@article{WadeWoodColladoFregosoetal.2017, author = {Wade, Jessica and Wood, Sebastian and Collado-Fregoso, Elisa and Heeney, Martin and Durrant, James and Kim, Ji-Seon}, title = {Impact of Fullerene Intercalation on Structural and Thermal Properties of Organic Photovoltaic Blends}, series = {The journal of physical chemistry : C, Nanomaterials and interfaces}, volume = {121}, journal = {The journal of physical chemistry : C, Nanomaterials and interfaces}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.7b05893}, pages = {20976 -- 20985}, year = {2017}, abstract = {The performance of organic photovoltaic blend devices is critically dependent on the polymer:fullerene interface. These interfaces are expected to impact the structural and thermal properties of the polymer with regards to the conjugated backbone planarity and transition temperatures during annealing/cooling processes. Here, we report the impact of fullerene intercalation on structural and thermal properties of poly(2,5-bis(3-tetradecylthiophen-2-yOthieno[3,2-b]thiophene (PBTTT), a highly stable material known to exhibit liquid crystalline behavior. We undertake a detailed systematic study of the extent of intercalation in the PBTTT:fullerene blend, considering the use of four different fullerene derivatives and also varying the loading ratios. Resonant Raman spectroscopy allows morphology in situ during controlled heating and cooling. We find that small fullerene molecules readily intercalate into PBTTT crystallites, resulting in a planarization of the polymer backbone, but high fullerene loading ratios or larger fullerenes result in nonintercalated domains. During cooling from melt, nonintercalated blend films are found to return to their original morphology and reproduce all thermal transitions on cooling with minimal hysteresis. Intercalated blend films show significant hysteresis on cooling due to the crystallized fullerene attempting to reintercalate. The strongest hysteresis is for intercalated blend films with excess fullerene loading ratio, which form a distinct nanoribbon morphology and exhibit a reduced geminate recombination rate. These results reveal that careful consideration should be taken during device fabrication, as postdeposition thermal treatments significantly impact the charge generation and recombination dynamics.}, language = {en} } @article{FudickarLinker2017, author = {Fudickar, Werner and Linker, Torsten}, title = {Synthesis of Pyridylanthracenes and Their Reversible Reaction with Singlet Oxygen to Endoperoxides}, series = {The journal of organic chemistry}, volume = {82}, journal = {The journal of organic chemistry}, publisher = {American Chemical Society}, address = {Washington}, issn = {0022-3263}, doi = {10.1021/acs.joc.7b01765}, pages = {9258 -- 9262}, year = {2017}, abstract = {The ortho, meta, and para isomers of 9,10-dipyridylanthracene 1 have been synthesized and converted into their endoperoxides 1-O-2 upon oxidation with singlet oxygen. The kinetics of this reaction can be controlled by the substitution pattern and the solvent: in highly polar solvents, the meta isomer is the most reactive, whereas the ortho isomer is oxidized fastest in nonpolar solvents. Heating of the endoperoxides affords the parent anthracenes by release of singlet oxygen.}, language = {en} } @article{BauchKrtitschkaLinker2017, author = {Bauch, Marcel and Krtitschka, Angela and Linker, Torsten}, title = {Photooxygenation of oxygen-substituted naphthalenes}, series = {Journal of physical organic chemistry}, volume = {30}, journal = {Journal of physical organic chemistry}, publisher = {Wiley}, address = {Hoboken}, issn = {0894-3230}, doi = {10.1002/poc.3734}, pages = {6803 -- 6813}, year = {2017}, abstract = {The reaction of oxygen-substituted naphthalenes with singlet oxygen (O-1(2)) has been investigated, and labile endoperoxides have been isolated and characterized at -78 degrees C for the first time. Low-temperature kinetics by UV spectroscopy revealed that alkoxy and silyloxy substituents remarkably increase the rate of photooxygenations compared to 1,4-dimethylnaphthalene, whereas acyloxy-substituted acenes are inert towards O-1(2). The reactivities nicely correlate with HOMO energies and free activation energies, which we determined by density functional theory calculations. The lability of the isolated endoperoxides is due to their very fast back reaction to the corresponding naphthalenes even at -20 degrees C under release of O-1(2), making them to superior sources of this reactive species under very mild conditions. Finally, a carbohydrate-substituted naphthalene has been synthesized, which reacts reversibly with O-1(2) and might be applied for enantioselective oxidations in future work.