共查询到18条相似文献,搜索用时 15 毫秒
1.
Rossella Yivlialin Claudia Filoni Francesco Goto Alberto Calloni Lamberto Du Franco Ciccacci Gianlorenzo Bussetti 《Molecules (Basel, Switzerland)》2022,27(22)
Reflectance anisotropy spectroscopy (RAS) coupled to an electrochemical cell represents a powerful tool to correlate changes in the surface optical anisotropy to changes in the electrochemical currents related to electrochemical reactions. The high sensitivity of RAS in the range of the absorption bands of organic systems, such as porphyrins, allows us to directly correlate the variations of the optical anisotropy signal to modifications in the solid-state aggregation of the porphyrin molecules. By combining in situ RAS to electrochemical techniques, we studied the case of vacuum-deposited porphyrin nanocrystals, which have been recently observed dissolving through electrochemical oxidation in diluted sulfuric acid. Specifically, we could identify the first stages of the morphological modifications of the nanocrystals, which we could attribute to the single-electron transfers involved in the oxidation reaction; in this sense, the simultaneous variation of the optical anisotropy with the electron transfer acts as a precursor of the dissolution process of porphyrin nanocrystals. 相似文献
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Thermal degradation of cellulose nanocrystals deposited on flat solid surfaces was monitored by AFM coupled with analysis of obtained images using image processor. The nanocrystals deposited on TiO2 substrate showed different degradation patterns compared to those deposited on the nanosized layer of amorphous cellulose. The degradation was complete within 20 minutes at 300 °C. The nanocrystal deposited on amorphous cellulose resisted the heat treatment up to 120 minutes. Visual comparison and analysis of the AFM images clearly demonstrated the impact of temperature on the degradation rate of the nanocrystals deposited on TiO2 substrate. 相似文献
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Carlos Gibaja David Rodriguez‐San‐Miguel Pablo Ares Prof. Julio Gómez‐Herrero Dr. Maria Varela Dr. Roland Gillen Prof. Janina Maultzsch Dr. Frank Hauke Prof. Andreas Hirsch Dr. Gonzalo Abellán Dr. Félix Zamora 《Angewandte Chemie (International ed. in English)》2016,55(46):14345-14349
We report on a fast and simple method to produce highly stable isopropanol/water (4:1) suspensions of few‐layer antimonene by liquid‐phase exfoliation of antimony crystals in a process that is assisted by sonication but does not require the addition of any surfactant. This straightforward method generates dispersions of few‐layer antimonene suitable for on‐surface isolation. Analysis by atomic force microscopy, scanning transmission electron microscopy, and electron energy loss spectroscopy confirmed the formation of high‐quality few‐layer antimonene nanosheets with large lateral dimensions. These nanolayers are extremely stable under ambient conditions. Their Raman signals are strongly thickness‐dependent, which was rationalized by means of density functional theory calculations. 相似文献
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Back Cover: Few‐Layer Antimonene by Liquid‐Phase Exfoliation (Angew. Chem. Int. Ed. 46/2016) 下载免费PDF全文
Carlos Gibaja David Rodriguez‐San‐Miguel Pablo Ares Prof. Julio Gómez‐Herrero Dr. Maria Varela Dr. Roland Gillen Prof. Janina Maultzsch Dr. Frank Hauke Prof. Andreas Hirsch Dr. Gonzalo Abellán Dr. Félix Zamora 《Angewandte Chemie (International ed. in English)》2016,55(46):14470-14470
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Dr. Mari Annadhasan Dr. Durga Prasad Karothu Ragaverthini Chinnasamy Dr. Luca Catalano Dr. Ejaz Ahmed Dr. Soumyajit Ghosh Prof. Panče Naumov Prof. Rajadurai Chandrasekar 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(33):13925-13934
Flexible organic single crystals are evolving as new materials for optical waveguides that can be used for transfer of information in organic optoelectronic microcircuits. Integration in microelectronics of such crystalline waveguides requires downsizing and precise spatial control over their shape and size at the microscale, however that currently is not possible due to difficulties with manipulation of these small, brittle objects that are prone to cracking and disintegration. Here we demonstrate that atomic force microscopy (AFM) can be used to reshape, resize and relocate single-crystal microwaveguides in order to attain spatial control over their light output. Using an AFM cantilever tip, mechanically compliant acicular microcrystals of three N-benzylideneanilines were bent to an arbitrary angle, sliced out from a bundle into individual crystals, cut into shorter crystals of arbitrary length, and moved across and above a solid surface. When excited by using laser light, such bent microcrystals act as active optical microwaveguides that transduce their fluorescence, with the total intensity of transduced light being dependent on the optical path length. This micromanipulation of the crystal waveguides using AFM is non-invasive, and after bending their emissive spectral output remains unaltered. The approach reported here effectively overcomes the difficulties that are commonly encountered with reshaping and positioning of small delicate objects (the “thick fingers” problem), and can be applied to mechanically reconfigure organic optical waveguides in order to attain spatial control over their output in two and three dimensions in optical microcircuits. 相似文献
7.
