JOURNAL OF PHYSICAL CHEMISTRY B
·
2023
·
IF 3.3
Meng Kou,Feng Qin,Yongda Wang,Xiyu Zhang,Zheng Hu,Zhiguo Zhang
Environmental heavy atoms can further enhance the room temperature phosphorescence (RTP) emissions of gadolinium-labeled hematoporphyrin monomethyl ether (Gd-HMME) by way of the external heavy atom effect (HAE). However, the macroscopic phosphorescence intensity covered the intrinsic effect of the environmental heavy atoms. In this study, a method of separating the external HAE from the total is performed, and a quantity to describe the intrinsic nature of external HAE is defined. The environmental Gd3+ concentration evolution of the phosphorescent transition rate (kP) is obtained by correlated absorption, emission, and time-resolved spectroscopy. The kP increases linearly with environmental Gd3+ concentration, while the intercept kP0 coincides with that of the internal HAE. The slope κ could be calculated, and it is a quantity free of the Gd3+ concentration and only relies on the type of environmental heavy atoms. In addition, the environmental Lu3+ exhibits similar functionality to Gd3+ in external HAE. Environmental Pd2+ quenches the phosphorescence intensity macroscopically, while it enhances the HAE intrinsically. Our method provides an alternative insight into the intrinsic nature of environmental heavy atoms.
研究领域:
化学
·
生物医学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Da Chen,Guangda Niu,Shiqiang Hao,Liubing Fan,Jing Zhao,Christopher Wolverton,Mengling Xia,Quanlin Liu
Halide double perovskites have attracted substantial attention for optoelectronic applications owing to their low toxicity and high stability. However, double perovskites have strict requirements in terms of the halide type, thus rendering many of their properties unchangeable, including the band gap, atomic number, and carrier transport. By introducing long-chain organic amines, the chloride site of double perovskites can be completely replaced by bromide. Using this strategy, two dimensions silver–indium–bromide double perovskites (PEA)4AgInBr8 and (i-BA)4AgInBr8 were successfully synthesized [(PEA)+ = C6H5(CH2)2NH3+, (i-BA)+ = CH(CH3)2CH2NH3+]. Density functional theory calculations and spectroscopy characterizations were performed to unveil the semiconducting behaviors and photoluminescence properties of the title compounds. Electrical characterization confirms their good carrier-transport property (μτ product: 2.0 × 10–3 cm2 V–1) and low dark current. Moreover, the presence of heavy atoms, together with the ultrastable baseline contributes to a high X-ray detection sensitivity (185 μC Gyair–1 cm–2), greater than that of most previous double-perovskite detectors. Our work lays the foundation for broadening the family of potential double perovskites, creating a new path for the realization of long-sought perovskites with low toxicity and high stability that retain good optoelectronic performance.
研究领域:
材料科学
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光学工程
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DOI
高影响因子
JOURNAL OF PORPHYRINS AND PHTHALOCYANINES
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2022
·Vol. 26
·期 12
·884-890
·
IF 1.914
Lixin Liu,Bo Han,Yu Cao,Jingji Wen
The room-temperature phosphorescence (RTP) of metalloporphyrins, induced by the heavy atom effect (HAE), has been widely concerned in many fields, and the intense emission of RTP is highly desired. The phosphorescent transition rate ( k P ) has been used to quantitatively characterize the HAE’s intrinsic nature. However, the phosphorescent intensity was not determined by k P alone, non-phosphorescent transition ( k n P ) induced by surrounding factors was also involved. In this study, the influence of k n P on the RTP of palladium octaethylporphyrin (PdOEP), platinum octaethylporphyrin (PtOEP), and platinum tetraphenylporphyrin (PtTPP) was studied. The effect of k n P can be quantitatively described by an introduced parameter η , which was defined as η = k P /( k P + k n P ) . The method is proposed for determining the η of PdOEP, PtOEP, and PtTPP by the UV-visible absorption spectra, luminescence spectra, and phosphorescence dynamic curves. Our research provides a way to understand the effect of knP on the RTP, and may benefit the development and optimization of metalloporphyrins aiming at intense RTP.