}, language = {en} } @misc{IhmelsLinkerTrofimov2017, author = {Ihmels, Heiko and Linker, Torsten and Trofimov, Aleksei}, title = {Editorial}, series = {Journal of physical organic chemistry}, volume = {30}, journal = {Journal of physical organic chemistry}, publisher = {Wiley}, address = {Hoboken}, issn = {0894-3230}, doi = {10.1002/poc.3745}, pages = {1}, year = {2017}, language = {en} } @article{RyabchunSakhnoStumpeetal.2017, author = {Ryabchun, Alexander and Sakhno, Oksana and Stumpe, Joachim and Bobrovsky, Alexey}, title = {Full-Polymer Cholesteric Composites for Transmission and Reflection Holographic Gratings}, series = {Advanced optical materials}, volume = {5}, journal = {Advanced optical materials}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2195-1071}, doi = {10.1002/adom.201700314}, pages = {376 -- 379}, year = {2017}, abstract = {A new type of self-organized materials based on cholesteric networks filled with photoactive side-chain copolymer is being developed. Supramolecular helical structure of cholesteric polymer network resulting in the selective reflection is used as a photonic scaffold. Photochromic azobenzene-containing nematic copolymer is embedded in cholesteric scaffold and utilized as a photoactive media for optical pattering. 1D and 2D transmission diffraction gratings are successfully recorded in composite films by holographic technique. For the first time the possibility to create selective reflection gratings in cholesteric material mimicking the natural optical properties of cholesteric mesophase is demonstrated. That enables the coexistence of two selective gratings, where one has an intrinsic cholesteric periodic helical structure and the other is a holographic grating generated in photochromic polymer. The full-polymer composites provide high light-induced optical anisotropy due to effective photo-orientation of side-chain fragments of the azobenzene-containing liquid crystalline polymer, and prevent the degradation of the helical superstructure maintaining all optical properties of cholesteric mesophase. The proposed class of optical materials could be easily applied to a broad range of polymeric materials with specific functionality. The versatility of the adjustment and material preprogramming combined with high optical performance makes these materials a highly promising candidate for modern optical and photonic applications.}, language = {en} } @article{YangDingKochovskietal.2017, author = {Yang, Guang and Ding, Hong-ming and Kochovski, Zdravko and Hu, Rongting and Lu, Yan and Ma, Yu-qiang and Chen, Guosong and Jiang, Ming}, title = {Highly Ordered Self-Assembly of Native Proteins into 1D, 2D, and 3D Structures Modulated by the Tether Length of Assembly-Inducing Ligands}, series = {Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition}, volume = {56}, journal = {Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1433-7851}, doi = {10.1002/anie.201703052}, pages = {10691 -- 10695}, year = {2017}, abstract = {In nature, proteins self-assemble into various structures with different dimensions. To construct these nanostructures in laboratories, normally proteins with different symmetries are selected. However, most of these approaches are engineering-intensive and highly dependent on the accuracy of the protein design. Herein, we report that a simple native protein LecA assembles into one-dimensional nanoribbons and nanowires, two-dimensional nanosheets, and three-dimensional layered structures controlled mainly by small-molecule assembly-inducing ligands RnG (n = 1, 2, 3, 4, 5) with varying numbers of ethylene oxide repeating units. To understand the formation mechanism of the different morphologies controlled by the small-molecule structure, molecular simulations were performed from microscopic and mesoscopic view, which presented a clear relationship between the molecular structure of the ligands and the assembled patterns. These results introduce an easy strategy to control the assembly structure and dimension, which could shed light on controlled protein assembly.}, language = {en} } @article{GhaisariWinklhoferStrauchetal.2017, author = {Ghaisari, Sara and Winklhofer, Michael and Strauch, Peter and Klumpp, Stefan and Faivre, Damien}, title = {Magnetosome Organization in Magnetotactic Bacteria Unraveled by Ferromagnetic Resonance Spectroscopy}, series = {Biophysical journal}, volume = {113}, journal = {Biophysical journal}, publisher = {Cell Press}, address = {Cambridge}, issn = {0006-3495}, doi = {10.1016/j.bpj.2017.06.031}, pages = {637 -- 644}, year = {2017}, abstract = {Magnetotactic bacteria form assemblies of magnetic nanoparticles called magnetosomes. These magnetosomes are typically arranged in chains, but other forms of assemblies such as clusters can be observed in some species and genetic mutants. As such, the bacteria have developed as a model for the understanding of how organization of particles can influence the magnetic properties. Here, we use ferromagnetic resonance spectroscopy to measure the magnetic anisotropies in different strains of Magnetosprillum gtyphiswaldense MSR-1, a bacterial species that is amendable to genetic mutations. We combine our experimental results with a model describing the spectra. The model includes chain imperfections and misalignments following a Fisher distribution function, in addition to the intrinsic magnetic properties of the magnetosomes. Therefore, by applying the model to analyze the ferromagnetic resonance data, the distribution of orientations in the bulk sample can be retrieved in addition to the average magnetosome arrangement. In this way, we quantitatively characterize the magnetosome arrangement in both wild-type cells and Delta mamJ mutants, which exhibit differing magnetosome organization.