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1.
Fang Pu Li Wu Xiang Ran Prof. Jinsong Ren Prof. Xiaogang Qu 《Angewandte Chemie (International ed. in English)》2015,54(3):892-896
Artificial light‐harvesting systems have received great attention for use in photosynthetic and optoelectronic devices. Herein, a system involving G‐quartet‐based hierarchical nanofibers generated from the self‐assembly of guanosine 5′‐monophosphate (GMP) and a two‐step Förster resonance energy transfer (FRET) is presented that mimics natural light‐harvesting antenna. This solid‐state property offers advantages for future device fabrication. The generation of photocurrent under visible light shows it has potential for use as a nanoscale photoelectric device. The work will be beneficial for the development of light‐harvesting systems by the self‐assembly of supramolecular nanostructures. 相似文献
2.
Dr. Peng‐Zhong Chen Prof. Dr. Yu‐Xiang Weng Dr. Li‐Ya Niu Dr. Yu‐Zhe Chen Prof. Dr. Li‐Zhu Wu Prof. Dr. Chen‐Ho Tung Prof. Dr. Qing‐Zheng Yang 《Angewandte Chemie (International ed. in English)》2016,55(8):2759-2763
We report the first highly efficient artificial light‐harvesting systems based on nanocrystals of difluoroboron chromophores to mimic the chlorosomes, one of the most efficient light‐harvesting systems found in green photosynthetic bacteria. Uniform nanocrystals with controlled donor/acceptor ratios were prepared by simple coassembly of the donors and acceptors in water. The light‐harvesting system funneled the excitation energy collected by a thousand donor chromophores to a single acceptor. The well‐defined spatial organization of individual chromophores in the nanocrystals enabled an energy transfer efficiency of 95 %, even at a donor/acceptor ratio as high as 1000:1, and a significant fluorescence of the acceptor was observed up to donor/acceptor ratios of 200 000:1. 相似文献
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4.
Xu‐Man Chen Qin Cao Hari Krishna Bisoyi Meng Wang Hong Yang Quan Li 《Angewandte Chemie (International ed. in English)》2020,59(26):10493-10497
Light‐harvesting systems are an important way for capturing, transferring and utilizing light energy. It remains a key challenge to develop highly efficient artificial light‐harvesting systems. Herein, we report a supramolecular co‐assembly based on lower‐rim dodecyl‐modified sulfonatocalix[4]arene (SC4AD) and naphthyl‐1,8‐diphenyl pyridinium derivative (NPS) as a light‐harvesting platform. NPS as a donor shows significant aggregation induced emission enhancement (AIEE) after assembling with SC4AD. Upon introduction of Nile blue (NiB) as an acceptor into the NPS‐SC4AD co‐assembly, the light‐harvesting system becomes near‐infrared (NIR) emissive (675 nm). Importantly, the NIR emitting NPS‐SC4AD‐NiB system exhibits an ultrahigh antenna effect (33.1) at a high donor/acceptor ratio (250:1). By co‐staining PC‐3 cells with a Golgi staining reagent, NBD C6‐ceramide, NIR imaging in the Golgi apparatus has been demonstrated using these NIR emissive nanoparticles. 相似文献
5.
Photosynthetic systems utilize hundreds of chlorophylls to collect sunlight and transport the energy to the reaction center with remarkably high quantum efficiency, however, the large size of the system together with the complex interactions among the components make it extremely challenging to understand the dynamics of light harvesting in large photosynthetic systems. To shed light on this problem, we present a structure-based theoretical framework that can be used to calculate transition rate matrix describing energy transport in photosynthetic systems and network clustering methods that provide simplified coarse-grained model revealing key structures guiding the light harvesting process. We constructed an effective model for energy transport in a Photosystem II supercomplex and applied several network clustering methods to generate coarse-grained kinetic cluster models for the system. Furthermore, we evaluated the performances of the network clustering methods, and show that a spectral clustering method and a minimum cut approach produce accurate coarse-grained models for the PSII-sc system. The results indicate that finding bottlenecks of energy transport is a crucial factor for reduced representations of photosynthetic light harvesting, and the overall work presented in this paper should provide a comprehensive theoretical framework to elucidate the dynamics of light harvesting in photosynthetic systems. 相似文献
6.
