Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Yang Ruixin,Cai Yanming,Qi Yongbing,Tang Zhuodong,Zhu Jun-Jie,Li Jinxiang,Zhu Wenlei,Chen Zixuan
C–C coupling is of utmost importance in the electrocatalytic reduction of CO 2 , as it governs the selectivity of diverse product formation. Nevertheless, the difficulties to directly observe C–C coupling pathways at a specific nanocavity hinder the advances in catalysts and electrolyzer design for efficient high-value hydrocarbon production. Here we develop a nano-confined Raman technology to elucidate the influence of the local electric field on the evolution of C–C coupling intermediates. Through precise adjustments to the Debye length in nanocavities of a copper catalyst, the overlapping of electrical double layers drives a transition in the C–C coupling pathway at a specific nanocavity from *CHO–*CO coupling to the direct dimerization of *CO species. Experimental evidence and simulations validate that a reduced potential drop across the compact layer promotes a higher yield of CO and promotes the direct dimerization of *CO species. Our findings provide insights for the development of highly selective catalyst materials tailored to promote specific products.
研究领域:
催化化学
·
电化学
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产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 12
·期 5
·3112-3120
·
IF 6.97
Li Li,Lei Wang,Chenglin Du,Zhongyuan Guan,Yinxiao Xiang,Wei Wu,Mengxin Ren,Xinzheng Zhang,Aiwei Tang,Wei Cai,Jingjun Xu
Strong coupling originating from excitons of quantum dots and plasmons in nanocavities can be realized at room temperature due to the large electromagnetic field enhancement of plasmons, offering building blocks for quantum information systems, ultralow-power switches and lasers. However, most of the current strong coupling effects were realized by the interaction between excitons and far-field light excited bright plasmon modes in the visible range. Beyond that, there is still a lack of direct imaging of polariton modes at the nanoscale. In this work, by using cathodoluminescence, ultrastrong coupling with Rabi splitting exceeding 1 eV between bonding breathing plasmons of aluminum (Al) metal–insulator–metal (MIM) cavities and excited states of CdZnS/ZnS quantum dots was observed in the near-ultraviolet (UV) spectrum. Further, the hybridization of the QDs excitons and bonding breathing plasmonic modes is verified by deep-subwavelength images of polaritonic modes in real-space. Analytic analysis based on the coupled oscillator model and full-wave electromagnetic simulations is consistent with our experimental results. Our work not only indicates the great potential of electron excited plasmon modes for strong coupling applications, but also extends the polaritonic frequency to the UV range with Al nanocavities.
研究领域:
光学
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材料科学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Yanyan Cheng,Shunfei Qiang,Jiaqi Li,Wenbo Wei,Yanmin Kuang,Wenkai Zhang,Xiaomin Fang,Tao Ding,Lijun Guo,Yujie Chen,Xudong Chen
Carbon dots (CDs) have great potentials in quantum emitters due to their simple synthesis, low cost, high stability, and tunable band gap; however, the low solid-state emission efficiency, as well as nanosecond-scale radiative lifetime, limits their applications requiring bright and fast emission. Here, a bright and ultrafast emission of red-emissive carbon dots (R-CDs) with narrow bandwidth (<30 nm) is achieved at room temperature by coupling with a plasmonic nanopatch antenna (NPA). The NPA manufacturing combines a conventional spin-coating process with a conformal transfer-print thin film technology, providing a widely applicable nanocavity for field enhancement with uniform quality in centimeter scale and accurate control of the position of emitters. The effective NPA–CD coupling generates an increase in the emission intensity of a factor of 76 and a shortened radiative lifetime of 80 ps, which demonstrates an 82-fold faster rate than the emission rate of uncoupled R-CDs. The NPA structure also shows striking enhancement of Raman spectra of carbon dots with an enhancement factor over 105. These results may benefit the low-cost and large-scale fabrication of plasmonic cavity and enable carbon dots to find applications in quantum optics, from low-threshold nanolaser to single-photon source.
