upconversion luminescence

上转换发光
  • 文章类型: Journal Article
    持续发光描述了在停止激发之后发光仍然存在的现象。最近,可以通过近红外(NIR)光直接充电的上转换持久发光(UCPL)磷光体由于其从光子学到生物医学的有前途的应用而受到了广泛的关注。然而,当前基于镧系元素的UCPL磷光体显示小的吸收截面和低的上转换充电效率。由于缺乏灵活的上转换充电路径和差的设计灵活性,UCPL磷光体的开发面临挑战。在这里,我们在Cr掺杂的没食子酸锌纳米颗粒中发现了晶格缺陷介导的宽带光子上转换过程和伴随的NIR到NIRUCPL。没食子酸锌纳米颗粒可以通过700-1000nm范围内的宽带NIR光直接激活,以在约700nm处产生持久的发光,通过合理地调整磷光体中的晶格缺陷也很容易增强。这种提出的UCPL磷光体通过有效地避免来自自发荧光和光散射的干扰,在生物成像中实现了超过200的信号-背景比。我们的工作报道了晶格缺陷介导的光子上转换现象,这极大地扩展了UCPL磷光体的灵活设计的视野,使其应用范围从生物成像到光催化。
    Persistent luminescence describes the phenomenon whereby luminescence remains after the stoppage of excitation. Recently, upconversion persistent luminescence (UCPL) phosphors that can be directly charged by near-infrared (NIR) light have gained considerable attention due to their promising applications ranging from photonics to biomedicine. However, current lanthanide-based UCPL phosphors show small absorption cross sections and low upconversion charging efficiency. The development of UCPL phosphors faces challenges due to the lack of flexible upconversion charging pathways and poor design flexibility. Herein, we discovered a lattice defect-mediated broadband photon upconversion process and the accompanying NIR-to-NIR UCPL in Cr-doped zinc gallate nanoparticles. The zinc gallate nanoparticles can be directly activated by broadband NIR light in the 700-1000 nm range to produce persistent luminescence at about 700 nm, which is also readily enhanced by rationally tailoring the lattice defects in the phosphors. This proposed UCPL phosphor achieved a signal-to-background ratio of over 200 in bioimaging by efficiently avoiding interference from autofluorescence and light scattering. Our work reported a lattice defect-mediated photon upconversion phenomenon, which significantly expands the horizons for the flexible design of UCPL phosphors toward broad applications ranging from bioimaging to photocatalysis.
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  • 文章类型: Journal Article
    协同治疗已成为临床治疗恶性肿瘤的主要方法。光动力疗法(PDT)和放射疗法(RT)总是结合在一起,因为它们相同的抗肿瘤机制,也就是说,通过X射线照射后使用放射增敏剂产生活性氧,以有效杀死癌细胞,PDT也遵循类似的机制。纳米材料中的能量吸收物种完全暴露于X射线或近红外光照射下,使纳米材料与周围H2O或溶解氧之间的能量交换更容易,然而,它仍然具有挑战性。在这里,开发了一种超薄二维(2D)纳米片(NS),Bi2O2CO3,掺杂镧系元素离子,发出上转换发光,其中高Z元素Bi,Yb,Er促进放射增敏作用。令人惊讶的是,与传统的上转换纳米粒子相比,镧系元素激活剂离子给出了完全不同的发光特性。纳米片晶格中Er离子的掺杂剂较少导致更亮的红色发射,这提供了更有效的PDT。在RT/PDT联合治疗下,NS显示出良好的肿瘤生长抑制作用。此外,协同治疗需要比常规放射治疗更低的辐射剂量和比单一光动力治疗更低的光功率。从而大大减少了由RT引起的辐射损伤和由PDT引起的热损伤。
    Synergistic therapy has become the major therapeutic method for malignant tumors in clinical. Photodynamic therapy (PDT) and radiotherapy (RT) always combine together because of their identical anti-tumor mechanisms, that is reactive oxygen species are generated by the use of radiosensitizers after irradiation by X-ray to efficiently kill cancer cells, PDT also follows similar mechanism. Full exposure of energy-absorbing species in nanomaterials to X-ray or near-infrared light irradiation makes the energy interchange between nanomaterials and surrounding H2O or dissolved oxygen easier, however, it remains challenging. Herein, an ultrathin two-dimensional (2D) nanosheet (NS) is developed, Bi2O2CO3, doped with lanthanide ions to give out upconversion luminescence, where the high Z elements Bi, Yb, and Er promote the radio-sensitizing effect. To the surprise, lanthanide activator ions gave out completely different luminescence properties compared with traditional upconversion nanoparticles. Less dopant of Er ions in nanosheets lattice resulted in brighter red emission, which provides more efficient PDT. Under RT/PDT combined treatment, NS shows a good tumor growth-inhibiting effect. In addition, synergistic therapy requires lower radiation dose than conventional radiotherapy and lower light power than single photodynamic therapy, thus greatly reducing radiation damage caused by RT and thermal damage caused by PDT.
