Yanwei Feng, Yongfeng Yuan, Gaoshen Cai, Bingxu Wang, Jun Zhang, Yang Xia, Shaoyi Guo
Interfacial pH fluctuation is one of the primary reasons for issues related to Zn metal anodes. Herein, polar amphoteric alanine, as a multifunctional electrolyte additive, is designed to regulate the electric double layer (EDL) and solvation structure. Alanine with self-adaptation capability to pH can stabilize electrolyte pH. Due to more negative adsorption energy, alanine preferentially adsorbs on the Zn surface and repels water molecules within the EDL. Alanine-enriched EDL effectively shields the surface tips, homogenizes interfacial electric field distribution, and promotes preferential deposition of horizontal flaky Zn. Alanine-enriched EDL limits the contact between water and the Zn anode. Alanine additive decreases the quantity of water molecules in the Zn2+ solvation sheath and disrupts H-bond networks in the electrolyte. Consequently, a dense and textured Zn deposition is achieved. Corrosion and side reactions are suppressed. Cycling stability of symmetrical cells attains 2700 h at 3 mA cm−2/1 mAh cm−2 and 2050 h at 5 mA cm−2/1 mAh cm−2. Average coulombic efficiency reaches 99.8% over 4500 cycles at 5 mA cm−2/1 mAh cm−2. Even within KOH alkaline electrolytes, alanine additive still improves the cycling lifespan of symmetrical cells to 100 h at 0.5 mA cm−2/0.5 mAh cm−2.
界面 pH 值波动是造成锌金属阳极相关问题的主要原因之一。在此，极性两性丙氨酸作为一种多功能电解质添加剂，旨在调节电双层（EDL）和溶解结构。具有 pH 自适应能力的丙氨酸可以稳定电解质的 pH 值。由于丙氨酸具有更高的负吸附能，它能优先吸附在 Zn 表面，并排斥 EDL 中的水分子。富含丙氨酸的 EDL 能有效屏蔽表面尖端，均匀界面电场分布，促进水平片状 Zn 的优先沉积。富含丙氨酸的 EDL 限制了水与锌阳极之间的接触。丙氨酸添加剂会减少 Zn2+ 溶剂鞘中的水分子数量，并破坏电解质中的氢键网络。因此，可以实现致密、纹理清晰的锌沉积。腐蚀和副反应受到抑制。对称电池在 3 mA cm-2/1 mAh cm-2 条件下的循环稳定性达到 2700 小时，在 5 mA cm-2/1 mAh cm-2 条件下达到 2050 小时。在 5 mA cm-2/1 mAh cm-2 条件下循环 4500 次，平均库仑效率达到 99.8%。即使在 KOH 碱性电解质中，丙氨酸添加剂仍可将对称电池的循环寿命提高到 100 小时（0.5 mA cm-2/0.5 mAh cm-2）。
{"title":"Multifunctional Amphoteric Additive Alanine Enables High-Performance Wide-pH Zn Metal Anodes","authors":"Yanwei Feng, Yongfeng Yuan, Gaoshen Cai, Bingxu Wang, Jun Zhang, Yang Xia, Shaoyi Guo","doi":"10.1002/smll.202405144","DOIUrl":"https://doi.org/10.1002/smll.202405144","url":null,"abstract":"Interfacial pH fluctuation is one of the primary reasons for issues related to Zn metal anodes. Herein, polar amphoteric alanine, as a multifunctional electrolyte additive, is designed to regulate the electric double layer (EDL) and solvation structure. Alanine with self-adaptation capability to pH can stabilize electrolyte pH. Due to more negative adsorption energy, alanine preferentially adsorbs on the Zn surface and repels water molecules within the EDL. Alanine-enriched EDL effectively shields the surface tips, homogenizes interfacial electric field distribution, and promotes preferential deposition of horizontal flaky Zn. Alanine-enriched EDL limits the contact between water and the Zn anode. Alanine additive decreases the quantity of water molecules in the Zn<sup>2+</sup> solvation sheath and disrupts H-bond networks in the electrolyte. Consequently, a dense and textured Zn deposition is achieved. Corrosion and side reactions are suppressed. Cycling stability of symmetrical cells attains 2700 h at 3 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup> and 2050 h at 5 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup>. Average coulombic efficiency reaches 99.8% over 4500 cycles at 5 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup>. Even within KOH alkaline electrolytes, alanine additive still improves the cycling lifespan of symmetrical cells to 100 h at 0.5 mA cm<sup>−2</sup>/0.5 mAh cm<sup>−2</sup>.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"65 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601549","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1016/j.cej.2024.157656
Junpeng Jiang, Liwen Yan, Jiangtao Li, Yunjia Xue, Chensi Zhang, Xiaoxia Hu, Anran Guo, Haiyan Du, Jiachen Liu
