mediated orthogonal excitations‐emissions UCL are power‐density independent. As a proof of concept, the core–multishell nanoparticles are used in multi‐dimensional security design and imaging‐guided combined photodynamic therapy and chemotherapy. 相似文献
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《化学:亚洲杂志》2017,12(16):2038-2043
The photonic upconversion in rare earth atoms is widely used to convert “invisible” near infrared photons to “visible” photons with continuous wave light. By using a patterned substrate, upconversion become a route for creating new information‐incorporating security codes. The amount of information in the cipher increases in proportion to the number of emission colors as well as the pattern structure. Subsequently, changing the chemical composition of upconversion phosphors on 2 D substrates is required to manufacture information‐rich upconversion cryptography. In this study, we exploited temperature‐controlled thermal reaction on upconversion films deposited on a quartz substrate to prepare security information codes. Multiple color emission was generated from upconversion films as the result of inserting high‐frequency molecular oscillators into the film structures. Fourier‐transform infrared (FTIR) and time‐resolved study corroborated the mechanism of spectral variation of upconversion films. 相似文献
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Aptamer‐Based Luminescence Energy Transfer from Near‐Infrared‐to‐Near‐Infrared Upconverting Nanoparticles to Gold Nanorods and Its Application for the Detection of Thrombin 下载免费PDF全文
Fei Yuan Prof. Dr. Hongqi Chen Juan Xu Yiyan Zhang Yong Wu Prof. Lun Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(10):2888-2894
A new luminescence energy transfer (LET) system has been designed for the detection of thrombin in the near‐infrared (NIR) region by utilizing NIR‐to‐NIR upconversion lanthanide nanophosphors (UCNPs) as the donor and gold nanorods (Au NRs) as the acceptor. The use of upconverting NaYF4:Yb3+,Tm3+ nanoparticles with sharp NIR emission peaks upon NIR excitation by an inexpensive infrared continuous wave laser diode provided large spectral overlap between the donor and the acceptor. Both the Au NRs and carboxyl‐terminated NaYF4:Yb3+,Tm3+ UCNPs were first modified with different thrombin aptamers. When thrombin was added, a LET system was then formed because of the specific recognition between the thrombin aptamers and thrombin. The LET system was used to monitor thrombin concentrations in aqueous buffer and human blood samples. The limits of detection for thrombin are as low as 0.118 nM in buffer solution and 0.129 nM in human serum. The method was also successfully applied to thrombin detection in blood samples. 相似文献
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Unprecedented Sensitization of Visible and Near‐Infrared Lanthanide Luminescence by Using a Tetrathiafulvalene‐Based Chromophore 下载免费PDF全文
Min Feng Dr. Fabrice Pointillart Dr. Boris Le Guennic Bertrand Lefeuvre Dr. Stéphane Golhen Dr. Olivier Cador Dr. Olivier Maury Dr. Lahcène Ouahab 《化学:亚洲杂志》2014,9(10):2814-2825
