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81.
Mono‐ and Bis(pyrrolo)tetrathiafulvalene Derivatives Tethered to C60: Synthesis,Photophysical Studies,and Self‐Assembled Monolayers 下载免费PDF全文
Dr. Marta Vico Solano Dr. Eduardo Antonio Della Pia Dr. Martyn Jevric Christina Schubert Xintai Wang Dr. Cornelia van der Pol Prof. Dr. Anders Kadziola Prof. Dr. Kasper Nørgaard Prof. Dr. Dirk M. Guldi Prof. Dr. Mogens Brøndsted Nielsen Prof. Dr. Jan O. Jeppesen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(32):9918-9929
A series of mono‐ (MPTTF) and bis(pyrrolo)tetrathiafulvalene (BPTTF) derivatives tethered to one or two C60 moieties was synthesized and characterized. The synthetic strategy for these dumbbell‐shaped compounds was based on a 1,3‐dipolar cycloaddition reaction between aldehyde‐functionalized MPTTF/BPTTF derivatives, two different tailor‐made amino acids, and C60. Electronic communication between the MPTTF/BPTTF units and the C60 moieties was studied by a variety of techniques including cyclic voltammetry and absorption spectroscopy. These solution‐based studies indicated no observable electronic communication between the MPTTF/BPTTF units and the C60 moieties. In addition, femtosecond and nanosecond transient absorption spectroscopy revealed, rather surprisingly, that no charge transfer from the MPTTF/BPTTF units to the C60 moieties takes place on excitation of the fullerene moiety. Finally, it was shown that the MPTTF–C60 and C60–BPTTF‐C60 dyad and triad molecules formed self‐assembled monolayers on a Au(111) surface by anchoring to C60. 相似文献
82.
Inside Cover: Bioinspired Intramolecular Diels–Alder Reaction: A Rapid Access to the Highly‐Strained Cyclopropane‐Fused Polycyclic Skeleton (Chem. Eur. J. 9/2014) 下载免费PDF全文
83.
HOMO Stabilisation in π‐Extended Dibenzotetrathiafulvalene Derivatives for Their Application in Organic Field‐Effect Transistors 下载免费PDF全文
Dr. Yan Geng Dr. Raphael Pfattner Antonio Campos Prof. Wei Wang Dr. Olivier Jeannin Dr. Jürg Hauser Dr. Joaquim Puigdollers Prof. Stefan T. Bromley Prof. Silvio Decurtins Prof. Jaume Veciana Prof. Concepció Rovira Dr. Marta Mas‐Torrent Dr. Shi‐Xia Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(50):16672-16679
Three new organic semiconductors, in which either two methoxy units are directly linked to a dibenzotetrathiafulvalene (DB‐TTF) central core and a 2,1,3‐chalcogendiazole is fused on the one side, or four methoxy groups are linked to the DB‐TTF, have been synthesised as active materials for organic field‐effect transistors (OFETs). Their electrochemical behaviour, electronic absorption and fluorescence emission as well as photoinduced intramolecular charge transfer were studied. The electron‐withdrawing 2,1,3‐chalcogendiazole unit significantly affects the electronic properties of these semiconductors, lowering both the HOMO and LUMO energy levels and hence increasing the stability of the semiconducting material. The solution‐processed single‐crystal transistors exhibit high performance with a hole mobility up to 0.04 cm2 V?1 s?1 as well as good ambient stability. 相似文献
84.