Owing to tunable dielectric properties, light weight and high porosity, polymer-derived SiBCN ceramic aerogels possess significant application prospects in electromagnetic wave (EMW) absorption and thermal insulation. However, due to inadequate oxidation resistance, the structural collapse and performance deterioration of SiBCN aerogels will easily occur in high-temperature aerobic environments, limiting their application. Herein, to address this issue, a novel and straightforward strategy based on typical polymer-derived-ceramic (PDC) aerogel method and impregnation with boehmite sol was proposed for synthesizing SiBCN/Al2O3 composite ceramic aerogels. The microstructure, phase composition, thermal insulation, oxidation resistance and EMW absorption properties of SiBCN/Al2O3 ceramic aerogels were investigated. The resulting SiBCN/Al2O3 composite aerogel demonstrates superior high-temperature structural stability, exhibiting an ultra-low linear shrinkage of only 6.5 % following heat treatment at 1200 °C for 2 h in air. Additionally, the composite aerogel shows a low thermal conductivity of 0.039 W/mK and a low density of 0.112 g/cm3. The SiBCN/Al2O3 composite aerogel, composed of dielectric SiBCN, conductive free carbon, and insulating alumina, demonstrates outstanding EMW absorption properties with a minimum reflection loss of −48.6 dB and an effective bandwidth of 5.8 GHz. The enhanced microwave absorption performance is mainly attributed to the improved impedance matching, multiple reflection, and enhanced interfacial polarization resulting from the introduction of Al2O3. Given prominent oxidation resistance, thermal insulation and EMW absorption properties, the SiBCN/Al2O3 composite aerogel paves the way for developing microwave absorption and thermal insulation integrated material in high-speed vehicles.
{"title":"Lightweight, thermally insulating SiBCN/Al2O3 ceramic aerogel with enhanced high-temperature resistance and electromagnetic wave absorption performance","authors":"Junpeng Jiang, Liwen Yan, Jiangtao Li, Yunjia Xue, Chensi Zhang, Xiaoxia Hu, Anran Guo, Haiyan Du, Jiachen Liu","doi":"10.1016/j.cej.2024.157656","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157656","url":null,"abstract":"Owing to tunable dielectric properties, light weight and high porosity, polymer-derived SiBCN ceramic aerogels possess significant application prospects in electromagnetic wave (EMW) absorption and thermal insulation. However, due to inadequate oxidation resistance, the structural collapse and performance deterioration of SiBCN aerogels will easily occur in high-temperature aerobic environments, limiting their application. Herein, to address this issue, a novel and straightforward strategy based on typical polymer-derived-ceramic (PDC) aerogel method and impregnation with boehmite sol was proposed for synthesizing SiBCN/Al<sub>2</sub>O<sub>3</sub> composite ceramic aerogels. The microstructure, phase composition, thermal insulation, oxidation resistance and EMW absorption properties of SiBCN/Al<sub>2</sub>O<sub>3</sub> ceramic aerogels were investigated. The resulting SiBCN/Al<sub>2</sub>O<sub>3</sub> composite aerogel demonstrates superior high-temperature structural stability, exhibiting an ultra-low linear shrinkage of only 6.5 % following heat treatment at 1200 °C for 2 h in air. Additionally, the composite aerogel shows a low thermal conductivity of 0.039 W/mK and a low density of 0.112 g/cm<sup>3</sup>. The SiBCN/Al<sub>2</sub>O<sub>3</sub> composite aerogel, composed of dielectric SiBCN, conductive free carbon, and insulating alumina, demonstrates outstanding EMW absorption properties with a minimum reflection loss of −48.6 dB and an effective bandwidth of 5.8 GHz. The enhanced microwave absorption performance is mainly attributed to the improved impedance matching, multiple reflection, and enhanced interfacial polarization resulting from the introduction of Al<sub>2</sub>O<sub>3</sub>. Given prominent oxidation resistance, thermal insulation and EMW absorption properties, the SiBCN/Al<sub>2</sub>O<sub>3</sub> composite aerogel paves the way for developing microwave absorption and thermal insulation integrated material in high-speed vehicles.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"157 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601370","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qinhui Bao, Chuwu Xing, Miao He, Zhiwei Nie, Rihua Wang, Chunsheng Wan, Tianjin Zhang, Duofa Wang
