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YbCu5−x
Al
x
provides the possibility to tune ground state properties by a change of the valence due to the Cu/Al substitution, by pressure
as well as by the application of a magnetic field. Near to the critical concentration x
cr≈1.5 non-Fermi-liquid properties (NFL) are obvious, obeying hyperscaling. If magnetic order sets in for x>1.5, the application of moderate magnetic fields quenches order and again NFL features become evident. Hyperscaling in this
case indicates strongly interacting spin fluctuations. 相似文献
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Lucien N. Lameijer Simon Budzak Nadja A. Simeth Mickel J. Hansen Ben L. Feringa Denis Jacquemin Wiktor Szymanski 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21847-21854
Molecular photoswitches enable reversible external control of biological systems, nanomachines, and smart materials. Their development is driven by the need for low energy (green-red-NIR) light switching, to allow non-invasive operation with deep tissue penetration. The lack of clear design principles for the adaptation and optimization of such systems limits further applications. Here we provide a design rulebook for tetra-ortho-chloroazobenzenes, an emerging class of visible-light-responsive photochromes, by elucidating the role that substituents play in defining their key characteristics: absorption spectra, band overlap, photoswitching efficiencies, and half-lives of the unstable cis isomers. This is achieved through joint photochemical and theoretical analyses of a representative library of molecules featuring substituents of varying electronic nature. A set of guidelines is presented that enables tuning of properties to the desired application through informed photochrome engineering. 相似文献
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Hogendorf WF Lameijer LN Beenakker TJ Overkleeft HS Filippov DV Codée JD Van der Marel GA 《Organic letters》2012,14(3):848-851
The use of perfluorooctylpropylsulfonylethanol as a new phosphate protecting group and fluorous linker is evaluated in the stepwise solution phase synthesis of a number of biologically relevant (carbohydrate substituted) glycerol teichoic acid fragments. Teichoic acid fragments, up to the dodecamer level, were assembled by means of phosphoramidite chemistry, using a relatively small excess of the building blocks and a repetitive efficient purification procedure of the protected intermediates by fluorous solid phase extraction (F-SPE). 相似文献
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d‐ Versus l‐Glucose Conjugation: Mitochondrial Targeting of a Light‐Activated Dual‐Mode‐of‐Action Ruthenium‐Based Anticancer Prodrug
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Lucien N. Lameijer Dr. Samantha L. Hopkins Tobias G. Brevé Sven H. C. Askes Dr. Sylvestre Bonnet 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(51):18484-18491
Light‐activated ruthenium polypyridyl anticancer prodrugs often suffer from poor water solubility, poor selectivity, and/or ill‐defined intracellular targets. Coordination of the d ‐ or l ‐glucose thioether ligand 3 (2‐(2‐(2‐(methylthio)ethoxy)ethoxy)ethyl‐β‐glucopyranoside) to the highly lipophilic ruthenium complex [Ru(tpy)(dppn)(H2O)]2+ ([ 1 ]2+; dppn=benzo[i]dipyrido‐[3,2‐a:2′,3′‐c]phenazine, tpy=2,2′:6′,2′′‐terpyridine) solved all these problems at once. The two enantiomers of [Ru(tpy)(dppn)( 3) ][PF6]2, [d ‐ 2 ][PF6]2 and [l ‐ 2 ][PF6]2, were soluble in water, which allowed the influence of the chirality of the glucose moiety on uptake, toxicity, and intracellular localization of the prodrug to be probed without changing any other physicochemical properties. Both compounds showed mild, but different, cytotoxicity in A549 (human lung carcinoma) and MCF‐7 (human breast adenocarcinoma) cancer cells in the dark, whereas following low doses of visible light irradiation (3.1 J cm?2 at λ = 454 nm), a similar, but high cytotoxicity (EC50 < 1 μm ), was observed. Irrespective of the chirality, both slightly emissive Ru complexes were found in the mitochondria, and two modes of action may contribute to light‐induced cell death: 1) the glucose thioether ligand is photosubstituted by water, thus [ 1 ]2+, which interacts with DNA at an exceptionally high 400:1 base pair/Ru ratio, is released; 2) both [ 1 ]2+ and [ 2 ]2+ produce massive amounts of singlet oxygen, which leads to very efficient photodynamic DNA cleavage. 相似文献
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Hans A. V. Kistemaker Lucien N. Lameijer Nico J. Meeuwenoord Prof. Dr. Herman S. Overkleeft Prof. Dr. Gijsbert A. van der Marel Dr. Dmitri V. Filippov 《Angewandte Chemie (International ed. in English)》2015,54(16):4915-4918
The post‐translational modification of proteins that is known as adenosine diphosphate ribosylation (ADPr) regulates a wide variety of important biological processes, such as DNA‐damage repair and cellular metabolism. This modification is also involved in carcinogenesis and the process of aging. Therefore, a better understanding of the function of ADP‐ribosylation is crucial for the development of novel therapeutics. To facilitate the elucidation of the biology of ADPr, the availability of well‐defined fragments of poly(ADP‐ribose) is essential. Herein we report a solid‐phase synthetic approach for the preparation of ADP‐ribose oligomers of exactly defined length. The methodology is exemplified by the first reported synthesis of an ADP‐ribose dimer and trimer. 相似文献
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Lameijer EW Kok JN Bäck T Ijzerman AP 《Journal of chemical information and modeling》2006,46(2):545-552
We developed a software tool to design drug-like molecules, the "Molecule Evoluator", which we introduce and describe here. An atom-based evolutionary approach was used allowing both several types of mutation and crossover to occur. The novelty, we claim, is the unprecedented interactive evolution, in which the user acts as a fitness function. This brings a human being's creativity, implicit knowledge, and imagination into the design process, next to the more standard chemical rules. Proof-of-concept was demonstrated in a number of ways, both computationally and in the lab. Thus, we synthesized a number of compounds designed with the aid of the Molecule Evoluator. One of these is described here, a new chemical entity with activity on alpha-adrenergic receptors. 相似文献
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Lameijer EW Kok JN Bäck T Ijzerman AP 《Journal of chemical information and modeling》2006,46(2):553-562
Nowadays millions of different compounds are known, their structures stored in electronic databases. Analysis of these data could yield valuable insights into the laws of chemistry and the habits of chemists. We have therefore explored the public database of the National Cancer Institute (>250,000 compounds) by pattern searching. We split the molecules of this database into fragments to find out which fragments exist, how frequent they are, and whether the occurrence of one fragment in a molecule is related to the occurrence of another, nonoverlapping fragment. It turns out that some fragments and combinations of fragments are so frequent that they can be called "chemical clichés". We believe that the fragment data can give insight into the chemical space explored so far by synthesis. The lists of fragments and their (co-)occurrences can help create novel chemical compounds by (i) systematically listing the most popular and therefore most easily used substituents and ring systems for synthesizing new compounds, (ii) being an easily accessible repository for rarer fragments suitable for lead compound optimization, and (iii) pointing out some of the yet unexplored parts of chemical space. 相似文献
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