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111.
Exploring the discrete complexes with multi-step coloration is still a challenge in the field of electron transfer photochromic materials. Herein, we synthesized a series of dinuclear Ln-diphosphonate compounds[Ln=Dy(1); Gd(2); Tb(3); Y(4)] with a remarkably and reversibly photoactive coloration phenomenon. These compounds showed two-step coloration behavior, which were the first discrete architectures in the reported electron transfer photochromic complexes. This two-step coloration phenomenon was originated from the large distortion of H3-TPT acceptors, which in turn reduced the π-conjugation of electron acceptors and slowed the decay process of electron transfer. The photogenerated stable doublet radicals originated from electron transfer from diphosphonate donor to polypyridine acceptor in these complexes were detected by UV-Vis and electron spin resonance(ESR) spectra. Furthermore, the photogenerated radicals were estimated by direct current magnetic susceptibilities and variable temperature ESR spectra, suggesting the doublet radicals in the dinuclear structure for all the compounds. This work revealed a series of discrete phosphonate-based systems with a multi-step coloration process, providing a new pathway for designing multicolor photochromic materials with potential photoswitching or other applications. 相似文献
112.
113.
Aaron D. W. Kennedy Isolde Sandler Prof. Joakim Andréasson Dr. Junming Ho Dr. Jonathon E. Beves 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(5):1103-1110
Three visible-light responsive photoswitches are reported, azobis(1-methyl-benzimidazole) ( 1 ), azobis(benzoxazole) ( 2 ) and azobis(benzothiazole) ( 3 ). Photostationary distributions are obtained upon irradiation with visible light comprising approximately 80 % of the thermally unstable isomer, with thermal half-lives up to 8 min and are mostly invariant to solvent. On protonation, compound 1 H+ has absorption extending beyond 600 nm, allowing switching with yellow light, and a thermal half-life just under 5 minutes. The two isomers have significantly different pKa values, offering potential as a pH switch. The absorption spectra of 2 and 3 are insensitive to acid, although changes in the thermal half-life of 3 indicate more basic intermediates that significantly influence the thermal barrier to isomerization. These findings are supported by high-level ab initio calculations, which validate that protonation occurs on the ring nitrogen and that the Z isomer is more basic in all cases. 相似文献
114.
Shi‐Chao Wei Dr. Mei Pan Yuan‐Zhong Fan Haoliang Liu Prof. Jianyong Zhang Prof. Cheng‐Yong Su 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(20):7418-7427
Creating cavities in varying levels, from molecular containers to macroscopic materials of porosity, have long been motivated for biomimetic or practical applications. Herein, we report an assembly approach to multiresponsive supramolecular gels by integrating photochromic metal–organic cages as predefined building units into the supramolecular gel skeleton, providing a new approach to create cavities in gels. Formation of discrete O‐Pd2L4 cages is driven by coordination between Pd2+ and a photochromic dithienylethene bispyridine ligand (O‐PyFDTE). In the presence of suitable solvents (DMSO or MeCN/DMSO), the O‐Pd2L4 cage molecules aggregate to form nanoparticles, which are further interconnected through supramolecular interactions to form a three‐dimensional (3D) gel matrix to trap a large amount of solvent molecules. Light‐induced phase and structural transformations readily occur owing to the reversible photochromic open‐ring/closed‐ring isomeric conversion of the cage units upon UV/visible light radiation. Furthermore, such Pd2L4 cage‐based gels show multiple reversible gel–solution transitions when thermal‐, photo‐, or mechanical stimuli are applied. Such supramolecular gels consisting of porous molecules may be developed as a new type of porous materials with different features from porous solids. 相似文献
115.
Regulation of Charge Delocalization in a Heteronuclear Fe2Ru System by a Stepwise Photochromic Process
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Guang‐Tao Xu Dr. Bin Li Dr. Jin‐Yun Wang Dr. Dao‐Bin Zhang Prof. Zhong‐Ning Chen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(8):3318-3326
Heteronuclear complexes FeCp2?DTE?C?C?Ru(dppe)2Cl ( 1 o ; dppe=1,2‐bis(diphenylphosphino)ethane, Cp=cyclopentadienyl, DTE=dithienylethene) and FeCp2?DTE?C?C?Ru(dppe)2?C?C?DTE?FeCp2 ( 2 oo ), with redox‐active ferrocenyl and ruthenium centers separated by a photochromic DTE moiety, were prepared to achieve photoswitchable charge delocalization and Fe???Ru electronic communication. Upon UV‐light irradiation of 2 oo , the Fe???Ru heterometallic electronic interaction is increasingly facilitated with stepwise photocyclization, 2 oo → 2 co → 2 cc ; this is ascribed to the gradual increase in π‐conjugated systems. The near‐infrared absorptions in mixed‐valence species [ 2 oo ]+/[ 2 co ]+/[ 2 cc ]+ are gradually intensified following the conversion of [ 2 oo ]+→[ 2 co ]+→[ 2 cc ]+, which demonstrates that the extent of charge delocalization shows progressive enhancement with stepwise photocyclization. As revealed by electrochemical, spectroscopic, and theoretical studies, complex 2 exhibits nine switchable states through stepwise photochromic and reversible redox processes. 相似文献
116.
