Light‐Harvesting Systems Based on Organic Nanocrystals To Mimic Chlorosomes

Chen, Peng‐Zhong; Weng, Yuxiang; Niu, Li‐Ya; Chen, Yuzhe; Wu, Li‐Zhu; Tung, Chen‐Ho; Yang, Qing‐Zheng

doi:10.1002/anie.201510503

Cited by 157 publications

(92 citation statements)

References 63 publications

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“…Ed. 55, 2759(2016] on organic nanocrystals self-assembled from difluoroboron chromophores, the spontaneous emission of an excited pigment should undergo a two-step process. It would first decay to an excitonic polariton confined by cavity resonance via strong photon-exciton coupling.The captive intermediate could then funnel the energy directly to doped acceptors, leading to the observed over 90% transfer efficiency at less than 1/1000 acceptor-donor ratio.…”

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“…Away from the living cells, efforts have been devoted to construct artificial light-harvesting systems that can emulate the success of their natural counterparts. Recently, one such success based on nanocrystals of difluoroboron chromophores was reported by Chen et al [2], with the transfer efficiency reaching 95%. We suggest in this letter that the high efficiency is a consequence of quantum confinement of excitonic polaritons via coherent exciton-photon coupling.…”

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“…The latter in turn emit in red light, making the energy transfer vivid to the naked eye by color changes . The nanocrystals of BF 2 bcz were reported to have smooth surfaces and uniform sizes of 400 -600 nm in thickness and 5 -7 µm in length [2,3].…”

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Resonant Confinement of an Excitonic Polariton and Ultraefficient Light Harvest in Artificial Photosynthesis

et al. 2019

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We show that in the recent artificial light-harvesting experiment [Angewandte Chemie Intl. Ed. 55, 2759(2016] on organic nanocrystals self-assembled from difluoroboron chromophores, the spontaneous emission of an excited pigment should undergo a two-step process. It would first decay to an excitonic polariton confined by cavity resonance via strong photon-exciton coupling.The captive intermediate could then funnel the energy directly to doped acceptors, leading to the observed over 90% transfer efficiency at less than 1/1000 acceptor-donor ratio. Theoretical, parameter-free analyses are in quantitative agreement with the experiment. Abstract This supplementary information covers additional algebra needed for the main article published in [1]. It consists of the following parts: A. The standing-wave solutions of Maxwell equations in a rectangle cavity of homogeneous dielectric medium. B. Diagonalization of the photon-exciton coupling Hamiltonian in the rectangle cavity. C. Escape rate of the intermediate polariton out of confinement. D. Transition rate from a trapped exciton-polariton to doped acceptors.

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Resonant Confinement of an Excitonic Polariton and Ultraefficient Light Harvest in Artificial Photosynthesis

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“…With an understanding of the Pep-cd assembly mechanism and the conditions needed to grow 1D cylindrical micelles,2D membranes and 3D intertwined ribbons,w ea ttempted to demonstrate ap otential application of these hierarchical structures,t aking ac ue from bacterial light harvesting complexes.I nt hose systems,c hromophores are positioned around ar oughly circular disk-shaped protein complex with as pacing that biases adsorbed photon energy to be transferred to nearby centers via FRET rather than be lost by radiative re-emission. [14] Thea dsorbed photon energy is eventually resonantly transferred to an active site at the center of the complex where it is converted into chemically stored energy.W hile many studies have been aimed at mimicking this natural light-harvesting process by achieving efficient and rapid energy transfer from donors to acceptors, [15] doing so in aqueous solution rather than in an organic environment has remained am ajor challenge. [16] Thea bility of Pep-cd cylindrical micelles to assemble and be stable in aqueous environments suggests they may offer ap latform from which to address this challenge due to several structural characteristics.F irst, they possess ahydrophobic core,w hich can serve as the "host" to accommodate hydrophobic "guest" molecules.T hus,hydrophobic donor molecules can be encapsulated inside the core and remain separated from one another to avoid p-p interactions.Second, the empty CD groups on the surface of Pep-cd cylindrical micelles can capture acceptors via ah ost-guest interaction.…”

Section: Introduction Of Fret Pairs To Create Pep-cd Light-harvestingmentioning

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Hierarchical Assembly of Peptoid‐Based Cylindrical Micelles Exhibiting Efficient Resonance Energy Transfer in Aqueous Solution