Systematic Tuning and Switching of Neutral and Ionic Phases in a Donor–Acceptor Chain Compound by Doping with Less‐Active Donors and by Pressure Application 下载免费PDF全文
Keita Nakabayashi Prof. Dr. Hitoshi Miyasaka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(17):5121-5131
The temperature‐induced stepwise neutral–ionic (N–I) phase transition in the covalently bonded donor–acceptor chain compound [Ru2(2,3,5,6‐F4PhCO2)4DMDCNQI] ? 2(p‐xylene) (2,3,5,6‐F4PhCO2?=2,3,5,6‐tetrafluorobenzoate; DMDCNQI=2,5‐dimethyl‐N,N′‐dicyanoquinodiimine) was systematically tuned over a wide temperature range using two techniques: 1) A chemical technique based on doping with a less‐active donor unit [Ru2II,II(F5PhCO2)4] (F5PhCO2?=pentafluorobenzoate), thereby providing an isostructural doped series [{Ru2II,II(2,3,5,6‐F4PhCO2)4}1?x{Ru2II,II(F5PhCO2)4}xDMDCNQI] ? 2(p‐xylene), with x=0.06, 0.10, 0.21, and 0.24; and 2) a physical technique, which was the application of hydrostatic pressure to the doped compounds. The stepwise N–I transition observed in the original compound was systematically varied in terms of the viewpoints of both transition temperature and transition features (stepwise or monotonic) dependent on the amount of dopants x. Application of pressure efficiently tuned the N–I transitions, with the oxidation phases being dramatically modified by applying only weak pressure up to 4 kbar. Even in cases that led to N–I transitions in small domains of the chains at ambient pressure, the application of pressure caused an expansion of the domains that enabled N–I transitions, finally leading to a complete change in the oxidation state of the chains, from neutral to ionic, accompanied by a change from a paramagnetic state to a ferrimagnetically ordered state. 相似文献
85.
Synthesis and Photophysical Properties of Multichromophoric Carbonyl‐Bridged Triarylamines 下载免费PDF全文
Natalie Hammer Dr. Richard Hildner Dr. Milan Kivala Prof. Dr. Jürgen Köhler Prof. Hans‐Werner Schmidt 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(37):11708-11718
The synthesis and photophysical properties of two novel multichromophoric compounds is presented. Their molecular design comprises a carbonyl‐bridged triarylamine core and either naphthalimides or 4‐(5‐hexyl‐2,2′‐bithiophene)naphthalimides as second chromophore in the periphery. The lateral chromophores are attached to the core via an amide linkage and a short alkyl spacer. The synthetic approach demonstrates a straightforward functionalization strategy for carbonyl‐bridged triarylamines. Steady‐state and time‐resolved spectroscopic investigations of these compounds, in combination with three reference compounds, provide clear evidence for energy transfer in both multichromophoric compounds. The direction of the energy transfer depends on the lateral chromophore used. Furthermore, the compound bearing the lateral 4‐(bithiophene)naphthaimides is capable of forming fluorescent gels at very low concentrations in the sub‐millimolar regime whilst retaining its energy transfer properties. 相似文献
86.
Experimental and Computational Studies of a Multi‐Electron Donor–Acceptor Ligand Containing the Thiazolo[5,4‐d]thiazole Core and its Incorporation into a Metal–Organic Framework 下载免费PDF全文
Felix J. Rizzuto Dr. Thomas B. Faust Dr. Bun Chan Carol Hua Dr. Deanna M. D'Alessandro Prof. Cameron J. Kepert 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(52):17597-17605
A ligand containing the thiazolo[5,4‐d]thiazole (TzTz) core (acceptor) with terminal triarylamine moieties (donors), N,N′‐(thiazolo[5,4‐d]thiazole‐2,5‐diylbis(4,1‐phenylene))bis(N‐(pyridine‐4‐yl)pyridin‐4‐amine ( 1 ), was designed as a donor–acceptor system for incorporation into electronically active metal–organic frameworks (MOFs). The capacity for the ligand to undergo multiple sequential oxidation and reduction processes was examined using UV/Vis‐near‐infrared spectroelectrochemistry (UV/Vis‐NIR SEC) in combination with DFT calculations. The delocalized nature of the highest occupied molecular orbital (HOMO) was found to inhibit charge‐transfer interactions between the terminal triarylamine moieties upon oxidation, whereas radical species localized on the TzTz core were formed upon reduction. Conversion of 1 to diamagnetic 2+ and 4+ species resulted in marked changes in the emission spectra. Incorporation of this highly delocalized multi‐electron donor–acceptor ligand into a new two‐dimensional MOF, [Zn(NO3)2( 1 )] ( 2 ), resulted in an inhibition of the oxidation processes, but retention of the reduction capability of 1 . Changes in the electrochemistry of 1 upon integration into 2 are broadly consistent with the geometric and electronic constraints enforced by ligation. 相似文献
87.