研究领域:
化学
·
材料科学
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Meng Kou,Feng Qin,Yongda Wang,Xiyu Zhang,Hua Zhao,Ye Tian,Zhiguo Zhang
The presence of room temperature phosphorescence emission in metalloporphyrin, via the transition from the excited triplet state (T1) to the ground state (S0), relies on the chelated heavy metal ions, which is known as the heavy atom effect (HAE). Despite the HAE being a reliable method to tune the phosphorescence process widely, the realization of the HAE nature is a tough task as the induced phosphorescence process is sensitive to not only the specie of bonded heavy atoms but also chemical environments such as the oxygen quenching and solvent effect. In this study, we have aimed at a quantitative determination of the intrinsic phosphorescent transition rate (kP) in metalloporphyrin gadolinium-labeled hematoporphyrin monomethyl ether (Gd-HMME). After the theoretical analysis based on the rate equation model to remove the nonintrinsic contribution and the experimental results of phosphorescence, the kP is calculated to be ∼2.4 × 10–4 μs–1. This study enables us to approach the intrinsic energy characteristic of metalloporphyrins; moreover, our work provides an effective pathway for the further optimization of the varied functional metalloporphyrin.
研究领域:
化学
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材料科学
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生物医学工程
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DOI
PubMed
高影响因子
DYES AND PIGMENTS
·
2024
·
IF 4.1
Tingwei Cai,Hanchang Hu,Qiangqiang Zhao,Zhong Zhang,Jinxin He
Fluorescein halogenated dyes are excellent photocatalysts for cross-dehydrogenation-coupled (CDC) reaction. In this paper, seven different halo-fluorescein dyes were selected to investigate the influence of heavy halogen atoms and proton concentrations on halo-fluoresceins for photocatalytic CDC reaction. The results showed that the heavy atoms directly affected intersystem crossing (ISC), which could act as a gatekeeper in the photoredox cycle and also affect photoinduced electron transfer (PET) process. Thus, the photocatalytic performance clearly increased in the following order: fluorescein FL (0.11 mol L −1 •h −1 )＜dibromo-fluorescein FL-2Br (0.19 mol L −1 •h −1 )＜diiodo-fluorescein FL-2I (0.29 mol L −1 •h −1 )＜tetrabromo-fluorescein FL-4Br (0.375 mol L −1 •h −1 )＜tetrabromo-tetrachloro-fluorescein FL-4Br–4Cl (0.53 mol L −1 •h −1 )＜tetraiodo-fluorescein FL-4I (0.58 mol L −1 •h −1 )＜ tetraiodo-tetrachloro-fluorescein FL-4I–4Cl (0.74 mol L −1 •h −1 ). Furthermore, the visible light absorption of halogenated fluorescein dyes varied significantly with pH, thereby affecting their photocatalytic activity of CDC reaction. The dianionic FL-4I–4Cl could fully absorb light energy and exhibit excellent photocatalytic performance under mildly alkaline conditions (pH = 8), achieving a CDC reaction conversion rate of 99.92 %, which was 2.6 times higher than that of the lactone form of FL-4I–4Cl under acidic conditions (pH = 2).
研究领域:
化学
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材料科学
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环境科学
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DOI
高影响因子
DALTON TRANSACTIONS
·
2017
·Vol. 46
·期 16
·5151-5158
·
IF 4.029
Enyi Chen,Xin Chen,Xiuxue Yuan,Shaohua Wei,Lin Zhou,Jiahong Zhou,Jian Shen
A facile and robust one-pot approach to prepare a theranostic nanoplatform, based on chelation between Gd3+ and hypericin photosensitizer (PS) and their controlled in situ hydrolysis precipitation, was developed. In this strategy, PS drugs and Gd3+ were directly used as building blocks to construct theranostic nanoparticles, resulting in a greatly increased active substance-loading efficiency and ensuring their theranostic effect. The resulting nanoparticles have multifunction capabilities for nuclear magnetic resonance (NMR) imaging and anticancer activity through adenosine triphosphate (ATP) deprivation and heavy atom effect (HAE)-improved photodynamic therapy (PDT) mechanisms.