Jiao

Jian

et al. 2019

Angewandte Chemie

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Herein we showt hat by appending bulky b-cyclodextrin (CD) groups onto sheet-forming peptoids,w eo btain cylindrical micelles that further assembly into membranes and intertwined ribbons on substrates in aqueous solution, depending on the choice of solution and substrate conditions.I nsitu atomic force microscopy( AFM) shows that micelle assembly occurs in two steps,s tarting with "precursor" particles that transform into worm-like micelles,w hiche xtend and coalesce to form the higher order structures with arate and adegree of cooperativity dependent on pH and Ca 2+ concentration. After co-assembly with hydrophobic 4-(2-hydroxyethylamino)-7nitro-2,1,3-benzoxadiazole (NBD) donors that occupyt he hydrophobic core,f ollowed by exposure to hydrophilic Rhodamine Ba sa cceptors that insert into cyclodextrin, the micelles exhibit highly efficient Fçrster resonance energy transfer efficiency in aqueous solution, thereby mimicking natural light harvesting systems.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

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Supramolecular Polymeric Fluorescent Nanoparticles Based on Quadruple Hydrogen Bonds

Peng

Sun

Niu

et al. 2016

Adv Funct Materials

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5483wileyonlinelibrary.com biocompatibility. Accordingly, there has been a surge in the exploitation of CPNs in numerous exciting studies. [ 9 ] Covalent polymers, however, suffer from the need for tedious chemical modifi cation to tune the emission color of their corresponding nanoparticles.Supramolecular polymers, which are formed from low-molecular-weight monomers by noncovalent interactions, provide a promising scaffold for the fabrication of fl uorescent nanoparticles with well fi ne-tuned emission properties. [ 10 ] On the one hand, the small building blocks of supramolecular polymers provide synthetic accessibility superior to that of covalent polymers. On the other hand, the excitation energy transfer from energy donor to acceptor fl uorophores of the monomers occurs effi ciently in supramolecular copolymers. Such a process can be used to adjust the emission properties of functional materials. [ 11 ] Recently, we have reported the synthesis of water-dispersible nanospheres of hydrogen-bonded supramolecular polymers by the miniemulsion method. [ 12 ] Bis-ureidopyrimidinone (Bis-UPy) monomers polymerized through the quadruple H-bonding of the ureidopyrimidinone (UPy) motif to form supramolecular polymers, [ 13 ] which further aggregated into nanospheres in the emulsifi ed organic droplets. Herein, we prepared FNPs based on fl uorophore-functionalized Bis-UPys by the miniemulsion method ( Scheme 1 ). The emission properties of the nanoparticles could be fi ne-tuned by effi cient excitation energy transfer in co-assemblies of the energy donor and acceptor fl uorophore-based monomers. The photoswitchable FNPs with high on-off fl uorescence contrast (85%) were prepared by copolymerization of Bis-UPys containing fl uorophore and photochromic dithienylethene. The FNPs have been successfully applied in cellular imaging and as fl uorescent inks. Results and Discussion Synthesis, Preparation, and Characterization of FNPsFour fl uorophore-functionalized Bis-UPys were synthesized for the preparation of supramolecular polymer-based fl uorescent nanoparticles: Based on their different emission colors, fl uorophore 9,10-diphenylanthracene, 1,3,5,7-tetramethyl boron dipyrromethene (BODIPY), 3,5-dithiolated BODIPY, and naphthalene bisimide were chosen as the functional groups A facile approach for the preparation of supramolecular polymer-based fl uorescent nanoparticles (FNPs) is reported. FNPs with homogeneous shape and size distribution are fabricated from low-molecular-weight molecules, and thus, different compositional constituents can be effi ciently incorporated via copolymerization. The emission color of the FNPs covers a wide region from blue to near infrared and can be easily tuned using effi cient excitation energy transfer. The photoswitchable fl uorescent nanoparticles with high on-off fl uorescence contrast are also simply prepared by copolymerization of monomers containing a fl uorophore and a photochromic unit. Our FNPs are successfully applied in living cell imaging and as fl uorescent inks.

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Light‐Harvesting Systems Based on Organic Nanocrystals To Mimic Chlorosomes

Cited by 157 publications

References 63 publications

Resonant Confinement of an Excitonic Polariton and Ultraefficient Light Harvest in Artificial Photosynthesis

Resonant Confinement of an Excitonic Polariton and Ultraefficient Light Harvest in Artificial Photosynthesis

Hierarchical Assembly of Peptoid‐Based Cylindrical Micelles Exhibiting Efficient Resonance Energy Transfer in Aqueous Solution

Supramolecular Polymeric Fluorescent Nanoparticles Based on Quadruple Hydrogen Bonds

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