Mari Annadhasan Durga Prasad Karothu Ragaverthini Chinnasamy Luca Catalano Ejaz Ahmed Soumyajit Ghosh Pan
e Naumov Rajadurai Chandrasekar 《Angewandte Chemie (International ed. in English)》2020,59(33):13821-13830
Flexible organic single crystals are evolving as new materials for optical waveguides that can be used for transfer of information in organic optoelectronic microcircuits. Integration in microelectronics of such crystalline waveguides requires downsizing and precise spatial control over their shape and size at the microscale, however that currently is not possible due to difficulties with manipulation of these small, brittle objects that are prone to cracking and disintegration. Here we demonstrate that atomic force microscopy (AFM) can be used to reshape, resize and relocate single‐crystal microwaveguides in order to attain spatial control over their light output. Using an AFM cantilever tip, mechanically compliant acicular microcrystals of three N‐benzylideneanilines were bent to an arbitrary angle, sliced out from a bundle into individual crystals, cut into shorter crystals of arbitrary length, and moved across and above a solid surface. When excited by using laser light, such bent microcrystals act as active optical microwaveguides that transduce their fluorescence, with the total intensity of transduced light being dependent on the optical path length. This micromanipulation of the crystal waveguides using AFM is non‐invasive, and after bending their emissive spectral output remains unaltered. The approach reported here effectively overcomes the difficulties that are commonly encountered with reshaping and positioning of small delicate objects (the “thick fingers” problem), and can be applied to mechanically reconfigure organic optical waveguides in order to attain spatial control over their output in two and three dimensions in optical microcircuits. 相似文献
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Dr. Pablo Cubillas Prof. Michael W. Anderson Dr. Martin P. Attfield 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(48):15406-15415
Crystal growth of the metal–organic framework MOF‐5 was studied by atomic force microscopy (AFM) for the first time. Growth under low supersaturation conditions was found to occur by a two‐dimensional or spiral crystal growth mechanism. Observation of developing nuclei during the former reveals growth occurs through a process of nucleation and spreading of metastable and stable sub‐layers revealing that MOFs may be considered as dense phase structures in terms of crystal growth, even though they contain sub‐layers consisting of ordered framework and disordered non‐framework components. These results also support the notion this may be a general mechanism of surface crystal growth at low supersaturation applicable to crystalline nanoporous materials. The crystal growth mechanism at the atomistic level was also seen to vary as a function of the growth solution Zn/H2bdc ratio producing square terraces with steps parallel to the <100> direction or rhombus‐shaped terraces with steps parallel to the <110> direction when the Zn/H2bdc ratio was >1 or about 1, respectively. The change in relative growth rates can be explained in terms of changes in the solution species concentrations and their influence on growth at different terrace growth sites. These results were successfully applied to the growth of as‐synthesized cube‐shaped crystals to increase expression of the {111} faces and to grow octahedral crystals of suitable quality to image using AFM. This modulator‐free route to control the crystal morphology of MOF‐5 crystals should be applicable to a wide variety of MOFs to achieve the desired morphological control for performance enhancement in applications. 相似文献
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Determination of the Preassembled Nucleating Units That Are Critical for the Crystal Growth of the Metal–Organic Framework CdIF‐4 下载免费PDF全文
Raghidah Wagia Dr. Ilya Strashnov Prof. Michael W. Anderson Dr. Martin P. Attfield 《Angewandte Chemie (International ed. in English)》2016,55(31):9075-9079
Identifying the form and role of the chemical species that traverse the stages of crystallization is critical to understanding the formation process of coordination polymers. Herein, we report the combined use of in situ atomic force microscopy and mass spectrometry to identify preformed, complex, cadmium 2‐ethylimidazole containing solution species in the growth solution of the cadmium 2‐ethylimidazolate metal–organic framework CdIF‐4, and show that they are critical in the surface nucleation for the crystal growth of this material. Surface nucleation appears to be instigated by these [Cdx(CH3CO2)y(C5H7N2/C5H8N2)z]‐containing solution species and not by sole addition of the ligand molecules. The CH3CO2? or Cd(CH3CO2)2 groups of the former are substituted subsequently as the framework growth proceeds. Our greater understanding of such solution species and their role in crystallization will guide future syntheses of designed functional coordination polymers. 相似文献
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Shan Zou Mark A. Hempenius Holger Schnherr G. Julius Vancso 《Macromolecular rapid communications》2006,27(2):103-108
Summary: Progress in the development of a redox‐driven macromolecular motor and the characterization of its redox‐mechanical cycle using electrochemical AFM‐based single‐molecule force spectroscopy (SMFS) is described. The elasticities of individual neutral and oxidized poly(ferrocenyldimethylsilane) (PFS) macromolecules were reversibly controlled in situ by adjusting the potential in electrochemical SMFS experiments. For the operating cycle of one individual PFS‐based molecular motor, an output of 3.4 × 10−19 J and an efficiency of 5% have been estimated.
