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Fluorescence quenching determination of tetracyclines based on the synergistic oxidation effect between Fe3O4nanoparticles and tetracyclines. 基于fe3o4纳米颗粒与四环素协同氧化效应的荧光猝灭测定四环素。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-04-13 DOI: 10.1088/2050-6120/acca61
Shiqi Guo, Yilin Chai, Yongjun Wu, Hongchao Guo, Fei Yu, Li-E Liu, Leiliang He, Songcheng Yu, Yongmei Tian, Jia Wang, Ruiying Yang, Ningge Jian, Yilin Wang

In recent years, tetracyclines (TCs) is a hot research topic. Herein, we report an interesting discovery using the complexation of oxytetracycline and metal ions. In this study, according to the properties of Fe3O4nanoparticles (Fe3O4NPs) as a nanoenzyme, it can be used to catalyze the oxidation of KI by H2O2to produceI3-,while at the same timeI3-binds to rhodamine 6G (Rh6G) to form a conjoined particle (Rh6G ∼ I3)n, leading to a decrease in the fluorescence intensity of Rh6G. However, in the presence of TCs, Fe3O4NPs have a synergistic effect with TCs, leading to enhanced catalytic activity, as well as better selectivity compared to the activity of other reducing enzymes. Consequently,the fluorescent signal based on a resonance scattering effect between Rh6G andI3-is dependent on the concentration of TCs, thus achieving highly facile and robust detection of TCs. The limits of detection (LOD) of the method were 20 nM, 10 nM and 40 nM for oxytetracycline(OTC), tetracycline(TC) and chlortetracycline(CTC), respectively. Most importantly, the method can be successfully applied to the detection of TCs in milk, eggs, and honey. The recoveries of spiked samples ranged from 83.11 to 118.95%. Thus, a stable, hands-on strategy for the detection of TCs is proposed, which has potential applications in the field of food safety and environmental protection.

近年来,四环素类药物是一个研究热点。在此,我们报告了一个有趣的发现,使用络合的土霉素和金属离子。在本研究中,根据fe3o4纳米粒子(Fe3O4NPs)作为纳米酶的性质,它可以用来催化h2o2氧化KI生成ei3 -,同时I3与罗丹明6G (Rh6G)结合形成连体粒子(Rh6G ~ I3)n,导致Rh6G的荧光强度降低。然而,在tc的存在下,Fe3O4NPs与tc有协同作用,导致催化活性增强,并且与其他还原酶的活性相比具有更好的选择性。因此,基于Rh6G和di3之间的共振散射效应的荧光信号依赖于tc的浓度,从而实现了对tc的高度方便和鲁棒性检测。方法对土霉素(OTC)、四环素(TC)和金霉素(CTC)的检出限(LOD)分别为20 nM、10 nM和40 nM。最重要的是,该方法可以成功地应用于牛奶、鸡蛋和蜂蜜中的TCs检测。加样回收率为83.11% ~ 118.95%。因此,本文提出了一种稳定、实用的TCs检测方法,在食品安全和环境保护领域具有潜在的应用前景。
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引用次数: 0
Room Temperature Phosphorescence of 5,6-Benzoquinoline. 5,6-苯并喹啉的室温磷光。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-04-03 DOI: 10.1088/2050-6120/acc716
Jose Chavez, Luca Ceresa, Emma Kitchner, Danh Pham, Zygmunt Gryczynski, Ignacy Gryczynski

Phosphorescence emission of 5,6-Benzoquinoline embedded in poly (vinyl alcohol) film has been studied at room temperature. A strong green long-lived emission was observed in films doped with 5,6-Benzoquinoline while illuminated on a UV plate. A broad phosphorescence emission spectrum is centered at about 500 nm. The phosphorescence excitation spectrum follows the absorption spectrum of 5,6-Benzoquinoline, except for a long-wavelength part, which is well beyond the absorption band. This long-wavelength part of the absorption spectrum is responsible for the forbidden S0-T1transition. The excitation at 430 nm resulted in the long-lived emission with a spectrum similar to the phosphorescence spectrum obtained with UV excitation within the absorption of 5,6-Benzoquinoline. The phosphorescence anisotropy obtained with a direct S0-T1excitation is positive, while the UV excitation is negative. In contrast to fluorescence, the phosphorescence intensity strongly depends on temperature. Phosphorescence lifetimes with UV and long-wavelength excitation are similar, with a mean value of about 0.5 s.

