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1.
Dr. Chenge Li Dr. Alison G. Tebo Marion Thauvin Marie-Aude Plamont Prof. Dr. Michel Volovitch Dr. Xavier Morin Prof. Dr. Sophie Vriz Prof. Dr. Arnaud Gautier 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(41):18073-18079
Far-red emitting fluorescent labels are highly desirable for spectral multiplexing and deep tissue imaging. Here, we describe the generation of frFAST (far-red Fluorescence Activating and absorption Shifting Tag), a 14-kDa monomeric protein that forms a bright far-red fluorescent assembly with (4-hydroxy-3-methoxy-phenyl)allylidene rhodanine (HPAR-3OM). As HPAR-3OM is essentially non-fluorescent in solution and in cells, frFAST can be imaged with high contrast in presence of free HPAR-3OM, which allowed the rapid and efficient imaging of frFAST fusions in live cells, zebrafish embryo/larvae, and chicken embryos. Beyond enabling the genetic encoding of far-red fluorescence, frFAST allowed the design of a far-red chemogenetic reporter of protein–protein interactions, demonstrating its great potential for the design of innovative far-red emitting biosensors. 相似文献
2.
Romain Plais Guy Gouarin Dr. Anne Gaucher Violette Haldys Arnaud Brosseau Dr. Gilles Clavier Dr. Jean-Yves Salpin Prof. Dr. Damien Prim 《Chemphyschem》2020,21(12):1249-1257
The intrinsic properties of tetrazine as a π-anion receptor and as an on/off recognition probe merged with H-bond ability of an urea motif into a single architecture constitutes a new generation of well-defined anion receptors. Complexation properties directly benefit from the dual and synergistic contribution of tetrazine and urea. In this study, we report on the synthesis and assessment of binding properties to anions of diverse geometries. Association constants have been predicted by theoretical calculations and evaluated by multiple and complementary experimental techniques including electrospray-mass tandem spectroscopy, NMR, UV-visible, steady state fluorescence spectroscopies and time resolved fluorescence. These results provide the basis for a better understanding of both the complexation and the anion-dependent quenching mechanism. 相似文献
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4.
Manon Catherin Olatz Uranga-Barandiaran Arnaud Brosseau Dr. Rémi Métivier Dr. Gabriel Canard Dr. Anthony D'Aléo Dr. David Casanova Prof. Frédéric Castet Dr. Elena Zaborova Prof. Frédéric Fages 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(17):3818-3828
We describe the synthesis of a series of covalently linked dimers of quadrupolar curcuminoid-BF2 dyes and the detailed investigation of their solvent-dependent spectroscopic and photophysical properties. In solvents of low polarity, intramolecular folding induces the formation of aggregated chromophores, the UV/Vis absorption spectra of which display the optical signature characteristic of weakly-coupled H-aggregates. The extent of folding and, in turn, of ground-state aggregation is strongly dependent on the nature of the flexible linker. Steady-state and time-resolved fluorescence emission spectroscopies show that the Frenkel exciton relaxes into a fluorescent symmetrical excimer state with a long lifetime. Furthermore, our in-depth studies show that a weakly emitting excimer lies on the pathway toward a photocyclomer. Two-dimensional 1H NMR spectroscopy and density functional theory (DFT) allowed the structure of the photoproduct to be established. To our knowledge, this represents the first example of a [2π+2π] photodimerization of the curcuminoid chromophore. 相似文献
5.
Joy Ann Panis Prof. Marine Louis Arnaud Brosseau Shouhei Katao Florencio de los Reyes Prof. Takuya Nakashima Dr. Rémi Métivier Dr. Clémence Allain Prof. Tsuyoshi Kawai 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(44):e202201012
We synthesized two bichromophoric difluoroboron-β-diketonates (DFB) connected in para and meta positions by using cyclohexane diamine as a chiral bridge ( para and meta (R/S)-CyDFB ). TD-DFT calculations revealed that the variation in connectivity of the DFB units leads to different spatial arrangements and a chirality inversion of the bichromophoric DFB. Higher gabs values were obtained in (R/S)-CyDFB connected in para as compared to meta position. Aggregation of para (R/S)-CyDFB in mixture of solvents increase the glum values as compared to its monomeric form. Ultrasonication and heating induced the formation of highly ordered nano-helical wires of para (R/S)-CyDFB that increased the glum values to 0.015. On the other hand, meta (R/S)-CyDFB failed to form highly ordered self-assembled wires due to hindered H-binding sites. These observations indicate that the chiroptical properties of DFB bi-chromophore system can be modulated with self-assembly and spatial arrangement of the chromophores. 相似文献
6.
Strong,Thermally Superinsulating Biopolymer–Silica Aerogel Hybrids by Cogelation of Silicic Acid with Pectin 下载免费PDF全文
Dr. Shanyu Zhao Dr. Wim J. Malfait Dr. Arnaud Demilecamps Dr. Yucheng Zhang Dr. Samuel Brunner Lukas Huber Dr. Philippe Tingaut Dr. Arnaud Rigacci Dr. Tatiana Budtova Dr. Matthias M. Koebel 《Angewandte Chemie (International ed. in English)》2015,54(48):14282-14286
Silica aerogels are excellent thermal insulators, but their brittle nature has prevented widespread application. To overcome these mechanical limitations, silica–biopolymer hybrids are a promising alternative. A one‐pot process to monolithic, superinsulating pectin–silica hybrid aerogels is presented. Their structural and physical properties can be tuned by adjusting the gelation pH and pectin concentration. Hybrid aerogels made at pH 1.5 exhibit minimal dust release and vastly improved mechanical properties while remaining excellent thermal insulators. The change in the mechanical properties is directly linked to the observed “neck‐free” nanoscale network structure with thicker struts. Such a design is superior to “neck‐limited”, classical inorganic aerogels. This new class of materials opens up new perspectives for novel silica–biopolymer nanocomposite aerogels. 相似文献
7.
