Thermally activated delayed fluorescence (TADF)‐type compounds have great potential as emitter molecules in organic light‐emitting diodes, allowing for electrofluorescence with 100% internal quantum efficiency. In small molecules, TADF is achieved through the formation of intramolecular charge‐transfer states. The only design limitation is the requirement that donor and acceptor entities spatially decouple the highest occupied and lowest unoccupied molecular orbitals, respectively, to minimize exchange splitting. The development of polymeric TADF emitters, on the contrary, has seen comparably small progress and those are typically built up from monomeric units that show promising TADF properties in small molecule studies beforehand. By contrast, herein, a way to achieve TADF properties in cyclic oligomers and polymers composed of non‐TADF building blocks is shown. Due to a strongly decreased energy splitting of the polymer with respect to the individual repeating unit between the lowest singlet and triplet excited state (ΔEST) and a sufficiently high radiative decay rate kSr, a highly efficient TADF polymer with up to 71% photoluminescence quantum yield is obtained. For the first time, an encouraging method is provided for producing highly efficient TADF oligomers and polymers from solely non‐TADF units via induced conjugation, opening a new design strategy exclusive for polymers.
Infrared spectroscopic ellipsometry (IRSE), reflection absorption IR spectroscopy (RAIRS), IR transmission spectroscopy, and best-fit calculations are applied in a cooperative study to determine the anisotropic optical properties of a thin polyimide layer in the spectral range 4000–500 cm−1. The employed anisotropic uniaxial optical layer model afforded very good agreement between the calculated and the experimental spectra obtained by the different complementary IR methods. The main advantage of IRSE is that it is possible to obtain data for the optical constants and the thickness ( d = 1.81 μm) of the polyimide layer simultaneously within one experiment. From the ellipsometric spectra it was concluded that the layer structure can be regarded as possessing uniaxial symmetry where the layer is isotropic in directions (x, y) parallel to the sample surface. A qualitative determination of the anisotropic parameters of vibrational bands is possible by calculation of the ellipsometric spectra. The evaluation procedure can be improved by evaluation of polarized reflection spectra, provided the reference standard has been calibrated by ellipsometry. The oscillator parameters are then derived more accurately from the separate s- and p-polarized reflection spectra rather than from their ratio, which is measured in ellipsometry.
Matrix-assisted laser desorption/ionization mass spectrometry (MALDI MS) and MALDI MS imaging are ubiquitous analytical methods in medical, pharmaceutical, biological, and environmental research. Currently, there is a strong interest in the investigation of low molecular weight compounds (LMWCs), especially to trace and understand metabolic pathways, requiring the development of new matrix systems that have favorable optical properties and a high ionization efficiency and that are MALDI silent in the LMWC area. In this paper, five conjugated polymers, poly{[ N, N'-bis(2-octyldodecyl)-naphtalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]- alt-5,5'(2,2'-bithiophene)} (PNDI(T2)), poly(3-dodecylthiophene-2,5-diyl) (P3DDT), poly{[2,3-bis(3-octyloxyphenyl)quinoxaline-5,8-diyl]- alt-(thiophene-2,5-diyl)} (PTQ1), poly{[ N, N'-bis(2-octyldodecyl)-isoindigo-5,5'-diyl] -alt-5,5'(2,2'-bithiophene)} (PII(T2)), and poly(9,9-di- n-octylfluorenyl-2,7-diyl) (P9OFl) are investigated as matrices. The polymers have a strong optical absorption, are solution processable, and can be coated into thin films, allowing a vast reduction in the amount of matrix used. All investigated polymers function as matrices in both positive and negative mode MALDI, classifying them as rare dual-mode matrices, and show a very good analyte ionization ability in both modes. PNDI(T2), P3DDT, PTQ1, and PII(T2) are MALDI silent in the full measurement range (> m/ z = 150k), except at high laser intensities. In MALDI MS experiments of single analytes and a complex biological sample, the performance of the polymers was found to be as good as two commonly used matrices (2,5-DHB for positive and 9AA for negative mode measurements). The detection limit of two standard analytes was determined as being below 164 pmol for reserpine and below 245 pmol for cholic acid. Additionally P3DDT was used successfully in first MALDI MS imaging experiments allowing the visualization of the tissue morphology of rat brain sections.
The phenomenon of contact angle hysteresis was studied on smooth films of polyimide, a polymer type used in the microelectronic industry, by dynamic cycling contact angle measurements based on axisymmetric drop shape analysis-profile in combination with variable angle spectroscopic ellipsometry (VASE). It was found that both advancing and receding contact angles became smaller with increasing the number of cycles and are, therefore, not a property of the dry solid alone. The changes of the wetting behavior during these dynamic cycling contact angle measurements are attributed mainly to swelling and/or liquid retention. To reveal the water-induced changes of the polymer film, the polyimide surface was studied before and after the contact with a water droplet by VASE. Both the experimental ellipsometric spectrum for Delta and that for Psi as well as the corresponding simulations show characteristic shifts due to the contact with water. The so-called effective medium approximation was applied to recover information about the thickness and effective optical constants of the polymer layer from the ellipsometrically measured values of Delta and Psi. On the basis of these results, the swelling and retention behavior of the polyimide films in contact with water droplets were discussed.
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