研究了5,6-苯并喹啉包埋在聚乙烯醇薄膜中的室温磷光发射。在紫外板上照射时,在掺杂5,6-苯并喹啉的薄膜中观察到强烈的绿色长寿命发射。广泛的磷光发射光谱集中在约500纳米处。磷光激发光谱遵循5,6-苯并喹啉的吸收光谱,除了长波长部分远远超出吸收带。吸收光谱的长波长部分负责禁止的s0 - t1跃迁。在430 nm处激发产生了长寿命的发光,其光谱与5,6-苯并喹啉吸收范围内紫外激发获得的磷光光谱相似。直接s0 - t1激发得到的磷光各向异性为正,而紫外激发得到的磷光各向异性为负。与荧光相反,磷光强度强烈依赖于温度。紫外和长波激发下的磷光寿命相似,平均值约为0.5 s。
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引用次数: 0
Fluorescent carbon dots tailored iron oxide nano hybrid system forin vivooptical imaging of liver fibrosis. 荧光碳点定制氧化铁纳米混合系统用于肝纤维化的体内光学成像。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-03-21 DOI: 10.1088/2050-6120/acc009
Shaiju S Nazeer, Ariya Saraswathy, Nirmala Nimi, Elangovan Sarathkumar, A N Resmi, Sachin J Shenoy, Ramapurath S Jayasree

Hybrid nanoparticles are innovative invention of last decade designed to overcome limitations of single-component nanoparticles by introducing multiple functionalities through combining two or more different nanoparticles. In this study, we are reporting development of magneto-fluorescent hybrid nanoparticles by combining iron oxide and carbon nanoparticles to enablein vivofluorescence imaging which also has all the required characteristic properties to use as Magnetic Resonance Imaging (MRI) contrast agent. In order to achieve dual-functional imaging, alginate and pullulan coated super paramagnetic iron oxide nanoparticles (ASPION and PSPION) and Carbon dots (Cdts) were synthesised separately. ASPIONs and PSPIONs were further chemically conjugated with Cdts and developed dual-functional nanohybrid particles ASPION-Cdts and PSPION-Cdts. Subsequently, evaluation of the materials for its size, functionalisation efficiency, fluorescence and magnetic properties, biocompatibility and cellular uptake efficiency has been carried out. Fluorescence imaging of liver fibrosis was performedin vivoin rodent model of liver fibrosis using the two nanohybrids, which is further confirmed by high fluorescence signal from the harvested liver.

混合纳米颗粒是近十年来的创新发明,旨在通过结合两种或多种不同的纳米颗粒来引入多种功能,从而克服单组分纳米颗粒的局限性。在这项研究中,我们报告了通过结合氧化铁和碳纳米颗粒来开发磁荧光混合纳米颗粒,以实现体内荧光成像,该成像还具有用作磁共振成像(MRI)造影剂所需的所有特性。为了实现双功能成像,分别合成了海藻酸盐和普鲁兰包覆的超顺磁性氧化铁纳米粒子(ASPION和PSPION)和碳点(Cdts)。进一步将ASPIONs和PSPIONs与Cdts进行化学偶联,制备出双功能纳米杂化粒子ASPION-Cdts和PSPION-Cdts。随后,对材料的尺寸、功能化效率、荧光和磁性、生物相容性和细胞摄取效率进行了评估。利用这两种纳米杂交体对肝纤维化动物模型进行了肝纤维化荧光成像,并通过采集肝脏的高荧光信号进一步证实了这一点。
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引用次数: 1
Compact and robust deep learning architecture for fluorescence lifetime imaging and FPGA implementation. 用于荧光寿命成像和FPGA实现的紧凑和健壮的深度学习架构。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-03-20 DOI: 10.1088/2050-6120/acc0d9
Zhenya Zang, Dong Xiao, Quan Wang, Ziao Jiao, Yu Chen, David Day-Uei Li