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Assessing Chemical Heterogeneity at the Nanoscale in Mixed‐Ligand Metal–Organic Frameworks with the PTIR Technique 下载免费PDF全文
Dr. Aaron M. Katzenmeyer Dr. Jerome Canivet Glenn Holland Dr. David Farrusseng Dr. Andrea Centrone 《Angewandte Chemie (International ed. in English)》2014,53(11):2852-2856
Recently, the use of mixtures of organic‐building‐block linkers has given chemists an additional degree of freedom for engineering metal–organic frameworks (MOFs) with specific properties; however, the poor characterization of the chemical complexity of such MixMOF structures by conventional techniques hinders the verification of rational design. Herein, we describe the application of a technique known as photothermal induced resonance to individual MixMOF microcrystals to elucidate their chemical composition with nanoscale resolution. Results show that MixMOFs isoreticular to In‐MIL‐68, obtained either directly from solution or by postsynthetic linker exchange, are homogeneous down to approximately 100 nm. Additionally, we report a novel in situ process that enables the engineering of anisotropic domains in MOF crystals with submicron linker‐concentration gradients. 相似文献
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基于原子力显微镜技术(AFM)的单分子力谱是研究分子间分子内相互作用的有效手段.为了简化样品体系及数据的解析,真实的生物或材料体系通常被简化,其中的目标分子被提取并桥连于AFM的针尖与固体基片之间进行研究,这是认识真实体系的有效途径.随着技术的不断进步(包括样品固定方法的改进),使得直接研究真实生物及材料体系中的各种弱相互作用成为可能,此种条件下获得的信息对相关生命过程的调控及高性能材料的设计更具指导意义.本文概述了近几年基于AFM力谱技术在活体细胞以及高分子材料领域的研究进展,分析了存在的主要问题,并对相关领域的未来进行了展望. 相似文献
13.
Russell E. Morris Prof. 《Chemphyschem》2009,10(2):327-329
Metal–organic frameworks (MOFs) are one of the most important classes of material in current chemistry. One open question is what is the mechanism of their crystal growth? In situ atomic force microscopy (see image) can be used to look at the surface of crystals as they grow, revealing a number of interesting features and giving clues to the molecular species that are important in the growth mechanism.