The subsurface of perovskite (PVK) triggers non-radiative recombination and initiates film degradation due to the impurities and defects. This study investigates the limitations of the conventional surface post-treatment and proposes an innovative pre-treatment strategy to achieve complete impurity elimination and defect passivation of the subsurface. The considerable activity of unannealed PVK films provides a sufficient basis for effective subsurface modification. Following the pre-treatment, the cadmium ions (Cd2+) can occupy the lead (Pb) vacancies or substitute lead ions(Pb2+), while the introduced ionic ions (I-) are able to fill the ionic (I) vacancies. The stronger ionic bond between Cd2+ and I− helps prevent the loss of I-, leading to a reduction of defects in film, inhibiting non-radiative recombination and ionic migration at the interface. This innovative strategy successfully eliminates impurities and passivates defects, resulting in a perovskite subsurface characterized by high crystallinity, low defect density, and minimal impurity. These enhancements contribute to enhanced open circuit voltage (VOC)and fill factor (FF), leading to an impressive power conversion efficiency (PCE) of 24.49%. Notably, after 1600 h of aging in ambient air, the cell retained 87% of its initial performance.
{"title":"High-Quality Subsurface Construction of Perovskite Film for Efficient and Stable Solar Cells","authors":"Qinhui Bao, Chuwu Xing, Miao He, Zhiwei Nie, Rihua Wang, Chunsheng Wan, Tianjin Zhang, Duofa Wang","doi":"10.1002/smll.202406386","DOIUrl":"https://doi.org/10.1002/smll.202406386","url":null,"abstract":"The subsurface of perovskite (PVK) triggers non-radiative recombination and initiates film degradation due to the impurities and defects. This study investigates the limitations of the conventional surface post-treatment and proposes an innovative pre-treatment strategy to achieve complete impurity elimination and defect passivation of the subsurface. The considerable activity of unannealed PVK films provides a sufficient basis for effective subsurface modification. Following the pre-treatment, the cadmium ions (Cd<sup>2+</sup>) can occupy the lead (Pb) vacancies or substitute lead ions(Pb<sup>2+</sup>), while the introduced ionic ions (I<sup>-</sup>) are able to fill the ionic (I) vacancies. The stronger ionic bond between Cd<sup>2+</sup> and I<sup>−</sup> helps prevent the loss of I<sup>-</sup>, leading to a reduction of defects in film, inhibiting non-radiative recombination and ionic migration at the interface. This innovative strategy successfully eliminates impurities and passivates defects, resulting in a perovskite subsurface characterized by high crystallinity, low defect density, and minimal impurity. These enhancements contribute to enhanced open circuit voltage (V<sub>OC</sub>)and fill factor (FF), leading to an impressive power conversion efficiency (PCE) of 24.49%. Notably, after 1600 h of aging in ambient air, the cell retained 87% of its initial performance.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"17 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610452","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Carrier selective contacts with passivation effects are considered to have a significant influence on the performance of crystalline silicon (c-Si) solar cells. It is essential for electron selective contact materials to meet the requirements of ultra-low contact resistance and excellent passivation effects. This work introduces a stack layer of Lithium Phosphate (Li3PO4) /Titanium Dioxide (TiO2) as a new electron selective passivating contact. It is found that the stack achieves an impressive contact resistivity (ρc) of 0.128 mΩ cm2 on n-type c-Si substrates with resistivity ranging from 1 to 3 Ω cm (14.6 mΩ cm2 for the n-Si/a-Si:H/Li3PO4/TiO2/Al contact). Furthermore, it effectively reduces the surface recombination parameter (J0) to less than 4 fA by incorporating a 6 nm a-Si:H(i) layer. The characterization of the n-Si/Li3PO4/TiO2 interface reveals that phosphorus diffusion into silicon plays a crucial role in achieving the ultra-low contact resistivity, while the presence of PO43− groups helps in fixing hydrogen atoms to maintain the desired chemical passivation effect. Finally, a silicon heterojunction solar cell (SHJ) with a rear full-area configuration of a-Si:H/Li3PO4/TiO2/Al is successfully demonstrated achieving an impressive power conversion efficiency of 22.89%. The result proves the efficacy of employing hydrogen-rich low-work function metal oxide stacks as electron selective passivating contacts.