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  • 文章类型: Journal Article
    尼古丁(3-(1-甲基-2-吡咯烷基)吡啶)是最常见的成瘾性物质之一,导致尼古丁的痕量检测是非常必要的。在这里,我们设计并制备了一种功能化的纳米复合材料CS-PAA(NaYF4:19.5%Yb,0.5%Tm@NaYF4-PAA)使用简单的方法。通过尼古丁对胆碱氧化酶活性的抑制和Fe3抑制CS-PAA的发光强度来定量检测尼古丁浓度。通过发光寿命和紫外-可见吸收光谱表征推断了Fe3猝灭CS-PAA发射的机理。在尼古丁检测过程中,CS-PAA的激发(980nm)和发射(802nm)波长都可以避免背景荧光在复杂的食物对象中的干扰,从而提供高选择性和灵敏度,线性范围为5-750ng/mL,检测限为9.3nM。该方法具有良好的回收率和相对标准偏差,表明尼古丁检测的高准确性和可重复性。
    Nicotine (3-(1-methyl-2-pyrrolidinyl)pyridine) is one of the most common addictive substances, causing the trace detection of nicotine to be very necessary. Herein, we designed and prepared a functionalized nanocomposite CS-PAA (NaYF4:19.5%Yb,0.5%Tm@NaYF4-PAA) using a simple method. The nicotine concentration was quantitatively detected through the inhibition of choline oxidase activity by nicotine and the luminescence intensity of CS-PAA being quenched by Fe3+. The mechanism of Fe3+ quenching CS-PAA emission was inferred by luminescence lifetime and UV-vis absorption spectra characterization. During the nicotine detection, both excitation (980 nm) and emission (802 nm) wavelengths of CS-PAA enable the avoidance of the interference of background fluorescence in complicated food objects, thus providing high selectivity and sensitivity with a linear range of 5-750 ng/mL and a limit of detection of 9.3 nM. The method exhibits an excellent recovery and relative standard deviation, indicating high accuracy and repeatability of the detection of nicotine.
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  • 文章类型: Journal Article
    在这项研究中,我们研究了微米级NaYF4晶体双掺杂Yb3+/Er3+镧系元素离子,专为温度传感应用。与以前的研究相比,主要关注高温环境,我们的调查涵盖了高温和超低温的全面范围。我们在频域和时域中探索温度与上转换发光(UCL)光谱之间的关系。我们的发现强调了镧系元素掺杂的NaYF4晶体的这些光谱特征对温度的强烈依赖性。此外,我们介绍了一种双模式发光温度测量技术,利用绿色和红色排放的上转换排放强度比。这项研究还考察了温度传感之间的相关性,能级差异,和Er3+离子在各种温度尺度上的热耦合。我们的研究有助于推进镧系元素掺杂材料的理解和应用,为未来在不同领域的温度传感创新奠定基础。
    In this study, we investigate micrometer-sized NaYF4 crystals double-doped with Yb3+/Er3+ lanthanide ions, designed for temperature-sensing applications. In contrast to previous studies, which focused predominantly on the high-temperature regime, our investigation spans a comprehensive range of both high and ultralow temperatures. We explore the relationship between temperature and the upconversion luminescence (UCL) spectra in both frequency and time domains. Our findings highlight the strong dependence of these spectral characteristics of lanthanide-doped NaYF4 crystals on temperature. Furthermore, we introduce a dual-mode luminescence temperature measurement technique, leveraging the upconversion emission intensity ratio for both green and red emissions. This study also examines the correlation between temperature sensing, energy level disparities, and thermal coupling in Er3+ ions across various temperature scales. Our research contributes to advancing the understanding and application of lanthanide-doped materials, setting a foundation for future innovations in temperature sensing across diverse fields.