We review recent theoretical calculations of quantum entanglement in photosynthetic light harvesting complexes. These works establish, for the first time, a manifestation of this characteristically quantum mechanical phenomenon in biologically functional structures. We begin by summarizing calculations on model biomolecular systems that aim to reveal non-trivial characteristics of quantum entanglement in non-equilibrium biological environments. We then discuss and compare several calculations performed recently of excitonic dynamics in the Fenna-Matthews-Olson light harvesting complex and of the electronic entanglement present in this widely studied pigment-protein structure. We point out the commonalities between the derived results and also identify and explain the differences. We also discuss recent work that examines entanglement in the structurally more intricate light harvesting complex II (LHCII). During this overview, we take the opportunity to clarify several subtle issues relating to entanglement in such biomolecular systems, including the role of entanglement in biological function, the complexity of dynamical modeling that is required to capture the salient features of entanglement in such biomolecular systems, and the relationship between entanglement and other quantum mechanical features that are observed and predicted in light harvesting complexes. Finally, we suggest possible extensions of the current work and also review the options for experimental confirmation of the predicted entanglement phenomena in light harvesting complexes. 相似文献
7.
Zeyuan Zhang Zhengqing Zhao Yali Hou Heng Wang Xiaopeng Li Gang He Mingming Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(26):8954-8958
Photosynthesis is a process wherein the chromophores in plants and bacteria absorb light and convert it into chemical energy. To mimic this process, an emissive poly(ethylene glycol)‐decorated tetragonal prismatic platinum(II) cage was prepared and used as the donor molecule to construct a light‐harvesting system in water. Eosin Y was chosen as the acceptor because of its good spectral overlap with that of the metallacage, which is essential for the preparation of light‐harvesting systems. Such a combination showed enhanced catalytic activity in catalyzing the cross‐coupling hydrogen evolution reaction, as compared with eosin Y alone. This study offers a pathway for using the output energy from the light‐harvesting system to mimic the whole photosynthetic process. 相似文献
8.
Synthesis and Confinement of Carbon Dots in Lysozyme Single Crystals Produces Ordered Hybrid Materials with Tuneable Luminescence
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Dr. Matt W. England Dr. Avinash J. Patil Prof. Stephen Mann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(25):9008-9013
The synthesis and confinement of graphitic nanoparticles (carbon dots) in the nanoscale solvent channels of cross‐linked lysozyme single crystals is used to prepare novel biohybrid luminescent materials. Co‐sequestration of acridine orange within the biohybrid crystals from acidic or neutral solutions yields FRET‐mediated phosphors emitting white or green light, respectively. The results offer a route to new types of tuneable multicolour luminescent materials based on microcrystalline host–guest energy‐transfer systems. 相似文献
9.
Ermilov EA Menting R Lau JT Leng X Röder B Ng DK 《Physical chemistry chemical physics : PCCP》2011,13(39):17633-17641
Porphyrins and phthalocyanines are two attractive classes of functional dyes for the construction of artificial light harvesting and charge separation molecular systems. The assembly of these components by supramolecular approach is of particular interest as this provides a facile route to build multi-chromophoric arrays with various architectures and tuneable photophysical properties. We report herein a series of host-guest complexes formed between a tetrasulfonated porphyrin and several silicon(IV) phthalocyanines substituted axially with two permethylated β-cyclodextrin units via different spacers. As shown by electronic absorption and fluorescence spectroscopic methods, the two components bind spontaneously in a 1:1 manner in water with large binding constants in the range of 1.1 × 10(7) to 3.5 × 10(8) M(-1). The photophysical properties of the resulting supramolecular complexes have also been studied in detail using steady-state and time-resolved optical spectroscopic methods. It has been found that two major photoinduced processes, namely fluorescence resonance energy transfer and charge transfer are involved which are controlled by the spacer between the β-cyclodextrin units and the silicon centre of phthalocyanine. Despite the fact that charge transfer is a thermodynamically favourable process for all the complexes, only the ones with a tetraethylene glycol or oxo linker exhibit an efficient charge transfer from the excited phthalocyanine to the porphyrin entity. The lifetimes of the corresponding charge-separated states have been determined to be 200 and 70 ps by picosecond pump-probe experiments. 相似文献
10.