{"title":"Self-Diffusion Effect Assisted TiO2/Li3PO4 Electron Selective Passivating Contact in Silicon Solar Cells Approaching 23% Efficiency","authors":"Zhiyuan Xu, Yu Yan, Wei Li, Qianfeng Gao, Yaya Song, Maobin Zhang, Junming Xue, Huizhi Ren, Shengzhi Xu, Xinliang Chen, Yi Ding, Qian Huang, Xiaodan Zhang, Ying Zhao, Guofu Hou","doi":"10.1002/smll.202407398","DOIUrl":"https://doi.org/10.1002/smll.202407398","url":null,"abstract":"Carrier selective contacts with passivation effects are considered to have a significant influence on the performance of crystalline silicon (c-Si) solar cells. It is essential for electron selective contact materials to meet the requirements of ultra-low contact resistance and excellent passivation effects. This work introduces a stack layer of Lithium Phosphate (Li<sub>3</sub>PO<sub>4</sub>) /Titanium Dioxide (TiO<sub>2</sub>) as a new electron selective passivating contact. It is found that the stack achieves an impressive contact resistivity (<i>ρ</i><sub>c</sub>) of 0.128 mΩ cm<sup>2</sup> on n-type c-Si substrates with resistivity ranging from 1 to 3 Ω cm (14.6 mΩ cm<sup>2</sup> for the n-Si/a-Si:H/Li<sub>3</sub>PO<sub>4</sub>/TiO<sub>2</sub>/Al contact). Furthermore, it effectively reduces the surface recombination parameter (<i>J</i><sub>0</sub>) to less than 4 fA by incorporating a 6 nm a-Si:H(i) layer. The characterization of the n-Si/Li<sub>3</sub>PO<sub>4</sub>/TiO<sub>2</sub> interface reveals that phosphorus diffusion into silicon plays a crucial role in achieving the ultra-low contact resistivity, while the presence of PO<sub>4</sub><sup>3−</sup> groups helps in fixing hydrogen atoms to maintain the desired chemical passivation effect. Finally, a silicon heterojunction solar cell (SHJ) with a rear full-area configuration of a-Si:H/Li<sub>3</sub>PO<sub>4</sub>/TiO<sub>2</sub>/Al is successfully demonstrated achieving an impressive power conversion efficiency of 22.89%. The result proves the efficacy of employing hydrogen-rich low-work function metal oxide stacks as electron selective passivating contacts.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"13 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1021/acschemneuro.4c00369
A N Resmi, Shaiju S Nazeer, M E Dhushyandhun, Willi Paul, Binu P Chacko, Ramshekhar N Menon, Ramapurath S Jayasree
Accurate and early disease detection is crucial for improving patient care, but traditional diagnostic methods often fail to identify diseases in their early stages, leading to delayed treatment outcomes. Early diagnosis using blood derivatives as a source for biomarkers is particularly important for managing Alzheimer's disease (AD). This study introduces a novel approach for the precise and ultrasensitive detection of multiple core AD biomarkers (Aβ40, Aβ42, p-tau, and t-tau) using surface-enhanced Raman spectroscopy (SERS) combined with machine-learning algorithms. Our method employs an antibody-immobilized aluminum SERS substrate, which offers high precision, sensitivity, and accuracy. The platform achieves an impressive detection limit in the attomolar (aM) range and spans a wide dynamic range from aM to micromolar (μM) concentrations. This ultrasensitive and specific SERS immunoassay platform shows promise for identifying mild cognitive impairment (MCI), a potential precursor to AD, from blood plasma. Machine-learning algorithms applied to the spectral data enhance the differentiation of MCI from AD and healthy controls, yielding excellent sensitivity and specificity. Our integrated SERS-machine-learning approach, with its interpretability, advances AD research and underscores the effectiveness of a cost-efficient, easy-to-prepare Al-SERS substrate for clinical AD detection.