This paper reports a bespoke adder-based deep learning network for time-domain fluorescence lifetime imaging (FLIM). By leveraging thel1-norm extraction method, we propose a 1D Fluorescence Lifetime AdderNet (FLAN) without multiplication-based convolutions to reduce the computational complexity. Further, we compressed fluorescence decays in temporal dimension using a log-scale merging technique to discard redundant temporal information derived as log-scaling FLAN (FLAN+LS). FLAN+LS achieves 0.11 and 0.23 compression ratios compared with FLAN and a conventional 1D convolutional neural network (1D CNN) while maintaining high accuracy in retrieving lifetimes. We extensively evaluated FLAN and FLAN+LS using synthetic and real data. A traditional fitting method and other non-fitting, high-accuracy algorithms were compared with our networks for synthetic data. Our networks attained a minor reconstruction error in different photon-count scenarios. For real data, we used fluorescent beads' data acquired by a confocal microscope to validate the effectiveness of real fluorophores, and our networks can differentiate beads with different lifetimes. Additionally, we implemented the network architecture on a field-programmable gate array (FPGA) with a post-quantization technique to shorten the bit-width, thereby improving computing efficiency. FLAN+LS on hardware achieves the highest computing efficiency compared to 1D CNN and FLAN. We also discussed the applicability of our network and hardware architecture for other time-resolved biomedical applications using photon-efficient, time-resolved sensors.

本文报道了一种定制的基于加法器的时域荧光寿命成像(FLIM)深度学习网络。通过利用1范数提取方法,我们提出了一种不基于乘法卷积的一维荧光寿命AdderNet (FLAN),以降低计算复杂度。此外,我们使用对数尺度合并技术在时间维度上压缩荧光衰减,以丢弃作为对数尺度FLAN (FLAN+LS)衍生的冗余时间信息。与FLAN和传统1D卷积神经网络(1D CNN)相比,FLAN+LS的压缩比分别为0.11和0.23,同时在检索寿命方面保持了较高的准确性。我们使用合成和真实数据广泛评估了FLAN和FLAN+LS。将传统的拟合方法与其他非拟合的高精度算法进行了比较。我们的网络在不同的光子计数场景下获得了较小的重建误差。对于真实数据,我们使用共聚焦显微镜获得的荧光珠数据来验证真实荧光团的有效性,并且我们的网络可以区分不同寿命的珠。此外,我们在现场可编程门阵列(FPGA)上实现了网络架构,并采用后量化技术缩短了位宽,从而提高了计算效率。与1D CNN和FLAN相比,硬件上的FLAN+LS实现了最高的计算效率。我们还讨论了我们的网络和硬件架构在使用光子效率、时间分辨传感器的其他时间分辨生物医学应用中的适用性。
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引用次数: 2
Multi-stimuli-responsive and dynamic color tunable security ink for multilevel anticounterfeiting. 多刺激响应和动态颜色可调安全油墨,多级防伪。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-03-15 DOI: 10.1088/2050-6120/acbe92
Charu Dubey, Anjana Yadav, Diksha Baloni, Sachin Singh, Anjani Kumar Singh, Sunil Kumar Singh, Akhilesh Kumar Singh

Luminescent security features have been used for anticounterfeiting for a long time. However, constant effort is required to strengthen these security features to be ahead of counterfeiters. Here, we developed a multi-stimuli-responsive luminescent security ink containing Tb(ASA)3Phen, K2SiF6:Mn4+,and NaYF4:Yb3+/Er3+luminescent materials in PVC gold medium. Tb(ASA)3Phen complex shows a broad excitation band in the UV region; upon UV light radiation it shows strong greenish emission of Tb3+ions through the antenna effect. K2SiF6:Mn4+, on the other hand, has three excitation bands with maxima at 248, 354, and 454 nm which emit red light after excitation through these bands. NaYF4:Yb3+/Er3+is used as an upconverting nanophosphor showing green emission under 976 nm laser excitation. Thus, the multi-stimuli-responsive luminescent security ink shows greenish, red, and green emissions under 367 nm, 450 nm, and 976 nm excitations, respectively. Furthermore, the distinct lifetimes of the activators in Tb(ASA)3Phen and K2SiF6:Mn4+, i.e. 0.1708 ms and 8.165 ms, respectively, under 380 nm excitation make this ink suitable for dynamic anticounterfeiting as well. The ink shows a change in the emission color with time delay, after the removal of the 380 nm excitation source, from greenish yellow (at 0 delays) to reddish color after a delay of 7.5 ms. These unique optical features along with excellent photo-, chemical- and environmental stability make this ink useful for advanced-level anticounterfeiting.