Precision PEGylated Polymers Obtained by Sequence‐Controlled Copolymerization and Postpolymerization Modification 下载免费PDF全文
Sansanee Srichan Dr. Hatice Mutlu Dr. Nezha Badi Dr. Jean‐François Lutz 《Angewandte Chemie (International ed. in English)》2014,53(35):9231-9235
Copolymers containing water‐soluble poly(ethylene glycol) (PEG) side chains and precisely controlled functional microstructures were synthesized by sequence‐controlled copolymerization of donor and acceptor comonomers, that is, styrene derivatives and N‐substituted maleimides. Two routes were compared for the preparation of these structures: a) the direct use of a PEG–styrene macromonomer as a donor comonomer, and b) the use of an alkyne‐functionalized styrenic comonomer, which was PEGylated by copper‐catalyzed alkyne–azide cycloaddition after polymerization. The latter method was found to be the most versatile and enabled the synthesis of high‐precision copolymers. For example, PEGylated copolymers containing precisely positioned fluorescent (e.g. pyrene), switchable (e.g. azobenzene), and reactive functionalities (e.g. an activated ester) were prepared. 相似文献
88.
Stereospecific Formal [3+2] Dipolar Cycloaddition of Cyclopropanes with Nitrosoarenes: An Approach to Isoxazolidines 下载免费PDF全文
Shyamal Chakrabarty Dr. Indranil Chatterjee Birgit Wibbeling Dr. Constantin Gabriel Daniliuc Prof. Dr. Armido Studer 《Angewandte Chemie (International ed. in English)》2014,53(23):5964-5968
The MgBr2‐catalyzed formal [3+2] cycloaddition of donor–acceptor activated cyclopropanes with nitrosoarenes offers a novel approach to various structurally diverse isoxazolidines. The reactions, which are experimentally easy to conduct, occur with complete stereospecificity and perfect control of regioselectivity. Product isoxazolidines can be readily transformed into α‐amino lactones by reductive or decarboxylative N? O cleavage and subsequent lactonisation, and the N‐aryl bond cleavage is also possible under oxidative conditions. 相似文献
89.
Luminous Butterflies: Efficient Exciton Harvesting by Benzophenone Derivatives for Full‐Color Delayed Fluorescence OLEDs 下载免费PDF全文
Sae Youn Lee Prof. Dr. Takuma Yasuda Dr. Yu Seok Yang Dr. Qisheng Zhang Prof. Dr. Chihaya Adachi 《Angewandte Chemie (International ed. in English)》2014,53(25):6402-6406
Butterfly‐shaped luminescent benzophenone derivatives with small energy gaps between their singlet and triplet excited states are used to achieve efficient full‐color delayed fluorescence. Organic light‐emitting diodes (OLEDs) with these benzophenone derivatives doped in the emissive layer can generate electroluminescence ranging from blue to orange–red and white, with maximum external quantum efficiencies of up to 14.3 %. Triplet excitons are efficiently harvested through delayed fluorescence channels. 相似文献
90.
Pd Uptake and H2S Sensing by an Amphoteric Metal–Organic Framework with a Soft Core and Rigid Side Arms 下载免费PDF全文
Jieshun Cui Yan‐Lung Wong Dr. Matthias Zeller Dr. Allen D. Hunter Dr. Zhengtao Xu 《Angewandte Chemie (International ed. in English)》2014,53(52):14438-14442
Molecular components of opposite character are often incorporated within a single system, with a rigid core and flexible side arms being a common design choice. Herein, molecule L has been designed and prepared featuring the reverse design, with rigid side arms (arylalkynyl) serving to calibrate the mobility of the flexible polyether links in the core. Crystallization of this molecule with PbII ions led to a dynamic metal–organic framework (MOF) system that not only exhibits dramatic, reversible single‐crystal‐to‐single‐crystal transformations, but combines distinct donor and acceptor characteristics, allowing for substantial uptake of PdCl2 and colorimetric sensing of H2S in water. 相似文献