Light Harvesting and White‐Light Generation in a Composite of Carbon Dots and Dye‐Encapsulated BSA‐Protein‐Capped Gold Nanoclusters
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Monoj Kumar Barman Bipattaran Paramanik Dipankar Bain Prof. Amitava Patra 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(33):11699-11705
Several strategies have been adopted to design an artificial light‐harvesting system in which light energy is captured by peripheral chromophores and it is subsequently transferred to the core via energy transfer. A composite of carbon dots and dye‐encapsulated BSA‐protein‐capped gold nanoclusters (AuNCs) has been developed for efficient light harvesting and white light generation. Carbon dots (C‐dots) act as donor and AuNCs capped with BSA protein act as acceptor. Analysis reveals that energy transfer increases from 63 % to 83 % in presence of coumarin dye (C153), which enhances the cascade energy transfer from carbon dots to AuNCs. Bright white light emission with a quantum yield of 19 % under the 375 nm excitation wavelength is achieved by changing the ratio of components. Interesting findings reveal that the efficient energy transfer in carbon‐dot–metal‐cluster nanocomposites may open up new possibilities in designing artificial light harvesting systems for future applications. 相似文献
11.
Highly Efficient Artificial Light‐Harvesting Systems Constructed in Aqueous Solution Based on Supramolecular Self‐Assembly
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Shuwen Guo Yongshang Song Yuling He Dr. Xiao‐Yu Hu Prof. Dr. Leyong Wang 《Angewandte Chemie (International ed. in English)》2018,57(12):3163-3167
Highly efficient light‐harvesting systems were successfully fabricated in aqueous solution based on the supramolecular self‐assembly of a water‐soluble pillar[6]arene (WP6), a salicylaldehyde azine derivative (G), and two different fluorescence dyes, Nile Red (NiR) or Eosin Y (ESY). The WP6‐G supramolecular assembly exhibits remarkably improved aggregation‐induced emission enhancement and acts as a donor for the artificial light‐harvesting system, and NiR or ESY, which are loaded within the WP6‐G assembly, act as acceptors. An efficient energy‐transfer process takes place from the WP6‐G assembly not only to NiR but also to ESY for these two different systems. Furthermore, both of the WP6‐G‐NiR and WP6‐G‐ESY systems show an ultrahigh antenna effect at a high donor/acceptor ratio. 相似文献
12.
Multichromophoric Organic Molecules Encapsulated in Polymer Nanoparticles for Artificial Light Harvesting
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We designed a self‐assembled multichromophoric organic molecular arrangement inside polymer nanoparticles for light‐harvesting antenna materials. The self‐assembled molecular arrangement of quaterthiophene molecules was found to be an efficient light‐absorbing antenna material, followed by energy transfer to Nile red (NR) dye molecules, which was confined in polymer nanoparticles. The efficiency of the antenna effect was found to be 3.2 and the effective molar extinction coefficient of acceptor dye molecules was found to be enhanced, which indicates an efficient light‐harvesting system. Based on this energy‐transfer process, tunable photo emission and white light emission has been generated with 14 % quantum yield. Such self‐assembled oligothiophene–NR systems encapsulated in polymer nanoparticles may open up new possibilities for fabrication of artificial light harvesting system. 相似文献
13.
Jiratheep Pruchyathamkorn William J. Kendrick Andrew T. Frawley Andrea Mattioni Felipe Caycedo‐Soler Susana F. Huelga Martin B. Plenio Harry L. Anderson 《Angewandte Chemie (International ed. in English)》2020,59(38):16455-16458
A nanoring‐rotaxane supramolecular assembly with a Cy7 cyanine dye (hexamethylindotricarbocyanine) threaded along the axis of the nanoring was synthesized as a model for the energy transfer between the light‐harvesting complex LH1 and the reaction center in purple bacteria photosynthesis. The complex displays efficient energy transfer from the central cyanine dye to the surrounding zinc porphyrin nanoring. We present a theoretical model that reproduces the absorption spectrum of the nanoring and quantifies the excitonic coupling between the nanoring and the central dye, thereby explaining the efficient energy transfer and demonstrating similarity with structurally related natural light‐harvesting systems. 相似文献
14.