研究领域:
医学影像学
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纳米医学
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肿瘤学
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DOI
PubMed
高影响因子
JOURNAL OF LUMINESCENCE
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2022
·
IF 4.171
Tianmou Xu,Peiqing Cai,Qi Ai,Qi He,Junjie Si,Xin Yao,Zugang Liu
Organometallic materials with room temperature phosphorescence (RTP) emission are of bright development prospects in optoelectronic application. Herein, we prepared two types of isostructural zero-dimensional metal-organic single crystals with RTP effect named as bis(tetraphenylphosphonium) titanium hexafluoride (Ph 4 P) 2 TiF 6 ·2H 2 O and bis(tetraphenylphosphonium) zirconium hexafluoride (Ph 4 P) 2 ZrF 6 ·2H 2 O. The as-prepared fluoride crystals can simultaneously emit ultraviolet (UV) fluorescence and green phosphorescent emission under 290 nm excitation at room temperature. The RTP could be observed by naked eyes for more than 6 s after removing the excited UV source . By introducing bromide ions into the crystal framework to enhance the heavy-atom effect, the photoluminescence quantum yield of the compounds dramatically boosted to 19.47%. These results provide a facile design strategy for the adjustment of efficient transient and long-lasting RTP. Furthermore, the as-prepared materials were blended in the resins and printed as the anti-counterfeiting signal labels. Therefore, this work does not only reveal the efficient RTP phenomenon in the zero-dimensional metal-organic ionic compounds , but also provide potential candidates for the realization of anti-counterfeiting technology.
研究领域:
材料科学
·
光学
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产品关联
DOI
高影响因子
DYES AND PIGMENTS
·
2021
·
IF 4.889
Hao Liu,Juanjuan Yin,Enyun Xing,Yingying Du,Yu Su,Yaqing Feng,Shuxian Meng
Cyanine dyes are widely used in the field of tumor phototherapy due to their excellent photophysical properties. To explore the heavy atoms effects on the photothermal and photodynamic performance of phototherapeutic agents, chlorine, bromine, and iodine were introduced to synthesize a series of cyanine dyes (IR6, IR7, and IR8). We have found that all halogenated cyanine dyes exhibited high excitation wavelength (around 800 nm) and low dark toxicity. Among them, IR8 behaved the best singlet oxygen production ability in the three dyes. For photothermal performance, IR8 exhibited the best photothermal conversion rate (46.6%), photothermal stability, and excellent therapy efficiency (half-maximal inhibitory concentration, IC 50 = 16.2 μg/mL). IR7 behaved a greater enhancement of the photothermal conversion rate (43.4%) than IR6 (42.3%). In conclusion, the heavy atoms effects on the photothermal and photodynamic properties of cyanine dyes are positively correlated with the increase of the atomic number of the halogen atom, and the iodine atom may be the most worthy of consideration in the all halogen atoms.
研究领域:
肿瘤学
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生物医学工程
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药理学
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DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Xiao-Shuo Wu,Ru Zhang,Jian-Lan Liu
A new 2D phosphorescence lead metal cluster-based coordination polymer (CP) [Pb 4 ( μ 2 -OH) ( μ 3 -OH) ( μ 4 -O) (3-qlc) 4 ] n ( 1 ; 3-qlc = 3-quinolinecarboxylate) has been successfully synthesized by solvothermal reaction. CP 1 is a robust Pb(II) CP constructed by a rare [Pb 8 ( μ 2 -OH) 2 ( μ 3 -OH) 2 ( μ 4 -O) 2 (COO) 8 ] cluster units and 3-qlc ligands. The bulky clusters provide architectural stability to the framework of 1 . Interestingly, CP 1 exhibited almost pure room-temperature orange phosphorescence with absolute phosphorescence quantum yields of 3.3% and a phosphorescence lifetime of 1.52 ms benefiting from the restriction of molecular vibrations/rotations of organic luminogens (3-qlc) and the heavy-atom effect of Pb(II).