{"title":"Ultrasensitive Detection of Blood-Based Alzheimer's Disease Biomarkers: A Comprehensive SERS-Immunoassay Platform Enhanced by Machine Learning.","authors":"A N Resmi, Shaiju S Nazeer, M E Dhushyandhun, Willi Paul, Binu P Chacko, Ramshekhar N Menon, Ramapurath S Jayasree","doi":"10.1021/acschemneuro.4c00369","DOIUrl":"https://doi.org/10.1021/acschemneuro.4c00369","url":null,"abstract":"<p><p>Accurate and early disease detection is crucial for improving patient care, but traditional diagnostic methods often fail to identify diseases in their early stages, leading to delayed treatment outcomes. Early diagnosis using blood derivatives as a source for biomarkers is particularly important for managing Alzheimer's disease (AD). This study introduces a novel approach for the precise and ultrasensitive detection of multiple core AD biomarkers (Aβ<sub>40</sub>, Aβ<sub>42</sub>, p-tau, and t-tau) using surface-enhanced Raman spectroscopy (SERS) combined with machine-learning algorithms. Our method employs an antibody-immobilized aluminum SERS substrate, which offers high precision, sensitivity, and accuracy. The platform achieves an impressive detection limit in the attomolar (aM) range and spans a wide dynamic range from aM to micromolar (μM) concentrations. This ultrasensitive and specific SERS immunoassay platform shows promise for identifying mild cognitive impairment (MCI), a potential precursor to AD, from blood plasma. Machine-learning algorithms applied to the spectral data enhance the differentiation of MCI from AD and healthy controls, yielding excellent sensitivity and specificity. Our integrated SERS-machine-learning approach, with its interpretability, advances AD research and underscores the effectiveness of a cost-efficient, easy-to-prepare Al-SERS substrate for clinical AD detection.</p>","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":" ","pages":""},"PeriodicalIF":4.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The development of near-infrared (NIR) luminescent materials featuring high photoluminescence quantum yield (ΦPL) at aggregated state is of great significance for achieving highly efficient non-doped organic light-emitting diodes (OLEDs) but remains formidable challenging. Herein, a design strategy of introducing electron-rich thiophene groups between electron acceptor and donor is proposed for efficient NIR luminescent materials, and a tailored D-π-A-π-D type emitter, namely, 4,4′-(benzo[c][1], [2], [5]thiadiazole-4,7-diylbis(thiophene-5,2-diyl))bis(N,N-diphenylaniline) (TPATBT), is designed and prepared. The photophysical investigation and density functional theory analysis disclose that TPATBT is a hot exciton emitter feature with hybridized local and charge-transfer state. Additionally, TPATBT demonstrates aggregation-induced emission characteristic, prefers high thermal stability, and exhibits a strong emission at 692 nm with a decent ΦPL of 20 % in the neat film. The non-doped device based on TPATBT neat film presents a maximum external quantum efficiency (ηext,max) of 1.22 % with electroluminescence peak at 718n m. Moreover, we first try to use interlayer sensitization to sensitize non-doped devices, which achieves better ηext,max of 1.34 % with low turn-on voltage of 3.2 V. The proposed molecular design strategy in this work is promising for exploring robust NIR luminescent materials for high-performance OLEDs.