Jeroen A. Rombouts Janneke Ravensbergen Dr. Raoul N. Frese Dr. John T. M. Kennis Dr. Andreas W. Ehlers Dr. J. Chris Slootweg Dr. Eelco Ruijter Prof. Dr. Koop Lammertsma Prof. Dr. Romano V. A. Orru 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(33):10285-10291
In search of supramolecular antenna systems for light‐harvesting applications, we report on a short and effective synthesis of a fused NDI–zinc–salphen‐based chromophore (salphen = bis‐salicylimide phenylene) and its photophysical properties. A supramolecular recognition motif is embedded into the chromophoric π‐system of this compound. The fused π‐chromophore behaves as one pigment, absorbs light between 600 and 750 nm and displays a modest Stokes shift. Upon binding pyridines, the compound ( DATZnS ) does not change its redox potentials, does not undergo any internal excited state quenching and does not appreciably alter its excited state lifetime. These notable properties define DATZnS as an alternative to porphyrin‐based components used in supramolecular light‐harvesting architectures. 相似文献
15.
Synthesis and Functional Reconstitution of Light‐Harvesting Complex II into Polymeric Membrane Architectures
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Thomas Zapf Dr. Cherng‐Wen Darren Tan Tobias Reinelt Dr. Christoph Huber Dr. Ding Shaohua Prof. Dr. Susana Geifman‐Shochat Prof. Dr. Harald Paulsen Prof. Dr. Eva‐Kathrin Sinner 《Angewandte Chemie (International ed. in English)》2015,54(49):14664-14668
One of most important processes in nature is the harvesting and dissipation of solar energy with the help of light‐harvesting complex II (LHCII). This protein, along with its associated pigments, is the main solar‐energy collector in higher plants. We aimed to generate stable, highly controllable, and sustainable polymer‐based membrane systems containing LHCII–pigment complexes ready for light harvesting. LHCII was produced by cell‐free protein synthesis based on wheat‐germ extract, and the successful integration of LHCII and its pigments into different membrane architectures was monitored. The unidirectionality of LHCII insertion was investigated by protease digestion assays. Fluorescence measurements indicated chlorophyll integration in the presence of LHCII in spherical as well as planar bilayer architectures. Surface plasmon enhanced fluorescence spectroscopy (SPFS) was used to reveal energy transfer from chlorophyll b to chlorophyll a, which indicates native folding of the LHCII proteins. 相似文献
16.
Popere BC Della Pelle AM Poe A Thayumanavan S 《Physical chemistry chemical physics : PCCP》2012,14(12):4043-4057
Research in the field of organic photovoltaics has gained considerable momentum in the last two decades owing to the need for developing low-cost and efficient energy harvesting systems. Elegant molecular architectures have been designed, synthesized and employed as active materials for photovoltaic devices thereby leading to a better molecular structure-device property relationship understanding. In this perspective, we outline new macromolecular scaffolds that have been designed within the purview of each of the three fundamental processes involving light harvesting, charge separation and charge transport. 相似文献
17.
Chuanqi Li Jing Zhang Shiyong Zhang Yan Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(6):1657-1661
Light harvesting is a key step in photosynthesis but creation of synthetic light‐harvesting systems (LHSs) with high efficiencies has been challenging. When donor and acceptor dyes with aggregation‐induced emission were trapped within the interior of cross‐linked reverse vesicles, LHSs were obtained readily through spontaneous hydrophobically driven aggregation of the dyes in water. Aggregation in the confined nanospace was critical to the energy transfer and the light‐harvesting efficiency. The efficiency of the excitation energy transfer (EET) reached 95 % at a donor/acceptor ratio of 100:1 and the energy transfer was clearly visible even at a donor/acceptor ratio of 10 000:1. Multicolor emission was achieved simply by tuning the donor/acceptor feed ratio in the preparation and the quantum yield of white light emission from the system was 0.38, the highest reported for organic materials in water to date. 相似文献
18.