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  • 文章类型: Journal Article
    随着荧光比技术(FIR)和荧光寿命(FL)策略的出现,光学传感器技术经历了变革性的发展。革命性的精度,性能,和可靠性。本研究深入研究了掺杂Ho3/Nd3的Ba2GdV3O11荧光粉的合成,Er3+,Yb3+,采用溶胶-凝胶方法进行上转换材料制造。对结构进行彻底调查,形态学,并对所合成的荧光粉进行了光学性能分析。980nm的激发揭示了绿色和红色光谱的上转换(UC)发射。观察到的Ho3发射带的强度,Nd3+,和Er3+表现出对温度波动的显著敏感性。温度传感依赖于4S3/2和2H11/2上转换发射带,除了4S3/2的排放寿命。获得增强的热灵敏度值,使用FIR策略达到1.03%K-1和1.07%K-1,对于Ho3+/Er3+/Yb3+和Nd3+/Er3+/Yb3+三掺杂Ba2GdV3O11荧光粉,采用FL策略,最高可达0.146%K-1和0.47%K-1,分别。此外,所研究的荧光粉在检测微小的温度变化(0.3K)方面表现出卓越的精度,将它们定位为有希望的候选人进行精确的温度传感。这项研究开创了推进光学测温技术的创新方法,为科学和工业应用提供有希望的前景依赖于精确的光学温度传感。
    Optical sensor technology has undergone a transformative evolution with the advent of fluorescence ratio techniques (FIR) and fluorescence lifetime (FL) strategies, revolutionizing precision, performance, and reliability. This study delves into the synthesis of Ba2GdV3O11 phosphors doped with Ho3+/Nd3+, Er3+, and Yb3+, employing the sol-gel method for upconverting material fabrication. A thorough investigation into the structural, morphological, and optical properties of the synthesized phosphors is conducted. Excitation at 980 nm unveils upconversion (UC) emissions across green and red spectra. The intensities of the observed emission bands for Ho3+, Nd3+, and Er3+ demonstrate significant sensitivity to fluctuations in temperature. Temperature sensing relies on the 4S3/2 and 2H11/2 upconversion emissions bands, in addition to the emission lifetimes at 4S3/2. Enhanced thermal sensitivity values are attained, reaching up to 1.03 % K-1 and 1.07 % K-1 using the FIR strategy, and up to 0.146 % K-1 and 0.47 % K-1 with the FL strategy for Ho3+/Er3+/Yb3+ and Nd3+/Er3+/Yb3+ tri-doped Ba2GdV3O11 phosphors, respectively. Furthermore, the studied phosphors exhibit remarkable precision in detecting minute temperature changes (0.3 K), positioning them as promising candidates for precise temperature sensing. This study pioneers innovative methodologies to advance optical thermometry techniques, offering promising prospects for scientific and industrial applications reliant on precise optical temperature sensing.
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  • 文章类型: Journal Article
    试图通过故意掺入晶格缺陷来优化Nd3敏化近红外(808nm)上转换核壳(CS)纳米晶体的上转换发光(UCL)输出,使用高能同步加速器X射线(λ=0.568551µ)衍射的积分宽度计算,对CS界面和核心层内的微应变进行了综合分析。使用高能总散射的对分布函数分析对这种微应变进行了原子级解释。核心数控开发了压缩微应变,随着外延壳的生长逐渐转变为拉伸微应变。就一致的负晶格失配而言,这种逆转是合理的。在掺入Li+后将晶格缺陷引入CS体系后,相应的UCL强度在某些特定的Li+掺入下最大化,其中CS的拉伸微应变,岩心的压缩微应变,和原子级紊乱表现出各自的极值,而与活化剂离子无关。
    In an attempt to optimize the upconversion luminescence (UCL) output of a Nd3+-sensitized near-infrared (808 nm) upconverting core-shell (CS) nanocrystal through deliberate incorporation of lattice defects, a comprehensive analysis of microstrain both at the CS interface and within the core layer was performed using integral breadth calculation of high-energy synchrotron X-ray (λ = 0.568551 Å) diffraction. An atomic level interpretation of such microstrain was performed using pair distribution function analysis of the high-energy total scattering. The core NC developed compressive microstrain, which gradually transformed into tensile microstrain with the growth of the epitaxial shell. Such a reversal was rationalized in terms of a consistent negative lattice mismatch. Upon introduction of lattice defects into the CS systems upon incorporation of Li+, the corresponding UCL intensity was maximized at some specific Li+ incorporation, where the tensile microstrain of CS, compressive microstrain of the core, and atomic level disorders exhibited their respective extreme values irrespective of the activator ions.