发光防伪特性被用于防伪已经很长时间了。然而,需要不断的努力来加强这些安全功能,以领先于造假者。在此,我们在PVC金介质中开发了一种含有Tb(ASA)3Phen, K2SiF6:Mn4+和NaYF4:Yb3+/Er3+发光材料的多刺激响应发光安全油墨。Tb(ASA)3Phen配合物在紫外区表现出较宽的激发带;在紫外光照射下,通过天线效应显示出Tb3+离子的强绿色发射。另一方面,K2SiF6:Mn4+具有三个激发带,在248、354和454 nm处达到最大值,激发后通过这些激发带发出红光。采用NaYF4:Yb3+/Er3+作为上转换纳米荧光粉,在976 nm激光激发下显示绿色发射。因此,多刺激响应发光安全油墨在367nm, 450nm和976nm激发下分别显示绿色,红色和绿色发射。此外,在380 nm激发下,活化剂在Tb(ASA)3Phen和K2SiF6:Mn4+中的寿命分别为0.1708 ms和8.165 ms,这也使得该油墨适合动态防伪。在去除380 nm激发源后,墨水的发射颜色随时间延迟的变化,从绿黄色(0延迟)到红红色(7.5 ms延迟)。这些独特的光学特性以及优异的光、化学和环境稳定性使这种油墨可用于高级防伪。
{"title":"Multi-stimuli-responsive and dynamic color tunable security ink for multilevel anticounterfeiting.","authors":"Charu Dubey,&nbsp;Anjana Yadav,&nbsp;Diksha Baloni,&nbsp;Sachin Singh,&nbsp;Anjani Kumar Singh,&nbsp;Sunil Kumar Singh,&nbsp;Akhilesh Kumar Singh","doi":"10.1088/2050-6120/acbe92","DOIUrl":"https://doi.org/10.1088/2050-6120/acbe92","url":null,"abstract":"<p><p>Luminescent security features have been used for anticounterfeiting for a long time. However, constant effort is required to strengthen these security features to be ahead of counterfeiters. Here, we developed a multi-stimuli-responsive luminescent security ink containing Tb(ASA)<sub>3</sub>Phen, K<sub>2</sub>SiF<sub>6</sub>:Mn<sup>4+,</sup>and NaYF<sub>4</sub>:Yb<sup>3+</sup>/Er<sup>3+</sup>luminescent materials in PVC gold medium. Tb(ASA)<sub>3</sub>Phen complex shows a broad excitation band in the UV region; upon UV light radiation it shows strong greenish emission of Tb<sup>3+</sup>ions through the antenna effect. K<sub>2</sub>SiF<sub>6</sub>:Mn<sup>4+</sup>, on the other hand, has three excitation bands with maxima at 248, 354, and 454 nm which emit red light after excitation through these bands. NaYF<sub>4</sub>:Yb<sup>3+</sup>/Er<sup>3+</sup>is used as an upconverting nanophosphor showing green emission under 976 nm laser excitation. Thus, the multi-stimuli-responsive luminescent security ink shows greenish, red, and green emissions under 367 nm, 450 nm, and 976 nm excitations, respectively. Furthermore, the distinct lifetimes of the activators in Tb(ASA)<sub>3</sub>Phen and K<sub>2</sub>SiF<sub>6</sub>:Mn<sup>4+</sup>, i.e. 0.1708 ms and 8.165 ms, respectively, under 380 nm excitation make this ink suitable for dynamic anticounterfeiting as well. The ink shows a change in the emission color with time delay, after the removal of the 380 nm excitation source, from greenish yellow (at 0 delays) to reddish color after a delay of 7.5 ms. These unique optical features along with excellent photo-, chemical- and environmental stability make this ink useful for advanced-level anticounterfeiting.</p>","PeriodicalId":18596,"journal":{"name":"Methods and Applications in Fluorescence","volume":"11 2","pages":""},"PeriodicalIF":3.2,"publicationDate":"2023-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9118341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Tutorial: multiphoton microscopy to advance neuroscience research. 教程:多光子显微镜推进神经科学研究。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-02-22 DOI: 10.1088/2050-6120/acba66
Iván Coto Hernández, Jenny Yau, Lars Rishøj, Nanke Cui, Steven Minderler, Nate Jowett

