Author response for "Facilitating Intrinsic Delayed Fluorescence of Conjugated Emitters by Inter-Chromophore Interaction"
Yixuan GaoYingman SunZilong GuoG. YuYaxin WangYan WanYandong HanWensheng YangDongbing ZhaoXiaonan Ma
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Delayed fluorescence (DF) is a unique emitting phenomenon of great interest for important applications in organic optoelectronics. In general, DF requires well-separated frontier orbitals, inherently corresponding to charge transfer (CT)-type emitters. However, facilitating intrinsic DF for local excited (LE)-type conjugated emitters remains very challenging. Aiming to overcome this obstacle, we demonstrate a new molecular design strategy with a DF-inactive B,N-multiple resonance (MR) emitter as a model system. Without the necessity of doping with heavy atoms, we synthesized a co-facial dimer in which an excimer-like state (S
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We have successfully synthesized several new substituted thiophene-based electro-optic chromophores. All of these chromophores have structures similar to FTC but they incorporated our newly designed tricyanovinyldihydrofuran acceptors. Since these acceptors possess an anisotropic structure, all of the chromophores are very soluble in a wide range of organic solvents. Thermal study of these chromophores by TGA shows all of them are very stable in air. UV spectra indicate the chromophores have a large solvatochromic effect, implying very large molecular nonlinearities.
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The Review begins with consideration of the absorption spectra of dyes whose molecules contain non-conjugated (isolated) chromophores. The major portion of the Review, however, is devoted to the spectra of dyes having two conjugated chromophores. According to the view adopted until recently the interaction of conjugated chromophores is apparent in a displacement of the absorption band to longer wavelengths and in an increase in its intensity. The Reviewer and his coworkers have recently established that this view is valid only for the particular case of conjugated chromophores which absorb similar light quanta and lie on the same straight line. If the light quanta absorbed by the conjugated chromophores are very different, the chromophores do not interact. If the conjugated chromophores are at an angle, their absorption bands do not merge into a single band: on the contrary, they either split or move apart. The intensities of the two new bands are then determined by the angle between the interacting chromophores. The spectra of bis-dyes which illustrate these principles are examined, and an elementary theory is given for the interaction of conjugated chromophores. A list of 61 references is included.
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Phenoxazine
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We have studied phenylenevinylene chromophore pairs whose spacing and orientation are varied by coupling them to peptide backbones. Copious interchromophore photoexcitations are observed and explain reduced fluorescence yields in conjugated polymer films relative to solutions.
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Photochromic dithienylethene moieties were covalently attached to fluorescent 4,4-difluoro-8-(4'-iodophenyl)-1,3,5,7-tetramethyl-4-bora-3a,4a-diaza-s-indacene (iodo-BODIPY) via a phenylacetylene linker. UV light induced isomerization of the photochrome results in significant decrease in fluorescence intensity. This fluorescence can be recovered with visible light. Steady-state fluorescence measurements demonstrate that the emission of the dye can be modulated by external light. An intramolecular energy transfer mechanism accounts for the fluorescence quenching in the UV light produced isomers.
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Abstract A novel class of fluorescent dyes based on the conformationally locked heterocyclic core of the chromophore of the fluorescent protein Kaede was discovered. Introduction of a single conformational lock at the benzylidene fragment of the Kaede chromophore resulted in an increase in the fluorescence quantum yield (FQY) by one order of magnitude and a redshift of ca. 60 nm in the emission spectrum. Imposing the second lock at the ethylene fragment of the Kaede chromophore provided a further increase in the FQY. Locked analogues demonstrated bright and redshifted emission in a broad range of solvents, which makes them good candidates for a wide spectrum of fluorescent‐labeling applications.
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When analyzing the emission of a large number of individual chromophores embedded in a matrix, the spread of the observed parameters is a characteristic property for the particular chromophore−matrix system. To quantitatively assess the influence of the matrix on the single molecule emission parameters, it is imperative to have a system with a well-defined chromophore nanoenvironment and the possibility to alter these surroundings in a precisely controlled way. Such a system is available in the form of the visible fluorescent proteins, where the chromophore nanoenvironment is defined by the specific protein sequence. We analyze the influence of the chromophore embedding within this defined protein environment on the distribution of the emission maximum wavelength for a number of variants of the fluorescent protein DsRed, and show that this parameter is characteristic of the chromophore−protein matrix combination and largely independent of experimental conditions. We observe that the chemical changes in the vicinity of the chromophore of different variants do not account for the different distributions of emission maximum positions but that the flexibility of the chromophore surrounding has a dominant role in determining the distribution. We find, surprisingly, that the more rigid the chromophore surrounding, the broader the distribution of observed maximum positions. We hypothesize that, after a thermally induced reorientation in the chromophore surrounding, a more flexible system can easily return to its energetic minimum position by fast reorientation, while in more rigid systems the return to the energetic minimum occurs in a stepwise fashion, leading to the broader distribution observed.
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