Elarbi Chatir Dr. Martial Boggio-Pasqua Prof. Frederique Loiseau Dr. Christian Philouze Prof. Guy Royal Dr. Saioa Cobo 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(7):e202103755
A phenanthrene unit has been functionalized by several methylthiophene units in order to bring it a photochromic behavior. These compounds were characterized by NMR, absorption and emission spectroscopies, theoretical calculations as well as cyclic voltammetry. The association of a phenanthrene group with a photochromic center could open the door to a new generation of organic field-effect transistors. 相似文献
117.
Dr. Victor de Seauve Dr. Marie-Angélique Languille Dr. Mathieu Kociak Dr. Stéphanie Belin Dr. James Ablett Prof. Christine Andraud Prof. Odile Stéphan Dr. Jean-Pascal Rueff Dr. Emiliano Fonda Prof. Bertrand Lavédrine 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):9198-9204
The first colour photographs were created by a process introduced by Edmond Becquerel in 1848. The nature of these photochromatic images colours motivated a debate between scientists during the XIXth century, which is still not settled. We present the results of chemical analysis (EDX, HAXPES and EXAFS) and morphology studies (SEM, STEM) aiming at explaining the optical properties of the photochromatic images (UV-visible spectroscopy and low loss EELS). We rule out the two hypotheses (pigment and interferences) that have prevailed since 1848, respectively based on variations in the oxidation degree of the compound forming the sensitized layer and periodically spaced photolytic silver planes. A study of the silver nanoparticles dispersions contained in the coloured layers showed specific localizations and sizes distributions of the nanoparticles for each colour. These results allow us to formulate a plasmonic hypothesis on the origin of the photochromatic images colours. 相似文献
118.
Scalable Preparation of Photochromic Composite Foils with Excellent Reversibility for Light Printing
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Photochromic inks for repeatable light‐printed media have attracted increasing attention owing to the fact that they may be widely applied to reduce the consumption of papers and plastics and conserve the environment. Therefore, it is of practical significance to develop convenient photochromic inks with a low cost and on a large scale. In this study, a simple one‐step hydrothermal route was used to prepare tungsten trioxide (WO3) nanoparticles, which were further used to make photochromic inks and transparent photochromic films. The obtained transparent photochromic film could rapidly respond to UV light within tens of seconds, then return to its initial state, with different recovery times at different temperatures, and also exhibit good reversible coloration–bleaching effect. A typical polyethylene terephthalate (PET) foil coated with the photochromic ink could also be repeatedly printed with various patterns and displayed excellent rewritable performance over tens of cycles. This study proposes a simple method for widespread applications of WO3‐based photochromic inks. 相似文献
119.
H. Ünver M. Kabak D. Mehmet Zengin T. Nuri Durlu 《Journal of chemical crystallography》2001,31(4):203-209
1-[N-(4-chlorophenyl)]aminomethylidene-2(1H)naphthalenone (C17H12NOCl) (1) was synthesized and the crystal structure was determined. Compound 1 crystallizes in the monoclinic space group P21/n with a = 4.761(3) Å, b = 20.347(1) Å, c = 13.773(2) Å, = 92.89(3)°, V = 1332.4(3) Å3, Z = 4, D
c = 1.404 g cm–3, (Mo K) = 0.28 mm–1, and R = 0.036 for 2680 reflections [I > 2(I)]. Molecule 1 is not planar, and the dihedral angle between the naphthaldeyde plane A [C1–C11, 01] and the 4-chloroaniline plane B [C12–C17, C11, N1] is 20.1(3)°. An intramolecular hydrogen bond occurs between the hydroxyl oxygen and imine nitrogen atoms [2.528(3) Å]. IR, 1H NMR, and UV measurements and AM1 semiempirical quantum mechanical calculations support the keto form found in the X-ray structure. 相似文献
120.