Multiphoton microscopy (MPM) employs ultrafast infrared lasers for high-resolution deep three-dimensional imaging of live biological samples. The goal of this tutorial is to provide a practical guide to MPM imaging for novice microscopy developers and life-science users. Principles of MPM, microscope setup, and labeling strategies are discussed. Use of MPM to achieve unprecedented imaging depth of whole mounted explants and intravital imaging via implantable glass windows of the mammalian nervous system is demonstrated.

多光子显微镜(MPM)采用超快红外激光对活体生物样品进行高分辨率深三维成像。本教程的目标是为新手显微镜开发人员和生命科学用户提供MPM成像的实用指南。讨论了MPM的原理、显微镜设置和标记策略。利用MPM实现前所未有的全植体成像深度和通过哺乳动物神经系统植入式玻璃窗的活体成像。
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引用次数: 0
Enhanced emission intensity in (Li+/Ca2+/Bi3+) ions co-doped NaLa(MoO4)2: Dy3+phosphors and their Judd-Ofelt analysis for WLEDs applications. 增强(Li+/Ca2+/Bi3+)离子共掺杂的 NaLa(MoO4)2:Dy3+ 磷光体及其用于 WLED 应用的 Judd-Ofelt 分析。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-02-13 DOI: 10.1088/2050-6120/acbbb9
Sonali Sonali, C Shivakumara

In the present study, we have synthesized a series of Dy3+ ion doped NaLa(MoO4)2phosphors by the conventional solid-state method at 750 °C for 4h. All the compounds were crystallized in the tetragonal scheelite type structure with space group (I41/a, No.88). The morphology and functional group were confirmed by the field emission scanning electron microscopy (FE-SEM) and Fourier transform infrared(FTIR)spectroscopy. Upon near-Ultraviolet (n-UV) excitation, the PL spectra exhibit the two characteristic emissions of Dy3+ ions, blue (4F9/2→6H15/2) at 487 nm and yellow (4F9/2→6H13/2) at 574nm respectively. The optimum concentration of Dy3+ionis 3 mol% and then quenching occurred due to multipolar interaction. Further, enhanced the emission intensity by co-doping with monovalent (Li+), divalent (Ca2+) and trivalent (Bi3+) ions. Among them, Li+ ion co-doped samples are shown maximum intensity (50 times) more than Dy3+ doped phosphors as relaxation of parity restriction of electric dipole transition because of local distortion of crystal field around the Dy3+ ions. In addition, by incorporation of Eu3+ ions into NaLa(MoO4)2:Dy3+system, tuned the emission color from white to red, owing to energy transfer from Dy3+ to Eu3+ ions. The intensity parameters (Ω2, Ω4) and radiative properties such as transition probabilities (AT), radiative lifetime (rad), and branching ratio were calculated using the Judd-Ofelt theory. CIE color coordinates, CCT values indicates that these phosphors exhibit an excellent white emission. The determined radiative properties, CIE and CCT results revealed that the Dy3+-activated NaLa(MoO4)2phosphors are potential materials for developing white LEDs, and optoelectronic device fabrications.