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  • 文章类型: Journal Article
    在这项工作中,报告了一种基于荧光粉轮动态调整NaGdF4:Yb3+/Ho3+/Ce3+/Sc3+的上转换发光(UCL)颜色的策略。已经证明,旋转相关的UCL主要源于Ho3:5I6水平的耗尽模式的调节。由于主要的线性衰减,在稳态激励下观察到高纯红色UCL。然而,随着稳态激励比例的降低,绿色-红色发光强度比逐渐增加,其次是颜色从红色到绿色的转换。提出了一个近似的物理模型来理解IG/IR对旋转速度的依赖性。我们不仅报告了一种UCL材料,该材料显示了在速度感测中的潜在应用,而且还提供了对基于车轮的动态UCL调节的新见解。
    In this work, a strategy for dynamically adjusting the upconversion luminescence (UCL) color of NaGdF4:Yb3+/Ho3+/Ce3+/Sc3+ is reported based on a phosphor wheel. It has been demonstrated that the rotation-dependent UCL mainly originated from the regulation of depletion mode for the Ho3+: 5I6 level. Due to the dominant linear decay, a high-pure red UCL is observed under the steady-state excitation. However, as the proportion of the steady-state excitation decreases, the green-red emission intensity ratio gradually increases, followed by the color conversion from red to green. An approximate physical model is proposed to understand the dependence of IG/IR on rotation speed. We not only report a UCL material that shows potential application in velocity sensing but also provide new insights into wheel-based dynamic UCL regulation.
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  • 文章类型: Journal Article
    这里,这项研究报道了通过掺杂Mn2在β-Ba2ScAlO5:Yb3/Er3荧光粉中的单波段红色上转换发射。β-Ba2ScAlO5:Yb3+/Er3+荧光粉中Mn2+离子的最佳浓度为0.20。红色和绿色排放强度分别提高了27.4和19.3倍,分别。与不含Mn2+离子的样品比拟,β-Ba2ScAlO5:Yb3+/Er3+/Mn2+样品的红绿积分强度比显著提高了28.4倍,达到110.9。通过分析下转换发光光谱,探索了UCL机制,吸收光谱,UCL光谱,和Yb3+/Er3+/Mn2+共掺杂β-Ba2ScAlO5的上转换荧光寿命衰减曲线。上转换红光的增强是通过缺陷带和Er3+离子之间的能量转移来实现的,以及Mn2+离子和Er3+离子之间的能量转移。此外,Mn2掺杂的β-Ba2ScAlO5:Yb3/Er3红色UCL荧光粉在298-523K温度范围内具有巨大的环境温度传感潜力。在523K时,β-Ba2ScAlO5:Yb3/Er3/Mn2荧光粉作为温度传感器的最大灵敏度为0.0247K-1。
    Here, this study reports single-band red upconversion emission in β-Ba2ScAlO5: Yb3+/Er3+ phosphor by doping Mn2+. The optimum concentration of Mn2+ ions in β-Ba2ScAlO5: Yb3+/Er3+ phosphor was 0.20. The intensity of red and green emissions is increased by 27.4 and 19.3 times, respectively. Compared with the samples without Mn2+ ions, the red-green integral strength ratio of β-Ba2ScAlO5: Yb3+/Er3+/Mn2+ sample was significantly increased by 28.4 times, reaching 110.9. The UCL mechanism was explored by analyzing the down-conversion luminescence spectra, absorption spectra, UCL spectra, and upconversion fluorescence lifetime decay curves of Yb3+/Er3+/Mn2+ co-doped β-Ba2ScAlO5. The enhancement of upconversion red light is achieved through energy transfer between defect bands and Er3+ ions, as well as energy transfer between Mn2+ ions and Er3+ ions. In addition, the Mn2+ doped β-Ba2ScAlO5: Yb3+/Er3+ red UCL phosphors have great potential for ambient temperature sensing in the 298-523 K temperature range. The maximum sensitivity of β-Ba2ScAlO5: Yb3+/Er3+/Mn2+ phosphor as a temperature sensor at 523 K is 0.0247 K-1.
