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Jester SS Idelson A Schmitz D Eberhagen F Höger S 《Langmuir : the ACS journal of surfaces and colloids》2011,27(13):8205-8215
Shape-persistent rigid phenylene-ethynylene-butadiynylenes form lamellar self-assembled monolayers (SAMs) at the HOPG/TCB interface, which were studied by scanning tunneling microscopy (STM) with submolecular resolution. Substitution of the terminating acetylene functions with polar cyanopropyldimethylsilyl groups leads to 2D phase separation and defined rod-rod interactions, which determine the packing distances between the rigid rods. The results stimulated the connection of rigid rods via septiarylene clamp units. They covalently link two rigid rod units and define the intramolecular rod-rod distance that matches the alkoxy substituent chain lengths. The systems can be described as half-ring structures of two rigid rods connected via a rotatable joint unit. These acetylene-terminated half-ring structures were also oligomerized under Cu and Pd catalysis to yield defined acyclic and cyclic oligomers. Detailed STM studies decoded the molecular origin of the surface patterning of such systems. The dodecyloxy side chains are adsorbed along the HOPG main axes and, together with the alkoxy backbone angle, determine the adsorption direction of the adlayers. 相似文献
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Tristan J. Keller Christopher Sterzenbach Joshua Bahr Taria L. Schneiders Markus Bursch Julia Kohn Theresa Eder John M. Lupton Stefan Grimme Sigurd Hger Stefan-S. Jester 《Chemical science》2021,12(27):9352
Molecular spoked wheels with D3h and Cs symmetry are synthesized by Vollhardt trimerization of C2v-symmetric dumbbell structures with central acetylene units and subsequent intramolecular ring closure. Scanning tunneling microscopy of the D3h-symmetric species at the solid/liquid interface on graphite reveals triporous chiral honeycomb nanopatterns in which the alkoxy side chains dominate the packing over the carboxylic acid groups, which remain unpaired. In contrast, Cs-symmetric isomers partially allow for pairing of the carboxylic acids, which therefore act as a probe for the reduced alkoxy chain nanopattern stabilization. This observation also reflects the adsorbate substrate symmetry mismatch, which leads to an increase of nanopattern complexity and unexpected templating of alkoxy side chains along the graphite armchair directions. State-of-the-art GFN-FF calculations confirm the overall structure of this packing and attribute the unusual side-chain orientation to a steric constraint in a confined environment. These calculations go far beyond conventional simple space-filling models and are therefore particularly suitable for this special case of molecular packing.Scanning tunneling microscopy investigations of phenylene-based molecular spoked wheels with D3h and Cs symmetries on graphite show the competitive or complementary effects of carboxylic acid groups and alkoxy chains on the nanopattern formation. 相似文献
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Dr. Stefan K. Maier Georgiy Poluektov Dr. Stefan‐S. Jester Prof. Dr. Heiko M. Möller Prof. Dr. Sigurd Höger 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(4):1379-1384
Macrocycles with quaterthiophene subunits were obtained by cyclooligomerization by direct oxidative coupling of unsubstituted dithiophene moieties. The rings were closed with high selectivity by an α,β′‐connection of the thiophenes as proven by NMR spectroscopy. The reaction of the precursor with terthiophene moieties yielded the symmetric α,α′‐linked macrocycle in low yield together with various differently connected isomers. Blocking of the β‐position of the half‐rings yielded selectively the α,α′‐linked macrocycle. Selected cyclothiophenes were investigated by scanning tunneling microscopy, which displayed the formation of highly ordered 2D crystalline monolayers. 相似文献
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Novel semiconducting materials have been prepared under ultrahigh-vacuum conditions by soft-landing mass-selected Cn+ (50< or =n<60; even n) on highly oriented pyrolytic graphite surfaces at mean kinetic energies of 6 eV. In all cases, Cn films grow according to the Volmer-Weber mechanism: the surface is initially decorated by two-dimensional fractal islands, which in later deposition stages become three-dimensional dendritic mounds. We infer that Cn aggregation is governed by reactive sites comprising adjacent pentagons (or heptagons) on individual cages. The resulting covalent cage-cage bonds are responsible for the unusually high thermal stability of the films