Dr. Laura Delafresnaye Fabian R. Bloesser Dr. Katrin B. Kockler Christian W. Schmitt Ishrath M. Irshadeen Prof. Christopher Barner-Kowollik 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(1):114-127
Chemiluminescence (CL) reactions have been widely employed and explored over the past 50 years because they offer unique light emission upon a defined chemical stimulus. In this Minireview, we focus on peroxyoxalate (PO) compounds because they feature very high quantum yields tuneable over the entire visible spectrum, allowing for visible-light detection by the naked eye without the necessity for expensive analytical instruments. Although analytical methods have been extensively described, PO-CL read-out is a strongly emerging field with ample industrial potential. The state-of-the-art PO-CL detection read-out systems for various key analytes is here explored. In particular, structural requirements, recent developments of PO-CL read-out probes and current limitations of selected examples are detailed. Furthermore, innovative approaches and synthetic routes to push the boundaries of PO-CL reactions into biological systems are highlighted. Underpinned by recent contributions, we share perspectives on embedding PO-CL molecules into polymeric materials, which they consider the next step in designing high performance solid-phase read-out systems. 相似文献
19.
Michelle A. Harris Tuba Sahin Jianbing Jiang Pothiappan Vairaprakash Pamela S. Parkes‐Loach Dariusz M. Niedzwiedzki Christine Kirmaier Paul A. Loach David F. Bocian Dewey Holten Jonathan S. Lindsey 《Photochemistry and photobiology》2014,90(6):1264-1276
Biohybrid light‐harvesting antennas are an emerging platform technology with versatile tailorability for solar‐energy conversion. These systems combine the proven peptide scaffold unit utilized for light harvesting by purple photosynthetic bacteria with attached synthetic chromophores to extend solar coverage beyond that of the natural systems. Herein, synthetic unattached chromophores are employed that partition into the organized milieu (e.g. detergent micelles) that house the LH1‐like biohybrid architectures. The synthetic chromophores include a hydrophobic boron‐dipyrrin dye (A1) and an amphiphilic bacteriochlorin (A2), which transfer energy with reasonable efficiency to the bacteriochlorophyll acceptor array (B875) of the LH1‐like cyclic oligomers. The energy‐transfer efficiencies are markedly increased upon covalent attachment of a bacteriochlorin (B1 or B2) to the peptide scaffold, where the latter likely acts as an energy‐transfer relay site for the (potentially diffusing) free chromophores. The efficiencies are consistent with a Förster (through‐space) mechanism for energy transfer. The overall energy‐transfer efficiency from the free chromophores via the relay to the target site can approach those obtained previously by relay‐assisted energy transfer from chromophores attached at distant sites on the peptides. Thus, the use of free accessory chromophores affords a simple design to enhance the overall light‐harvesting capacity of biohybrid LH1‐like architectures. 相似文献
20.
Exploiting Co‐solubilization of Warfarin,Curcumin, and Rhodamine B for Modulation of Energy Transfer: A Micelle FRET On/Off Switch
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Dr. Parvaiz Ahmad Bhat Dr. Oyais Ahmad Chat Prof. Aijaz Ahmad Dar 《Chemphyschem》2016,17(15):2360-2372
Two new FRET pairs, warfarin (WF)–curcumin (CUR) and curcumin–rhodamine B (RhB), are explored by using surfactant‐based self‐assembled soft systems as scaffolds. The study is extended to design a two‐step concurrent FRET system based on these three fluorophores, which is an important mechanism to devise artificial light‐harvesting/antenna systems. Surfactant systems of varying nature (cationic, anionic, nonionic, and zwitterionic) are exploited to modulate the energy transfer in different FRET systems. Interestingly, micelle/water interfacial‐charge‐responsive FRET is observed owing to selective solubilization of the fluorophores during co‐solubilization. The step‐one FRET (WF→CUR) is switched on in cationic and zwitterionic media but switched off in anionic/nonionic media, whereas the step‐two FRET from CUR to RhB is switched on in anionic/nonionic and zwitterionic media. However, both the FRET steps (WF→CUR→RhB) are observed to be active only in zwitterionic medium. Co‐solubilized, appropriately mixed fluorophores having multistep FRET possibilities can be switched on/off selectively as and when required and energy efficiency can be tuned to an optimal level by varying the nature and geometry of the micellar scaffold. Thus, the two FRET pairs selectively acknowledge all types of media for their anticipated applications in biological systems, as structural tools, and for the development of artificial light‐harvesting/antenna systems and lasers. 相似文献