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  • 文章类型: Journal Article
    多重侧流测定(LFA)通过同时检测单个样品中的多种生物标志物,提供高效的现场测试。降低成本。在癌症诊断中,生物标志物可能缺乏特异性,多参数检测提供了更多的信息在护理点。我们的研究集中在上皮性卵巢癌(EOC),其中STn-糖基化形式的CA125和CA15-3抗原可以更好地区分癌症与良性疾病。我们已经开发了双标记LFA,其在单个抗STn抗体测试线内检测CA125-STn和CA15-3-STn。这利用了绿色(540nm)和蓝色(450nm)发射铒(NaYF4:Yb3+,Er3)-和thulium(NaYF4:Yb3,与针对CA125或CA15-3中的蛋白质表位的抗体缀合的Tm3)掺杂的上转换纳米颗粒(UCNP)报道分子。该技术允许同时检测来自单个测试线的不同抗原变体。开发的概念验证双标签LFA能够区分来自诊断的卵巢癌患者的腹水样品(n=10)和用作阴性对照的肝硬化腹水样品(n=3)。CA125-STn对双标记LFA的分析灵敏度在缓冲液中为1.8U/ml,在腹水流体基质中为3.6U/ml。在这里,我们展示了一种通过使用UCNP报告技术对两种不同的癌症相关蛋白生物标志物的STn-糖基化形式进行光谱分离测量的新方法。
    Multiplexed lateral flow assays (LFAs) offer efficient on-site testing by simultaneously detecting multiple biomarkers from a single sample, reducing costs. In cancer diagnostics, where biomarkers can lack specificity, multiparameter detection provides more information at the point-of-care. Our research focuses on epithelial ovarian cancer (EOC), where STn-glycosylated forms of CA125 and CA15-3 antigens can better discriminate cancer from benign conditions. We have developed a dual-label LFA that detects both CA125-STn and CA15-3-STn within a single anti-STn antibody test line. This utilizes spectral separation of green (540 nm) and blue (450 nm) emitting erbium (NaYF4:Yb3+, Er3+)- and thulium (NaYF4: Yb3+, Tm3+)-doped upconverting nanoparticle (UCNP) reporters conjugated with antibodies against the protein epitopes in CA125 or CA15-3. This technology allows the simultaneous detection of different antigen variants from a single test line. The developed proof-of-concept dual-label LFA was able to distinguish between the ascites fluid samples from diagnosed ovarian cancer patients (n = 10) and liver cirrhosis ascites fluid samples (n = 3) used as a negative control. The analytical sensitivity of CA125-STn for the dual-label LFA was 1.8 U/ml in buffer and 3.6 U/ml in ascites fluid matrix. Here we demonstrate a novel approach of spectrally separated measurement of STn-glycosylated forms of two different cancer-associated protein biomarkers by using UCNP reporter technology.
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  • 文章类型: Journal Article
    温度和压力是材料科学领域的基本物理参数,使他们的监测对科学家和工程师来说意义非凡。这里,NaSrY(MoO4)3:0.02Er3/0.01Tm3/0.15Yb3纳米荧光粉被开发为光学传感器材料。在975nm激光激发下,研究了温度和压力(真空)多功能传感平台的上转换特性和光学检测性能。我们成功开发了一种新型检测平台,可对压力(真空)和温度进行光学检测。该平台利用热耦合水平(TCL)和Er3+和Tm3+的非TCL来实现比率检测。利用双发射中心的不同发射波段,成功实现了基于TCL和非TCL的多模态光学温度和压力检测,这使得自参考光学温度和压力测量模式成为可能。这些结果表明,开发的纳米荧光粉是光学传感器的有前途的候选,我们的发现提出了调制掺杂稀土离子的发光材料的传感器特性的潜在策略。
    Temperature and pressure are fundamental physical parameters in the field of materials science, making their monitoring of utmost significance for scientists and engineers. Here, the NaSrY(MoO4)3:0.02Er3+/0.01Tm3+/0.15Yb3+ nanophosphor is developed as an optical sensor material. Under 975 nm laser excitation, the upconversion characteristics and optical detection performance of the multifunctional sensing platform of temperature and pressure (vacuum) are investigated. We have successfully developed a novel detection platform that enables optical detection of pressure (vacuum) and temperature. This platform utilizes thermally coupled levels (TCLs) and non-TCLs of Er3+ and Tm3+ to achieve ratiometric detection. The multimodal optical temperature and pressure detection based on TCLs and non-TCLs is successfully realized by using different emission bands of double emission centers, which makes it possible for self-referencing optical temperature and pressure measurement modes. These results indicate that the developed nanophosphor is a promising candidate for optical sensors, and our findings suggest potential strategies for modulating the sensor properties of luminescent materials doped with rare-earth ions.
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