在本研究中,我们采用传统固态法,在 750 ℃ 下 4 小时合成了一系列掺杂 Dy3+ 离子的 NaLa(MoO4)2磷酸盐。所有化合物均为四方白钨矿型结构,空间群为(I41/a,No.88)。通过场发射扫描电子显微镜(FE-SEM)和傅立叶变换红外光谱(FTIR)确认了化合物的形态和官能团。在近紫外(n-UV)激发下,PL 光谱显示出 Dy3+ 离子的两种特征发射,分别是 487 纳米波长处的蓝色(4F9/2→6H15/2)和 574 纳米波长处的黄色(4F9/2→6H13/2)。Dy3+ 离子的最佳浓度为 3 摩尔%,然后由于多极相互作用发生淬灭。此外,通过与一价(Li+)、二价(Ca2+)和三价(Bi3+)离子共掺杂,还能增强发射强度。其中,共掺杂 Li+ 离子的样品比掺杂 Dy3+ 离子的荧光粉显示出最大的发射强度(50 倍),这是因为 Dy3+ 离子周围的晶体场发生了局部畸变,从而放松了电偶极转换的奇偶性限制。此外,在 NaLa(MoO4)2:Dy3+ 系统中加入 Eu3+ 离子后,由于 Dy3+ 离子向 Eu3+ 离子的能量转移,发射颜色从白色变为红色。利用 Judd-Ofelt 理论计算了强度参数(Ω2、Ω4)以及过渡概率(AT)、辐射寿命(rad)和支化比等辐射特性。CIE 色坐标、CCT 值表明这些荧光粉具有极佳的白光发射性能。测定的辐射特性、CIE 和 CCT 结果表明,Dy3+ 激活的 NaLa(MoO4)2 磷光体是开发白光 LED 和制造光电器件的潜在材料。
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引用次数: 0
Effect of buffers and pH in antenna sensitized Eu(III) luminescence. 缓冲液和pH对天线敏化Eu(III)发光的影响。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-02-07 DOI: 10.1088/2050-6120/acb63a
Lea Gundorff Nielsen, Thomas Just Sørensen

The photophysics of a europium(III) complex of 1,4,7,10-tetraazacycododecane-1,4,7-triacetic acid-10-(2-methylene)-1-azathioxanthone was investigated in three buffer systems and at three pH values. The buffers-phosphate buffered saline (PBS), 4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid (HEPES), and universal buffer (UB)-had no effect on the europium luminescence, but a lower overall emission intensity was determined in HEPES. It was found that this was due to quenching of the 1-azathioxanthone first excited singlet state by HEPES. The effect of pH on the photophysics of the complex was found to be minimal, and protonation of the pyridine nitrogen was found to be irrelevant. Even so, pH was shown to change the intensity ratio between 1-azathioxanthone fluorescence and europium luminescence. It was concluded that the full photophysics of a potential molecular probe should be investigated to achieve the best possible results in any application.

研究了铕(III)配合物1,4,7,10-四氮杂环十二烷-1,4,7-三乙酸-10-(2-亚甲基)-1-偶氮杂氧蒽酮在三种缓冲体系和三种pH值下的光物理性质。磷酸盐缓冲盐水(PBS)、4-(2-羟乙基)-1-哌嗪乙磺酸(HEPES)和通用缓冲液(UB)对铕的发光没有影响,但HEPES的总发光强度较低。发现这是由于1-硫杂蒽酮被HEPES猝灭了第一激发单重态。pH值对配合物的光物理性质的影响很小,并且发现吡啶氮的质子化是无关的。尽管如此,pH值还是改变了1-硫杂蒽酮荧光与铕发光的强度比。结论是,为了在任何应用中获得最好的结果,应该研究潜在分子探针的全部光物理特性。
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引用次数: 2
Structural and optical variation of pseudoisocyanine aggregates nucleated on DNA substrates. 在DNA底物上成核的假异氰酸聚集体的结构和光学变化。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-01-31 DOI: 10.1088/2050-6120/acb2b4
Matthew Chiriboga, Christopher M Green, Divita Mathur, David A Hastman, Joseph S Melinger, Remi Veneziano, Igor L Medintz, Sebastián A Díaz

Coherently coupled pseudoisocyanine (PIC) dye aggregates have demonstrated the ability to delocalize electronic excitations and ultimately migrate excitons with much higher efficiency than similar designs where excitations are isolated to individual chromophores. Here, we report initial evidence of a new type of PIC aggregate, formed through heterogeneous nucleation on DNA oligonucleotides, displaying photophysical properties that differ significantly from previously reported aggregates. This new aggregate, which we call the super aggregate (SA) due to the need for elevated dye excess to form it, is clearly differentiated from previously reported aggregates by spectroscopic and biophysical characterization. In emission spectra, the SA exhibits peak narrowing and, in some cases, significant quantum yield variation, indicative of stronger coupling in cyanine dyes. The SA was further characterized with circular dichroism and atomic force microscopy observing unique features depending on the DNA substrate. Then by integrating an AlexaFluorTM647 (AF) dye as an energy transfer acceptor into the system, we observed mixed energy transfer characteristics using the different DNA. For example, SA formed with a rigid DNA double crossover tile (DX-tile) substrate resulted in AF emission sensitization. While SA formed with more flexible non-DX-tile DNA (i.e. duplex and single strand DNA) resulted in AF emission quenching. These combined characterizations strongly imply that DNA-based PIC aggregate properties can be controlled through simple modifications to the DNA substrate's sequence and geometry. Ultimately, we aim to inform rational design principles for future device prototyping. For example, one key conclusion of the study is that the high absorbance cross-section and efficient energy transfer observed with rigid substrates made for better photonic antennae, compared to flexible DNA substrates.