{"title":"Introducing electron-rich thiophene bridges in hot exciton emitter for efficient non-Doped near-infrared OLEDs with low turn-on voltages","authors":"Ruming Jiang, Zhangshan Liu, Yuanyuan Han, Jiawei Long, Ting Guo, Xia Lan, Mingguang Yu, Ting Fan, Haijun Ma, Yen Wei, Ben Zhong Tang, Zujin Zhao","doi":"10.1016/j.cej.2024.157575","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157575","url":null,"abstract":"The development of near-infrared (NIR) luminescent materials featuring high photoluminescence quantum yield (Φ<sub>PL</sub>) at aggregated state is of great significance for achieving highly efficient non-doped organic light-emitting diodes (OLEDs) but remains formidable challenging. Herein, a design strategy of introducing electron-rich thiophene groups between electron acceptor and donor is proposed for efficient NIR luminescent materials, and a tailored D-π-A-π-D type emitter, namely, 4,4′-(benzo[c]<span><span>[1]</span></span>, <span><span>[2]</span></span>, <span><span>[5]</span></span>thiadiazole-4,7-diylbis(thiophene-5,2-diyl))bis(N,N-diphenylaniline) (TPATBT), is designed and prepared. The photophysical investigation and density functional theory analysis disclose that TPATBT is a hot exciton emitter feature with hybridized local and charge-transfer state. Additionally, TPATBT demonstrates aggregation-induced emission characteristic, prefers high thermal stability, and exhibits a strong emission at 692 nm with a decent Φ<sub>PL</sub> of 20 % in the neat film. The non-doped device based on TPATBT neat film presents a maximum external quantum efficiency (η<sub>ext,max</sub>) of 1.22 % with electroluminescence peak at 718n m. Moreover, we first try to use interlayer sensitization to sensitize non-doped devices, which achieves better η<sub>ext,max</sub> of 1.34 % with low turn-on voltage of 3.2 V. The proposed molecular design strategy in this work is promising for exploring robust NIR luminescent materials for high-performance OLEDs.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"10 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tong Wu, Xueqian Zhang, Quan Xu, Lehui Wang, Yao Li, Xiaohan Jiang, Qingwei Wang, Weili Zhang, Jiaguang Han
The ability to achieve independent complex amplitude control across multiple channels can significantly increase the information capacity of photonic devices. Diffraction inherently holds numerous channels, which are good candidates for dense light manipulation in angular space. However, no convenient method is currently available for attaining this. Here, a flexible interference approach utilizing silicon-based transmission-type heterogeneous-gradient supercell metasurfaces is proposed. By simply designing the phases of the meta-atoms’ radiations within a supercell, the complex amplitude of each diffraction channel can be individually and analytically controlled. Crucially, the complex amplitudes of multiple diffraction channels can be simultaneously controlled in a non-interleaved manner, where the number of channels is determined by the number of effective adjusting degrees of freedom (DoF). As a proof-of-concept validation, several meta-devices are experimentally demonstrated in the terahertz regime, which can generate multiple vortex beams, focal points, and splitting beams in different desired diffraction angles. This advancement heralds a new pathway for the development of multifunctional photonic devices with enhanced channel capacity, offering significant potential for both research and practical applications in photonics.
{"title":"Heterogeneous-Gradient Supercell Metasurfaces for Independent Complex Amplitude Control over Multiple Diffraction Channels","authors":"Tong Wu, Xueqian Zhang, Quan Xu, Lehui Wang, Yao Li, Xiaohan Jiang, Qingwei Wang, Weili Zhang, Jiaguang Han","doi":"10.1002/smll.202407303","DOIUrl":"https://doi.org/10.1002/smll.202407303","url":null,"abstract":"The ability to achieve independent complex amplitude control across multiple channels can significantly increase the information capacity of photonic devices. Diffraction inherently holds numerous channels, which are good candidates for dense light manipulation in angular space. However, no convenient method is currently available for attaining this. Here, a flexible interference approach utilizing silicon-based transmission-type heterogeneous-gradient supercell metasurfaces is proposed. By simply designing the phases of the meta-atoms’ radiations within a supercell, the complex amplitude of each diffraction channel can be individually and analytically controlled. Crucially, the complex amplitudes of multiple diffraction channels can be simultaneously controlled in a non-interleaved manner, where the number of channels is determined by the number of effective adjusting degrees of freedom (DoF). As a proof-of-concept validation, several meta-devices are experimentally demonstrated in the terahertz regime, which can generate multiple vortex beams, focal points, and splitting beams in different desired diffraction angles. This advancement heralds a new pathway for the development of multifunctional photonic devices with enhanced channel capacity, offering significant potential for both research and practical applications in photonics.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"4 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599938","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yueyue Wei, Yao Yang, Yuanyuan Du, Ning Zeng, Ziqiu Chen, Bowen Liu
Plasmonic nanolasers, which are promising coherent light sources for integrated photonics, super-resolution imaging, and ultrasensitive sensing applications, face the challenge of high thresholds due to inherent losses in plasmonic nanocavities. While considerable efforts have been made to improve the Q factor, typically quantified by the full width at half maximum (FWHM), intensity (ΔI) is another critical feature of plasmonic resonance. However, the combined influence of both the Q factor and resonance intensity of a plasmonic nanocavity on nanolasing threshold has not been sufficiently explored, as experimentally controlling one variable while keeping the other constant is challenging. Here, an ultra-low threshold plasmonic nanolaser is demonstrated by systematically optimizing the plasmonic nanocavity. By carefully controlling both the FWHMs and resonance intensities of the plasmonic resonators, a record low threshold of 2.6 µJ cm−2 for a dye-based nanolaser is achieved at room temperature– an order of magnitude lower than previous records. In addition, nanolasing under continuous-wave (CW) excitation is reported at room temperature gained by the same dye molecule. The results provide new insights into the design of high-performance plasmonic nanolasers and offer a promising path toward realizing applications of nanoscale coherent light sources.