Ligand L was synthesized and then coordinated to [Ln(hfac)3] ? 2 H2O (LnIII=Tb, Dy, Er; hfac?=1,1,1,5,5,5‐hexafluoroacetylacetonate anion) and [Ln(tta)3]?2 H2O (LnIII=Eu, Gd, Tb, Dy, Er, Yb; tta?=2‐thenoyltrifluoroacetonate) to give two families of dinuclear complexes [Ln2(hfac)6( L )] ? C6H14 and [Ln2(tta)6( L )] ? 2 CH2Cl2. Irradiation of the ligand at 37 040 cm?1 and 29 410 cm?1 leads to tetrathiafulvalene‐centered and 2,6‐di(pyrazol‐1‐yl)‐4‐pyridine‐centered fluorescence, respectively. The ligand acts as an organic chromophore for the sensitization of the infrared ErIII (6535 cm?1) and YbIII (10 200 cm?1) luminescence. The energies of the singlet and triplet states of L are high enough to guarantee an efficient sensitization of the visible EuIII luminescence (17 300–14 100 cm?1). The EuIII luminescence decay can be nicely fitted by a monoexponential function that allows a lifetime estimation of (0.49±0.01) ms. Finally, the magnetic and luminescence properties of [Yb2(hfac)6( L )] ? C6H14 were correlated, which allowed the determination of the crystal field splitting of the 2F7/2 multiplet state with MJ=±1/2 as ground states. 相似文献
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次硝酸(Nitroxyl,HNO)由一氧化氮(NO)经单电子还原和质子化作用产生,在生理和病理过程中都有着重要作用.本工作构建了一种基于发光共振能量转移(Luminescence resonance energy transfer,LRET)的比率型上转换纳米探针用于检测生物体系中HNO含量.该探针以上转换纳米颗粒(Upconversion nanoparticles,UCNPs)为能量供体,有机染料Fl-TP为能量受体构建.Fl-TP能特异性识别HNO并与之反应生成Fl-HNO,Fl-HNO在400~500 nm处具有明显的吸收峰,与UCNPs的蓝色发射光谱重叠,从而发生LRET过程.随着HNO浓度增加,Fl-HNO的荧光强度(F525 nm)逐渐增强,UCNPs的荧光强度(F480 nm)逐渐下降,比率信号(F525 nm/F480 nm)逐渐增加,并与HNO浓度对数呈良好的线性关系,该探针的线性检测范围为3~100 μmol·L-1,检出限23.4 nmol·L-1.实验结果表明该比率探针特异性强,灵敏度高,并可成功实现在活细胞和生物组织中HNO的检测. 相似文献
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Franz A. Mautner Florian Bierbaumer Ramon Vicente Saskia Speed nnia Tubau Merc Font-Bardía Roland C. Fischer Salah S. Massoud 《Molecules (Basel, Switzerland)》2022,27(3)
A new series of mononuclear Ho3+ complexes derived from the β-diketonate anions: 4,4,4-trifluoro-1-phenyl-1,3-butanedioneate (btfa−) and 4,4,4-trifuoro-1-(naphthalen-2-yl)-1,3-butanedionate (ntfa−) have been synthesized, [Ho(btfa)3(H2O)2] (1a), [Ho(ntfa)3(MeOH)2] (1b), (1), [Ho(btfa)3(phen)] (2), [Ho(btfa)3(bipy)] (3), [Ho(btfa)3(di-tbubipy)] (4), [Ho(ntfa)3(Me2bipy)] (5), and [Ho(ntfa)3(bipy)] (6), where phen is 1,10-phenantroline, bipy is 2,2′-bipyridyl, di-tbubipy is 4,4′-di-tert-butyl-2,2′-bipyridyl, and Me2bipy is 4,4′-dimethyl-2,2′-bipyridyl. These compounds have been characterized by elemental microanalysis and infrared spectroscopy as well as single-crystal X-ray difraction for 2–6. The central Ho3+ ions in these compounds display coordination number 8. The luminescence-emission properties of the pyridyl adducts 2–6 display a strong characteristic band in the visible region at 661 nm and a series of bands in the NIR region (excitation wavelengths (λex) of 367 nm for 2–4 and 380 nm for 5 and 6). The magnetic properties of the complexes revealed magnetically uncoupled Ho3+ compounds with no field-induced, single-molecule magnet (SMMs). 相似文献
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Jun Yang Dr. Cuimiao Zhang Chong Peng Chunxia Li Lili Wang Ruitao Chai Jun Lin Prof. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2009,15(18):4649-4655
Light fantastic! Lu2O3:Yb3+/Er3+/Tm3+ nanocrystals with controllable red, green, blue (RGB) and bright white upconversion luminescence by a single laser excitation of 980 nm have been successfully synthesized (see picture). Due to abundant UC PL colors, it can potentially be used as fluorophores in the field of color displays, back light, UC lasers, photonics, and biomedicine.