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Alenka Vesel Metod Kolar Ales Doliska Karin Stana‐Kleinschek Miran Mozetic 《Surface and interface analysis : SIA》2012,44(13):1565-1571
Films of polyethylene terephthalate were deposited on quartz crystals and exposed to oxygen atoms to study their etching characteristics and quantify the etching rate. Oxygen (O) atoms were created by passing molecular oxygen through plasma created in a microwave discharge. The discharge power was fixed at 250 W, while the pressure of oxygen was 50 Pa. Before exposure to oxygen atoms, a thin polymer film of polyethylene terephthalate (PET) was deposited uniformly over a crystal with a diameter of 12 mm. The crystal was mounted on a quartz crystal microbalance to accurately determine the thickness of the polymer film. The polymer film was exposed to O atoms in the flowing afterglow. The density of O atoms was measured with a cobalt catalytic probe mounted next to the sample and was determined to be 1.2 × 1021 m–3. Samples were treated with O atoms for different periods of up to 120 min. The thickness of the film decreased linearly with treatment time. After 90 min of treatment, a 65‐nm‐thick polymer film was completely removed. Therefore, the etching rate was 0.5 nm/min, so the interaction probability between an O atom and an atom in the sample was extremely low, just 1.4 × 10–6. Samples treated for different periods were investigated by atomic force microscopy and X‐ray photoelectron spectroscopy to examine the etching characteristics of O atoms in the flowing afterglow. Copyright © 2012 John Wiley & Sons, Ltd. 相似文献
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Dr. Pablo Cubillas Prof. Michael W. Anderson Dr. Martin P. Attfield 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(25):8236-8243
A new zeolitic–imidazolate framework (ZIF), [Zn(imidazolate)2?x(benzimidazolate)x], that has the zeolite A (LTA) framework topology and contains relatively inexpensive organic linkers has been revealed using in situ atomic force microscopy. The new material was grown on the structure‐directing surface of [Zn(imidazolate)1.5(5‐chlorobenzimidazolate)0.5] (ZIF‐76) crystals, a metal–organic framework (MOF) that also possesses the LTA framework topology. The crystal growth processes for both [Zn(imidazolate)2?x(benzimidazolate)x] and ZIF‐76 were observed using in situ atomic force microscopy; it is the first time the growth process of a nanoporous material with the complex zeolite A (LTA) framework topology has been monitored temporally at the nanoscale. The results reveal the crystal growth mechanisms and possible surface terminations on the {100} and {111} facets of the materials under low supersaturation conditions. Surface growth of these structurally complex materials was found to proceed through both “birth‐and‐spread” and spiral crystal‐growth mechanisms, with the former occurring through the nucleation and spreading of metastable and stable sub‐layers reliant on the presence of non‐framework species to bridge the framework during formation. These results support the notion that the latter process may be a general mechanism of surface crystal growth applicable to numerous crystalline nanoporous materials of differing complexity and demonstrate that the methodology of seeded crystal growth can be used to discover previously unobtainable ZIFs and MOFs with desirable framework compositions. 相似文献
17.
Eralci Moreira Therézio Erick Piovesan Maria Letícia Vega Raigna A. Silva Osvaldo N. Oliveira Jr. Alexandre Marletta 《Journal of Polymer Science.Polymer Physics》2011,49(3):206-213
The fabrication of controlled molecular architectures is essential for organic devices, as is the case of emission of polarized light for the information industry. In this study, we show that optimized conditions can be established to allow layer‐by‐layer (LbL) films of poly(p‐phenylene vinylene) (PPV)+dodecylbenzenesulfonate (DBS) to be obtained with anisotropic properties. Films with five layers and converted at 110 °C had a dichroic ratio δ = 2.3 and order parameter r = 34%, as indicated in optical spectroscopy and emission ellipsometry data. This anisotropy was decreased with the number of layers deposited, with δ = 1.0 for a 75‐layer LbL PPV + DBS film. The analysis with atomic force microscopy showed the formation of polymer clusters in a random growth process with the normalized height distribution being represented by a Gaussian function. In spite of this randomness in film growth, the self‐covariance function pointed to a correlation between clusters, especially for thick films. In summary, the LbL method may be exploited to obtain both anisotropic films with polarized emission and regular, nanostructured surfaces. © 2010 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2011 相似文献
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《Arabian Journal of Chemistry》2020,13(12):8848-8887
Phthalocyanine (Pc) complexes are an important class of dyes with numerous (e.g., biological, photophysical, and analytical) applications. Among the methods used to improve the properties of these complexes, one should mention the introduction of different substituents, variation of the central metal ion, ligand exchange, and conjugation to nanomaterials (e.g., carbon-based nanomaterials and metal nanoparticles (NPs)). This work briefly reviews Pc complex conjugation to Ag and Au NPs, highlights the different NP shapes, and discusses the diversity of conjugation approaches. Moreover, the use of UV–Vis spectroscopy, powder X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, atomic force microscopy, dynamic light scattering and Fourier transform infrared spectroscopy to characterize Pc-NP hybrids is summarized. The effect of conjugation on Pc photo-physicochemical properties (fluorescence, singlet oxygen generation, triplet state formation, and optical limiting behavior) is discussed, and future perspectives for the synthesis and applications of new hybrids are provided. 相似文献