compared to solid C60. The apparent activation energies for intact Cn sublimation range from 2.2 eV for C58 to 2.6 eV for C50 as derived from thermal desorption spectra. All Cn films exhibit a common valence-band ultraviolet photoelectron spectroscopy spectral feature located around the center of a broad highest occupied molecular-orbital (HOMO)-derived band (EB approximately 2.5 eV). This feature has been assigned to Cn units covalently linked to each other in polymeric structures. To within experimental accuracy, the same work function (4.8 eV) was determined for thick films of all Cn studied. In contrast, "HOMO" ionization potentials were cage size dependent and significantly lower than that obtained for C60. C58 exhibited the lowest HOMO (6.5 eV). Band gaps of Cn films have been determined by depositing small amounts of Cs atoms onto the topmost film layer. HOMO-lowest unoccupied molecular-orbital-derived band gaps between 0.8 eV (C52) and 1.8 eV (C50) were observed, compared to 1.5 eV for solid C60. 相似文献
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K. K. S. Pillay D. C. Driscoll W. A. Jester 《Journal of Radioanalytical and Nuclear Chemistry》1975,27(2):421-438
A systematic investigation using a variety of handguns has revealed the existence of distinguishable distribution patterns of firearm discharge residues on surfaces below the flight path of a bullet. The residues are identifiable even at distances of 12 meters from the gun using nondestructive neutron activation analysis. The results of these investigations show that the distribution pattern for a gun is reproducible using similar ammunition and that there exist two distinct regions to the patterns developed between the firearm and the target—one with respect to the position of the gun and the other in the vicinity of the target. The judicious applications of these findings could be of significant value in criminal investigations. 相似文献
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W. A. Jester T. Daubenspeck S. Pandey X. Xu 《Journal of Radioanalytical and Nuclear Chemistry》2000,244(2):453-456
Personnel from the Pennsylvania State University's Breazeale Nuclear Reactor assisted NRC (Nuclear Research Corporation) personnel in calibrating a new MSL/16N Nitrogen-16 Monitor. This paper describes the neutron flux calibration procedures utilized and the results obtained for the production of a nitrogen-16 source of known activity for a BGO detector calibration. 相似文献
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SS Jester E Sigmund LM Röck S Höger 《Angewandte Chemie (International ed. in English)》2012,51(34):8555-8559
Seeing stars: The two-dimensional patterns of the polycyclic heteroaromatic star molecules 1 on graphite vary with the side chain length. For n=12, frustrated self-assembly leads to hierarchically organized superstructures: up to 10?molecules form triangular aggregates which pack densely into hexagonal patterns with very large (15.5?nm) lattice constants. 相似文献
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Tong Gao Jester Itliong Sai Prashanth Kumar Zackerie Hjorth Issei Nakamura 《Journal of polymer science. Part A, Polymer chemistry》2021,59(21):2434-2457
Ionic liquid (IL)-containing polymers garner attention for electrochemical applications. This article overviews recent experimental and theoretical studies of polymer electrolytes that would be likely to cultivate new theoretical and computational frameworks for IL-containing polymers. The first two sections outline the uniqueness of ILs that differentiates them from inorganic salts in polymers and explore deviation from the concept of the metaphor “room-temperature molten salt.” Such distinct properties include (1) large intrinsic dipole moment and electronic polarizability, (2) hydrogen bonding, (3) π-interactions, (4) a broad distribution of charges over the entire ion, and (5) the anisotropy of the ions. Moreover, the complexity of these properties substantially increases when the ions are polymerized. Indeed, their exceptional features would overcome the hurdle due to a trade-off between ionic conductivity and mechanical robustness in inorganic salt-doped polymers. Given these facts, the rest of the article focuses on emerging trends in the study of the dielectric response, phase separation, ion conductivity, and mechanical robustness of the polymer electrolytes, highlighting outstanding observations in experiments that may inspire existing theory and simulation. Our discussion also includes improving computational complexity for IL-containing polymers. To this end, recent machine learning studies that consider ILs and polymer liquids are presented. 相似文献