研究领域:
光学
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材料科学
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量子光学
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DOI
高影响因子
Advanced Optical Materials
·
2022
·Vol. 10
·期 5
·2101762
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IF 10.05
Guangpeng Zhu,Xiuqi Shi,Guangyan Huang,Kaizhen Liu,Wei Wei,Qianqian Guo,Wei Du,Tao Wang
As contemporary star materials, 2D monolayer semiconductors have drawn huge research interests owing to their striking electrical and optical properties, rendering them ideal candidates as building blocks for novel optoelectronic devices. Towards light emitting devices with extended functions, it is necessary to manipulate the polarization of light emission from monolayer semiconductors. However, most of these monolayer semiconductors exhibit no or very limited polarization sensitivity inherited from their structural anisotropy, making it challenging to develop highly polarized light sources. Herein, by embedding monolayer tungsten diselenide (WSe 2 ) in a nanowire-on-film nanocavity, highly polarized light emission is demonstrated, featuring degree of polarization (DoP) of ≈99%. The highly anisotropic light emission originates from the near-field coupling between the WSe 2 monolayer with the polarization-dependent gap plasmons of the nanowire-on-film nanocavity. Moreover, as the width of the nanowire essentially defines the gap-plasmon resonance of the nanowire-on-film nanocavity, the anisotropy of the highly polarized light emission is systematically tuned by changing the nanowire width. The findings pave the way for engineering anisotropic optical properties of monolayer semiconductors and will boost the development of functional polarization-sensitive 2D optoelectronic devices.
研究领域:
光学
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材料科学
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纳米技术
✓ 已验证
DOI
高影响因子
Advanced Science
·
2024
·Vol. 11
·期 48
·2409838
·
IF 14.3
Abdur Rahim,Liqi Ma,Muhammad Saleem,Baiju Lyu,Muhammad Shafi,Yuxin You,Mingyue Li,Xiaoyu Zhang,Mei Liu
The field of semiconductor surface-enhanced Raman scattering (SERS) substrates has experienced significant advancements, leading to a wide range of applications in several fields. However, the quest for new ultra-sensitive semiconductor SERS materials is still of utmost importance. In this regard, an efficient and novel substrate, F 4 TCNQ/MoS 2 heterostructure is introduced, assisted by V-shaped aluminum anodic oxide (AAO) nanocavities with different depths. Utilizing the efficient charge transfer of organic/inorganic semiconducting heterostructure and the photoconfinement capability of the nanocavity structure of the AAO nanotemplate, excellent stability, fast sensing, enhanced Raman, and photodegradation activities are achieved. Due to its unique 3D structure, the optimized F 4 TCNQ/MoS 2 /AAO with 1500 nm depth achieves ultra-high sensitivity detection of 9.0×10 −16 M for conventional probe molecules. Furthermore, precise detection of water contaminants is observed for the first time with a V-shaped heterostructure due to combined organic/inorganic features that differ significantly from conventional MoS 2 structures or other metal/inorganic or inorganic/inorganic semiconductors. This research presents a novel and versatile strategy for SERS and demonstrates its diverse potential performance in practical applications.
研究领域:
材料科学
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光谱学
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemical Science
·
2025
·
IF 7.4
Xiaoxuan Zheng,Junjun Tan,Quanbing Pei,Yi Luo,Shuji Ye
Elucidating the ultrafast dynamics of interfacial molecules at the single-molecule level is pivotal for advancing our understanding of fundamental chemical and biological processes. Here, for the first time, we realized detection of ultrafast vibrational dynamics by a novel technique that integrates femtosecond sum frequency generation vibrational spectroscopy (SFG-VS) with nanoparticle-on-mirror (NPoM) nanocavities (NPoM-SFG-VS). Using a symmetric stretching vibrational mode of para-nitrothiophenol (νNO2) as a probe, we have successfully identified signals from self-assembled monolayers (SAMs) comprising ∼60 molecules, demonstrating the single-molecule-level sensitivity of the NPoM-SFG-VS. The dephasing time and vibrational relaxation time of νNO2 at the single-molecule level were determined to be 0.33 ± 0.01 ps and 2.2 ± 0.2 ps, respectively. By controlling the solution concentration used to prepare SAMs (C), a correlation between peak frequency of νNO2 and C is established. It was found that single-molecule-level detection was achieved at C ≤ 10−10 M. With this protocol, microregion distribution of interfacial molecule number can be mapped using NPoM-SFG imaging. This work provides insights into the structures and vibrational dynamics of individual interfacial molecules, aiding in precise engineering of surface properties and reactivity.