{"title":"A CW-Pumped Dye Nanolaser With an Optimized Nanocavity","authors":"Yueyue Wei, Yao Yang, Yuanyuan Du, Ning Zeng, Ziqiu Chen, Bowen Liu","doi":"10.1002/smll.202410019","DOIUrl":"https://doi.org/10.1002/smll.202410019","url":null,"abstract":"Plasmonic nanolasers, which are promising coherent light sources for integrated photonics, super-resolution imaging, and ultrasensitive sensing applications, face the challenge of high thresholds due to inherent losses in plasmonic nanocavities. While considerable efforts have been made to improve the <i>Q</i> factor, typically quantified by the full width at half maximum (<i>FWHM</i>), intensity (<i>ΔI</i>) is another critical feature of plasmonic resonance. However, the combined influence of both the <i>Q</i> factor and resonance intensity of a plasmonic nanocavity on nanolasing threshold has not been sufficiently explored, as experimentally controlling one variable while keeping the other constant is challenging. Here, an ultra-low threshold plasmonic nanolaser is demonstrated by systematically optimizing the plasmonic nanocavity. By carefully controlling both the <i>FWHMs</i> and resonance intensities of the plasmonic resonators, a record low threshold of 2.6 µJ cm<sup>−2</sup> for a dye-based nanolaser is achieved at room temperature– an order of magnitude lower than previous records. In addition, nanolasing under continuous-wave (CW) excitation is reported at room temperature gained by the same dye molecule. The results provide new insights into the design of high-performance plasmonic nanolasers and offer a promising path toward realizing applications of nanoscale coherent light sources.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"80 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiang Qianqian, Wang He, Yang Kaiguang, Zhao Baofeng, Liang Zhen, Zhang Yukui, Jiang Bo, Zhang Lihua
Photocatalytic proximity labeling has shown great promise for mapping the spatiotemporal dynamics of surfaceome. Although cell-surface targeting photosensitizers relying on antibodies, lipid molecules, and metabolic labeling have gained effects, the development of simpler and stable methods that avoid complex chemical synthesis and biosynthesis steps is still a huge challenge. Here, the study has introduced 2D nanomaterials with the ability of cell surface engineering to perform the in situ anchoring of photosensitizer on living cell surface. Photosensitizer can be stabilized on nanomaterials by coordination after one-step mixing, resulting in the nano-photosensitizer combining cell surface targeting ability and photosensitivity that allowing surface-specific proximity labeling. Nano-photosensitizer can be dispersed stably in aqueous solution, avoiding the defects of poor water solubility and aggregation of traditional organic photosensitizers. Singlet oxygen is generated locally under light irradiation, enabling spatiotemporally-resolved activating and labeling of cell surface proteome. Further application in the brain metastatic lung cancer has been found effective with numerous quantified differential cell surfaces proteins highly correlated with cancer metastasis and three potential players have been validated via immunoblotting and immunofluorescence, providing important insights for metastasis supported molecular mechanism.