研究领域:
材料化学
·
配位化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Tao Hua,Lisi Zhan,Nengquan Li,Zhongyan Huang,Xiaosong Cao,Zhengqi Xiao,Shaolong Gong,Changjiang Zhou,Cheng Zhong,Chuluo Yang
As one type of latest emitters with simultaneous high efficiency and color-purity, the development of multi-resonance thermally activated delayed fluorescence (MR-TADF) materials represents an important advancement for organic light-emitting diodes (OLEDs). We herein present a new strategy to improve the performance of MR-TADF emitters by fusing sulfur element into the B-N based framework, aiming to utilize the non-metal heavy-atom effect in accelerating the reverse intersystem crossing (RISC) process of the emitter. Two compounds, namely 2PTZBN and 2PXZBN, were developed in this work through rigidifying the DABNA-1 skeleton by sulfur or oxygen atoms. The theoretical calculations and photoluminescence studies reveal that the sulfur-incorporated 2PTZBN enable considerable rate constant of RISC ( k RISC ) up to 2.8 × 10 5 s −1 in toluene due to larger spin-orbital coupling (SOC) values and smaller singlet–triplet energy splitting (Δ E ST ) compared with 2PXZBN. Consequently, organic light-emitting diodes based on 2PTZBN exhibited highly efficient green emission with maximum external quantum efficiency (EQE) of 25.5%.
研究领域:
材料科学
·
光学
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Yu Zheng,Wanqing Liang,Xinyi Li,Cheng Zhang,Kui Zhang
The incorporation of heavy atoms into fluorescent emitters can efficiently facilitate spin-orbit coupling and enhance the intersystem crossing process from excited singlet states to triplet states. However, the introduction of heavy atoms into carbon dots (CDs) materials still remains challenges. In this work, CDs synthesized from polyethyleneimine and itaconic acid were subjected to a mild bromination process, yielding bromine-doped carbon dots (Br-CDs). Bromine atoms significantly enhanced the intersystem crossing process, leading to a 155.1 % increase in the phosphorescence intensity of the CDs. Moreover, the enhanced generation of excited triplet states endowed the Br-CDs with photosensitization performance, enabling them to produce singlet oxygen and superoxide anion radicals upon light irradiation. Interestingly, it was found that Cu 2+ ions could effectively inhibit this photosensitization process. By integrating the color changes of photosensitization oxidation substrates, a colorimetric method was developed for the rapid determination of Cu 2+ ion concentrations in water samples. This proposed method offers a novel approach for the design of sensors based on luminescent nanomaterials.
研究领域:
纳米材料
·
光化学
·
传感器
·
环境分析
·
荧光探针
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产品关联
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2024
·
IF 3.8
Liu Xuan,Cui Enna,Wang Mengxiao,Zhu Yujie,Li Hongliang,Guo Chao
We present a novel approach for iodide sensing based on the heavy-atom effect to quench the green fluorescent emission of organosilicon nanoparticles (OSiNPs). The fluorescence of OSiNPs was significantly quenched (up to 97.4% quenching efficiency) in the presence of iodide ions (I – ) through oxidation by hydrogen peroxide. Therefore, OSiNPs can serve as a fluorescent probe to detect I – with high selectivity and sensitivity. The highly selective response is attributed to the hydrophilic surface enabling good dispersion in aqueous solutions and the lipophilic core allowing the generated liposoluble I 2 to approach and quench the fluorescence of OSiNPs. The linear working range for I – was from 0 to 50 μM, with a detection limit of 0.1 μM. We successfully applied this nanosensor to determine iodine content in edible salt. Furthermore, the fluorescent OSiNPs can be utilized for the determination of total antioxidant capacity (TAC). Antioxidants reduce I 2 to I – , and the extent of quenching by the remaining I 2 on the OSiNPs indicates the TAC level. The responses to ascorbic acid, pyrogallic acid, and glutathione were investigated, and the detection limit for ascorbic acid was as low as 0.03 μM. It was applied to the determination of TAC in ascorbic acid tablets and fruit juices, indicating the potential application of the OSiNP-based I 2 sensing technique in the field of food analysis. Graphical Abstract
研究领域:
分析化学
·
纳米技术
·
传感器
·
食品科学
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产品关联
DOI
PubMed
高影响因子
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