研究领域:
化学
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物理学
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表面科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Caimei He,Danling Zhang,Fengshang Chen,Yezheng Cai,Xiangsi Wu,Zhaoling Ma,Youguo Huang,Kui Liu,Qiang Wu,Hongqiang Wang,Qingyu Li
Designed synthesis of robust while earth-abundant carbon-based electrocatalysts for oxygen reduction reaction (ORR) is central for the wide spread application of renewable energy conversion technologies. Herein, graphitized and curved carbon nanochambers decorated with boron and nitrogen tailored highly-dispersed cobalt moieties (B,N-Co/GCCN) were developed via a feasible strategy combining room temperature crosslinking and in situ catalytic graphitization processes. The graphitized and curved carbon nanochambers enhanced the electron transfer and structural stability and tailored the electronic structure of metal active sites. Moreover, the in situ coupled amorphous carbon and cobalt-nitrogen/boron moieties represented catalytically active sites for catalyzing ORR. Notably, the selected B doping made the electron density of Co of B,N-Co/GCCN higher compared to N-Co/GCCN, promoting the adsorption and activation of oxygen molecule. Benefiting from this integrated structure, the B,N-Co/GHC exhibited high ORR activity comparable to commercial Pt/C catalyst, along with robust electrocatalytic stability with little change in half-wave potential after 5000 cycles. Impressively, a homemade zinc-air battery driven by B,N-Co/GHC showed higher discharging performance than the one driven by Pt/C, demonstrating promising application prospect.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
OPTICS EXPRESS
·
2023
·Vol. 31
·期 10
·16484-16494
·
IF 3.8
Sha HaiYang,Wang Zhengkun,Zhu Yong,Zhang Jie
To achieve high sensitivity and uniformity simultaneously in a surface-enhanced Raman scattering (SERS) substrate, this paper presents the preparation of a flexible and transparent three-dimensional (3D) ordered hemispherical array polydimethylsiloxane (PDMS) film. This is achieved by self-assembling a single-layer polystyrene (PS) microsphere array on a silicon substrate. The liquid-liquid interface method is then used to transfer Ag nanoparticles onto the PDMS film, which includes open nanocavity arrays created by etching the PS microsphere array. An open nanocavity assistant soft SERS sample, “Ag@PDMS,” is then prepared. For electromagnetic simulation of our sample, we utilized Comsol software. It has been experimentally confirmed that the Ag@PDMS substrate with silver particles of 50 nm in size is capable of achieving the largest localized electromagnetic hot spots in space. The optimal sample, Ag@PDMS, exhibits ultra-high sensitivity towards Rhodamine 6 G (R6G) probe molecules, with a limit of detection (LOD) of 10−15 mol/L, and an enhancement factor (EF) of ∼1012. Additionally, the substrate exhibits a highly uniform signal intensity for probe molecules, with a relative standard deviation (RSD) of approximately 6.86%. Moreover, it is capable of detecting multiple molecules and can perform real detection on non-flat surfaces.
研究领域:
材料科学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemical Science
·
2024
·
IF 7.6
Xiaoxuan Zheng,Quanbing Pei,Junjun Tan,Shiyu Bai,Yi Luo,Shuji Ye
Plasmonic nanocavities enable the generation of strong light–matter coupling and exhibit great potential in plasmon-mediated chemical reactions (PMCRs). Although an electric field generated by nanocavities (En) has recently been reported, its effect on the vibrational energy relaxation (VER) of the molecules in the nanocavities has not been explored. In this study, we reveal the impact of an electric field sensed by molecules (para-substituted thiophenol derivatives) in a nanocavity (Ef) on VER processes by employing advanced time-resolved femtosecond sum frequency generation vibrational spectroscopy (SFG-VS) supplemented by electrochemical measurements. The magnitude of En is almost identical (1.0 ± 0.2 V nm−1) beyond the experimental deviation while Ef varies from 0.3 V nm−1 to 1.7 V nm−1 depending on the substituent. An exponential correlation between Ef and the complete recovery time of the ground vibrational CC state (T2) of the phenyl ring is observed. Substances with a smaller T2 are strongly correlated with the reported macroscopic chemical reactivity. This finding may aid in enriching the current understanding of PMCRs and highlights the possibility of regulating vibrational energy flow into desired reaction coordinates by using a local electric field.