相干耦合假异氰酸(PIC)染料聚集体已经证明了离域电子激发的能力,并最终以比类似设计更高的效率迁移激子,其中激子被隔离到单个发色团。在这里,我们报告了一种新型PIC聚集体的初步证据,通过DNA寡核苷酸的异质成核形成,显示出与先前报道的聚集体显着不同的光物理性质。这种新的聚集体,我们称之为超级聚集体(SA),因为需要增加染料过量形成它,通过光谱和生物物理表征与以前报道的聚集体明显不同。在发射光谱中,SA表现出峰变窄,在某些情况下,显著的量子产率变化,表明在菁染料中偶联更强。进一步用圆二色性和原子力显微镜对SA进行表征,观察到DNA底物的独特特征。然后,通过将AlexaFluorTM647 (AF)染料作为能量转移受体整合到系统中,我们观察了不同DNA的混合能量转移特性。例如,由刚性DNA双交叉瓦(dx -瓦)底物形成的SA导致AF发射敏化。而SA由更灵活的非dx -tile DNA(即双链和单链DNA)形成,导致AF发射猝灭。这些综合表征强烈暗示,基于DNA的PIC聚合特性可以通过简单修改DNA底物的序列和几何形状来控制。最终,我们的目标是为未来的设备原型设计提供合理的设计原则。例如,该研究的一个关键结论是,与柔性DNA衬底相比,刚性衬底观察到的高吸光度横截面和有效的能量传递可以用于更好的光子天线。
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引用次数: 2
Pulse-shaped broadband multiphoton excitation for single-molecule fluorescence detection in the far field. 用于远场单分子荧光检测的脉冲型宽带多光子激发。
IF 3.2 3区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2023-01-19 DOI: 10.1088/2050-6120/aca87f
David Nobis, Henry G Sansom, Steven W Magennis
Multiphoton excitation of fluorescence has many potential advantages over resonant (one-photon) excitation, but the method has not found widespread use for ultrasensitive applications. We recently described an approach to the multiphoton excitation of single molecules that uses a pulse shaper to compress and tailor pulses from an ultrafast broadband laser in order to optimise the brightness and signal-to-background ratio following non-linear excitation. Here we provide a detailed description of the setup and illustrate its use and potential by optimising two-photon fluorescence of a common fluorophore, rhodamine 110, at the single-molecule level. We also show that a DNA oligonucleotide labelled with a fluorescent nucleobase analogue, tC, can be detected using two-photon FCS, whereas one-photon excitation causes rapid photobleaching. The ability to improve the signal-to-background ratio and to reduce the incident power required to attain a given brightness can be applied to the multiphoton excitation of any fluorescent species, from small molecules with low multiphoton cross sections to the brightest nanoparticles.
荧光的多光子激发与共振(单光子)激发相比具有许多潜在的优点,但该方法尚未广泛用于超灵敏应用。我们最近描述了一种单分子多光子激发的方法,该方法使用脉冲整形器压缩和定制来自超快宽带激光器的脉冲,以优化非线性激发后的亮度和信本比。在这里,我们提供了设置的详细描述,并通过优化普通荧光团罗丹明110在单分子水平上的双光子荧光来说明其使用和潜力。我们还表明,用荧光核碱基类似物tC标记的DNA寡核苷酸可以使用双光子FCS检测到,而单光子激发会导致快速光漂白。提高信号背景比和降低达到给定亮度所需的入射功率的能力可以应用于任何荧光物种的多光子激发,从具有低多光子横截面的小分子到最亮的纳米颗粒。
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引用次数: 1
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Methods and Applications in Fluorescence
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