}, language = {en} } @article{LangeWagnerZentel2006, author = {Lange, Birger and Wagner, J{\"u}rgen and Zentel, Rudolf}, title = {Fabrication of robust high-quality ORMOCER (R) inverse opals}, series = {Macromolecular rapid communications}, volume = {27}, journal = {Macromolecular rapid communications}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1022-1336}, doi = {10.1002/marc.200600429}, pages = {1746 -- 1751}, year = {2006}, abstract = {The nanostructuring of ORMOCER (R) to form inverse opals is described. For this purpose a polymer opal is used as a template and infiltrated with liquid ORMOCER (R). After photopolymerization of the resin the host opal is dissolved in tetrahydrofuran and an ORMOCER (R) inverse opal is obtained. It shows excellent periodicity (by SEM) and optical properties to reveal a high degree of face centered cubic order. This replication process leads to a nanostructured photonic crystal with the outstanding mechanical properties of ORMOCER (R) and high temperature stability up to 350 degrees C.}, language = {en} } @article{KappBeissenhirtzGeyeretal.2006, author = {Kapp, A. and Beissenhirtz, Moritz Karl and Geyer, F. and Scheller, F. and Viezzoli, Maria Silvia and Lisdat, Fred}, title = {Electrochemical and sensorial behavior of SOD mutants immobilized on gold electrodes in aqueous/organic solvent mixtures}, series = {Electroanalysis : an international journal devoted to fundamental and practical aspects of electroanalysis}, volume = {18}, journal = {Electroanalysis : an international journal devoted to fundamental and practical aspects of electroanalysis}, publisher = {Wiley}, address = {Weinheim}, issn = {1040-0397}, doi = {10.1002/elan.200603620}, pages = {1909 -- 1915}, year = {2006}, abstract = {A cysteine mutant of a monomeric human Cu, Zn-SOD (Glycine 61, Serine 142) has been immobilized directly on gold electrodes using the thiol groups introduced. The electrochemical behavior of the surface confined protein was studied in mixtures of aqueous buffer and DMSO up to an organic solvent content of 60\%. The formal potential was found to be rather independent of the DMSO content. However, half peak width increased and the redoxactive amount clearly decreased with raising DMSO content. In addition, the kinetics of the heterogeneous electron transfer became slower; but still a quasireversible electrochemical conversion of the mutant SOD was feasible. Thus, the electrodes were applied for sensorial superoxide detection. At a potential of +220 mV vs. Ag/AgCl advantage was taken of the partial oxidation reaction of the enzyme. A defined superoxide signal was obtained in solutions up to 40\% DMSO. The sensitivity of the mutant electrodes decreased linearly with the organic solvent content in solution but was still higher compared to conventional cyt.c based sensors. At DMSO concentrations higher than 40\% no sensor response was detected.}, language = {en} } @article{LaiFengHeiletal.2019, author = {Lai, Feili and Feng, Jianrui and Heil, Tobias and Tian, Zhihong and Schmidt, Johannes and Wang, Gui-Chang and Oschatz, Martin}, title = {Partially delocalized charge in Fe-doped NiCo2S4 nanosheet-mesoporous carbon-composites for high-voltage supercapacitors}, series = {Journal of materials chemistry : A, Materials for energy and sustainability}, volume = {7}, journal = {Journal of materials chemistry : A, Materials for energy and sustainability}, number = {33}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2050-7488}, doi = {10.1039/c9ta06250e}, pages = {19342 -- 19347}, year = {2019}, abstract = {Unraveling the effect of transition-metal doping on the energy storage properties of bimetallic sulfides remains a grand challenge. Herein, we construct bimetallic sulfide nanosheets and hence deliberately introduce transition-metal doping domains on their surface. The resulting materials show not only an enhanced density of states near the Fermi level but also partially delocalized charge as shown by density functional theory (DFT) calculations. Fe-doped NiCo2S4 nanosheets wrapped on N,S-doped ordered mesoporous carbon (Fe-NiCo2S4@N,S-CMK-3) are prepared, which show an enhanced specific capacitance of 197.8 F g(-1) in ionic liquid-based supercapacitors at a scan rate of 2 mV s(-1). This is significantly higher as compared to the capacitance of 155.2 and 135.9 F g(-1) of non-iron-doped NiCo2S4@N,S-CMK and Fe-NiCo2S4@CMK-3 electrodes, respectively. This result arises from the enhanced ionic liquid polarization effect and transportation ability from the Fe-NiCo2S4 surface and N,S-CMK-3 structure. Furthermore, the importance of matching multi-dimensional structures and ionic liquid ion sizes in the fabrication of asymmetric supercapacitors (ASCs) is demonstrated. As a result, the ASC device exhibits a high energy density of 107.5 W h kg(-1) at a power density of 100 W kg(-1) in a working-voltage window of 4 V when using Fe-NiCo2S4@N,S-CMK-3 and N,S-CMK-3 as positive and negative electrodes, respectively. This work puts forward a new direction to design supercapacitor composite electrodes for efficient ionic liquid coupling.}, language = {en} }