研究领域:
物理化学
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材料科学
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光化学
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产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Yaxin Wang,Zhen Xu,Shuangshuang Zhao,Yongjun Zhang,Wei Li,Jiahong Wen,Renxian Gao,Bohong Zheng,Lijun Liang,Xiaoyu Zhao
The Ag nanonail rooted in Au cross-channel nanocavity is fabricated by plasmon-mediated chemical reactions (PMCRs). The Au cross-channel nanocavity is prepared based on two-dimensional polystyrene (PS) nanosphere template through wet etching, and the shape of Au cross-channel nanocavity changes from trapezoidal to triangular, depending on the wet etching time. The growth of Ag nanostructures in Au channels by PMCRs indicates the morphology of Ag nanostructures has changed from Ag nanoparticles to nanonails, which is regulated by the shape of Au nanocavities and the exciting light polarization. The hotspots distributions results in the anisotropic growth of Ag nanostructures induced by PMCRs, which leading to the different Ag nanostructures depending on the shape of Au nanocavity and light polarization, as confirmed by FDTD simulations. In comparison with others reports, our nanocavity provide more parameters to control the shapes of Ag nanostructures, the nanocavity shape, the light polarization and the growth time. Our work provides a profound insight into the construction of periodic nanostructures and reconstruction of hotspots.
研究领域:
纳米技术
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光学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Changkun Song,Hongbiao Huo,Wei Shi,Jianyong Xu,Xiaoting Lei,Bonan Gu,Zhongbo Han,Wenchao Zhang
Surface-enhanced Raman spectroscopy (SERS) is strongly dependent on the metallic plasmonic nanostructures that can generate plasmon resonance coupling effects. Plasmonic nanostructures with sub-nanometer interparticle gaps or cavities have shown great potential in generating high local electromagnetic fields. Unfortunately, achieving precise control over the geometrical morphology of these nanostructures at the sub-nanometer scale presents significant challenges, particularly in applications where high consistency and homogeneity are required. Here, a reliable approach is proposed to construct plasmon-coupled Ag nanosphere-internalized nanocavity (SIC) arrays to enhance sensitivity and reproducibility in SERS sensing. This novel SIC nanostructure consists of a precise arrangement of Ag nanospheres located at the bottom of Au nanocavities, separated by a precisely controlled nano-Al 2 O 3 dielectric layer. The Al 2 O 3 dielectric layer plays a crucial role in inhibiting quantum tunneling effects at the nanogaps, thereby suppressing charge recombination and leading to strong plasmon resonance coupling. The SERS enhancement tends to significantly diminishes as the nanogap size increases from 4 to 10 nm, a spatially averaged SERS enhancement factor of 3.5 * 10 8 was obtained when the gap size is 4 nm, aligning well with the FDTD simulation results. As a representative application, an indirect detection strategy is utilized to selectively detect TNT with a high level of homogeneity and reproducibility, achieving a relative standard deviation of less than 7.8 %. Together with the capability to be fabricated on a flexible polyimide substrate, the SIC substrate shows significant potential for practical applications.
研究领域:
纳米技术
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分析化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yue Yu,Lian Wu,Shuxi Gao,Kangle Jia,Wei Zeng,Bing Liao,Hao Pang
Through inserting SiO 2 @Au into the reduced graphene oxide (rGO) layers, the rGO-SiO 2 @Au composites were prepared via the vacuum-assisted electrostatic self-assembly method. The obtained composites exhibit excellent electromagnetic interference (EMI) shielding effectiveness due to the successful construction of multi-nanocavities (spherical SiO 2 cavities and layered air cavities between rGO), multi-reflection interfaces (rGO and Au shell) and continuous conductive network (rGO-Au-rGO). Among them, the total shielding effectiveness (SET) of the composites with 75.78 wt% SiO 2 and 19.38 wt% rGO can reach 38.4 dB at 18 GHz. Thereinto, the shielding effectiveness absorption (SEA) is 36.4 dB, 1.3 and 13.5 times higher than that of rGO and SiO 2 @Au. And the shielding effectiveness reflection (SER) is always below 5 dB from 1 to 18 GHz, much lower than that of rGO (about 15 dB). Further studies found that the SEA values were enhanced at 12.6 GHz and 6.2 GHz due to the construction of cavities and location of Au nanoparticles between the rGO layers. This study provides a simple and mild method to prepare high-performance thin-layered materials with applications in the field of EMI absorption shielding.
研究领域:
材料科学
·
电子工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）