Eliminating the contribution of interfering compounds is a key step in chemical analysis. In complex media, one possible approach is to perform a preliminary separation. However purification is often demanding, long, and costly; it may also considerably alter the properties of interacting components of the mixture (e.g. in a living cell). Hence there is a strong interest for developing separation-free non-invasive analytical protocols. Using photoswitchable probes as labelling and titration contrast agents, we demonstrate that the association of a modulated monochromatic light excitation with a kinetic filtering of the overall observable is much more attractive than constant excitation to read-out the contribution from a target probe under adverse conditions. An extensive theoretical framework enabled us to optimize the out-of-phase concentration first-order response of a photoswitchable probe to modulated illumination by appropriately matching the average light intensity and the radial frequency of the light modulation to the probe dynamics. Thus, we can selectively and quantitatively extract from an overall signal the contribution from a target photoswitchable probe within a mixture of species, photoswitchable or not. This simple titration strategy is more specifically developed in the context of fluorescence imaging, which offers promising perspectives. 相似文献
8.
We study the decimation to a sublattice of half the sites of the one-dimensional Dyson–Ising ferromagnet with slowly decaying long-range pair potentials of the form , deep in the phase transition region ( and low temperature). We prove non-Gibbsianness of the decimated measures at low enough temperatures by exhibiting a point of essential discontinuity for the (finite-volume) conditional probabilities of decimated Gibbs measures. This result complements previous work proving conservation of Gibbsianness for fastly decaying potentials () and provides an example of a “standard” non-Gibbsian result in one dimension, in the vein of similar results in higher dimensions for short-range models. We also discuss how these measures could fit within a generalized (almost vs. weak) Gibbsian framework. Moreover we comment on the possibility of similar results for some other transformations. 相似文献
9.
Dr. Abdulghani Ismail Dr. Silvia Voci Lucie Descamps Dr. Arnaud Buhot Prof. Dr. Neso Sojic Dr. Loïc Leroy Dr. Aurélie Bouchet-Spinelli 《Chemphyschem》2021,22(11):1094-1100
This work depicts the original combination of electrochemiluminescence (ECL) and bipolar electrochemistry (BPE) to map in real-time the oxidation of silicon in microchannels. We fabricated model silicon-PDMS microfluidic chips, optionally containing a restriction, and monitored the evolution of the surface reactivity using ECL. BPE was used to remotely promote ECL at the silicon surface inside microfluidic channels. The effects of the fluidic design, the applied potential and the resistance of the channel (controlled by the fluidic configuration) on the silicon polarization and oxide formation were investigated. A potential difference down to 6 V was sufficient to induce ECL, which is two orders of magnitude less than in classical BPE configurations. Increasing the resistance of the channel led to an increase in the current passing through the silicon and boosted the intensity of ECL signals. Finally, the possibility of achieving electrochemical reactions at predetermined locations on the microfluidic chip was investigated using a patterning of the silicon oxide surface by etched micrometric squares. This ECL imaging approach opens exciting perspectives for the precise understanding and implementation of electrochemical functionalization on passivating materials. In addition, it may help the development and the design of fully integrated microfluidic biochips paving the way for development of original bioanalytical applications. 相似文献
10.
Florian Venel Dr. Hiroki Nagashima Dr. Andrew G. M. Rankin Christelle Anquetil Dr. Vytautas Klimavicius Dr. Torsten Gutmann Prof. Gerd Buntkowsky Dr. Sylvie Derenne Prof. Olivier Lafon Dr. Arnaud Huguet Dr. Frédérique Pourpoint 《Chemphyschem》2021,22(18):1907-1913
Estuaries are key ecosystems with unique biodiversity and are of high economic importance. Along the estuaries, variations in environmental parameters, such as salinity and light penetration, can modify the characteristics of dissolved organic matter (DOM). Nevertheless, there is still limited information about the atomic-level transformations of DOM in this ecosystem. Solid-state NMR spectroscopy provides unique insights into the nature of functional groups in DOM. A major limitation of this technique is its lack of sensivity, which results in experimental time of tens of hours for the acquisition of 13C NMR spectra and generally precludes the observation of 15N nuclei for DOM. We show here how the sensitivity of solid-state NMR experiments on DOM of Seine estuary can be enhanced using dynamic nuclear polarization (DNP) under magic-angle spinning. This technique allows the acquisition of 13C NMR spectra of these samples in few minutes, instead of hours for conventional solid-state NMR. Both conventional and DNP-enhanced 13C NMR spectra indicate that the 13C local environments in DOM are not strongly modified along the Seine estuary. Furthermore, the sensitivity gain provided by the DNP allows the detection of 15N NMR signal of DOM, in spite of the low nitrogen content. These spectra reveal that the majority of nitrogen is in the amide form in these DOM samples and show an increased disorder around these amide groups near the mouth of the Seine. 相似文献