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Prof. Mei Pan Bin‐Bin Du Yi‐Xuan Zhu Mei‐Qin Yue Dr. Zhang‐Wen Wei Prof. Cheng‐Yong Su 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(7):2440-2451
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
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采用溶剂热法合成了超小尺寸三氟化镧(LaF3)纳米晶. 利用XRD、TEM等对其进行结构与形貌表征,结果显示制得的纳米颗粒为LaF3纳米晶,且具有高度均一的尺寸分布和良好的结晶度,颗粒尺寸为6±0.4 nm. 通过共掺杂镱铒两种稀土元素,所得材料在近红外光激发下(980 nm)可发射出明亮的绿光;发光光谱显示,在524,544,655 nm等位置有较强的发射峰. 利用聚琥珀酰亚胺高分子(PSI)对油溶性的纳米颗粒表面进行功能化修饰,将其成功转移水相. 利用叶酸对其进行进一步生物标记,可与肝癌细胞表面叶酸受体特异性识别,成功地实现了肝癌细胞上转换绿色发光成像研究. 相似文献
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Torelli S Imbert D Cantuel M Bernardinelli G Delahaye S Hauser A Bünzli JC Piguet C 《Chemistry (Weinheim an der Bergstrasse, Germany)》2005,11(11):3228-3242
Inert and optically active pseudo-octahedral Cr(III)N6 and Ru(II)N6 chromophores have been incorporated by self-assembly into heterobimetallic triple-stranded helicates HHH-[CrLnL3]6+ and HHH-[RuLnL3]5+. The crystal structures of [CrLnL(3)](CF(3)SO(3))(6) (Ln=Nd, Eu, Yb, Lu) and [RuLnL3](CF3SO3)5 (Ln=Eu, Lu) demonstrate that the helical structure can accommodate metal ions of different sizes, without sizeable change in the intermetallic MLn distances. These systems are ideally suited for unravelling the molecular factors affecting the intermetallic nd-->4f communication. Visible irradiation of the Cr(III)N6 and Ru(II)N6 chromophores in HHH-[MLnL3]5/6+ (Ln=Nd, Yb, Er; M=Cr, Ru) eventually produces lanthanide-based near infrared (NIR) emission, after directional energy migration within the complexes. Depending on the kinetic regime associated with each specific d-f pair, the NIR luminescence decay times can be tuned from micro- to milliseconds. The origin of this effect, together with its rational control for programming optical functions in discrete heterobimetallic entities, are discussed. 相似文献
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Dr. Fabrice Pointillart Dr. Thomas Cauchy Dr. Olivier Maury Yann Le Gal Dr. Stéphane Golhen Dr. Olivier Cador Dr. Lahcène Ouahab 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(39):11926-11941
The tetrathiafulvalene‐amido‐2‐pyridine‐N‐oxide ( L ) ligand has been employed to coordinate 4f elements. The architecture of the complexes mainly depends on the ionic radii of the lanthanides. Thus, the reaction of L in the same experimental protocol leads to three different molecular structure series. Binuclear [Ln2(hfac)5(O2CPhCl)( L )3] ? 2 H2O (hfac?=1,1,1,5,5,5‐hexafluoroacetylacetonate anion, O2CPhCl?=3‐chlorobenzoate anion) and mononuclear [Ln(hfac)3( L )2] complexes were obtained by using rare‐earth ions with either large (LnIII=Pr, Gd) or small (LnIII=Y, Yb) ionic radius, respectively, whereas the use of TbIII that possesses an intermediate ionic radius led to the formation of a binuclear complex of formula [Tb2(hfac)4(O2CPhCl)2( L )2]. Antiferromagnetic interactions have been observed in the three dinuclear compounds by using an extended empirical method. Photophysical properties of the coordination complexes have been studied by solid‐state absorption spectroscopy, whereas time‐dependent density functional theory (TD‐DFT) calculations have been carried out on the diamagnetic YIII derivative to build a molecular orbital diagram and to reproduce the absorption spectrum. For the [Yb(hfac)3( L )2] complex, the excitation at 19 600 cm?1 of the HOMO→LUMO+1/LUMO+2 charge‐transfer transition induces both line‐shape emissions in the near‐IR spectral range assigned to the 2F5/2→2F7/2 (9860 cm?1) ytterbium‐centered transition and a residual charge‐transfer emission around 13 150 cm?1. An efficient antenna effect that proceeds through energy transfer from the singlet excited state of the tetrathiafulvalene‐amido‐2‐pyridine‐N‐oxide chromophore is evidence of the YbIII sensitization. 相似文献