{"title":"2D Nano-Photosensitizer Facilitates Proximity Labeling for Living Cells Surfaceome Deciphering","authors":"Jiang Qianqian, Wang He, Yang Kaiguang, Zhao Baofeng, Liang Zhen, Zhang Yukui, Jiang Bo, Zhang Lihua","doi":"10.1002/smll.202407240","DOIUrl":"https://doi.org/10.1002/smll.202407240","url":null,"abstract":"Photocatalytic proximity labeling has shown great promise for mapping the spatiotemporal dynamics of surfaceome. Although cell-surface targeting photosensitizers relying on antibodies, lipid molecules, and metabolic labeling have gained effects, the development of simpler and stable methods that avoid complex chemical synthesis and biosynthesis steps is still a huge challenge. Here, the study has introduced 2D nanomaterials with the ability of cell surface engineering to perform the in situ anchoring of photosensitizer on living cell surface. Photosensitizer can be stabilized on nanomaterials by coordination after one-step mixing, resulting in the nano-photosensitizer combining cell surface targeting ability and photosensitivity that allowing surface-specific proximity labeling. Nano-photosensitizer can be dispersed stably in aqueous solution, avoiding the defects of poor water solubility and aggregation of traditional organic photosensitizers. Singlet oxygen is generated locally under light irradiation, enabling spatiotemporally-resolved activating and labeling of cell surface proteome. Further application in the brain metastatic lung cancer has been found effective with numerous quantified differential cell surfaces proteins highly correlated with cancer metastasis and three potential players have been validated via immunoblotting and immunofluorescence, providing important insights for metastasis supported molecular mechanism.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"61 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599941","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Poly(heptazine imide) (PHI) salts are extensively researched crystalline carbon nitride photocatalysts, but their photocatalytic water oxidation (PWO) performance is scarcely researched because of the difficulty in creating efficient active sites. Interference of metal ion (e.g., Na+ and K+) loss from the PHI salts in their PWO research has hardly been considered. Herein, metal single atom─OH (e.g., Co─OH) groups are incorporated into PHI to create efficient PWO active sites, via simple ion metathesis, hydrolysis, and deprotonation. The Co─OH modified PHI exhibits 9.3-fold higher PWO (oxygen evolution) activity than PHI, with an external quantum yield reaching 0.44% even at 600 nm. Excluding interference of the metal ion loss, the function of the Co─OH incorporation is evidenced mainly to facilitate the oxygen evolution reaction, as well as to promote photogenerated charge separation and raise visible light absorption, with the role of the OH especially revealed. Moreover, it is discovered that Na+ loss from sodium PHI will decrease its PWO activity, protonation of PHI has a detrimental effect on its PWO performance, and some other metal single atom─OH incorporation in PHI can also enhance its PWO activity. Overall, this work provides a general way to create PWO active sites in PHI.
{"title":"Metal Single Atom-Hydroxyl Incorporation in Poly(heptazine imide) to Create Active Sites for Photocatalytic Water Oxidation","authors":"Wenxuan Hu, Aifeng Li, Haiping Li, Yu Wang, Zhenke Fan, Quanhua Deng, Guoan Wang, Yuguo Xia, Wanguo Hou","doi":"10.1002/smll.202408436","DOIUrl":"https://doi.org/10.1002/smll.202408436","url":null,"abstract":"Poly(heptazine imide) (PHI) salts are extensively researched crystalline carbon nitride photocatalysts, but their photocatalytic water oxidation (PWO) performance is scarcely researched because of the difficulty in creating efficient active sites. Interference of metal ion (e.g., Na<sup>+</sup> and K<sup>+</sup>) loss from the PHI salts in their PWO research has hardly been considered. Herein, metal single atom─OH (e.g., Co─OH) groups are incorporated into PHI to create efficient PWO active sites, via simple ion metathesis, hydrolysis, and deprotonation. The Co─OH modified PHI exhibits 9.3-fold higher PWO (oxygen evolution) activity than PHI, with an external quantum yield reaching 0.44% even at 600 nm. Excluding interference of the metal ion loss, the function of the Co─OH incorporation is evidenced mainly to facilitate the oxygen evolution reaction, as well as to promote photogenerated charge separation and raise visible light absorption, with the role of the OH especially revealed. Moreover, it is discovered that Na<sup>+</sup> loss from sodium PHI will decrease its PWO activity, protonation of PHI has a detrimental effect on its PWO performance, and some other metal single atom─OH incorporation in PHI can also enhance its PWO activity. Overall, this work provides a general way to create PWO active sites in PHI.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"18 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599901","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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