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Iski EV Tierney HL Jewell AD Sykes EC 《Chemistry (Weinheim an der Bergstrasse, Germany)》2011,17(26):7205-7212
The hierarchical transfer of chirality in nature, from the nano‐, to meso‐, to macroscopic length scales, is very complex, and as of yet, not well understood. The advent of scanning probes has allowed chirality to be monitored at the single molecule or monolayer level and has opened up the possibility to track enantiospecific interactions and chiral self‐assembly with molecular‐scale detail. This paper describes the self‐assembly of a simple, model molecule (naphtho[2,3‐a]pyrene) that is achiral in the gas phase, but becomes chiral when adsorbed on a surface. This polyaromatic hydrocarbon forms a stable and reversibly ordered system on Cu(111) in which the transmission of chirality from single surface‐bound molecules to complex 2D chiral architectures can be monitored as a function of molecular packing density and surface temperature. In addition to the point chirality of the surface‐bound molecule, the unit cell of the molecular domains was also found to be chiral due to the incommensurate alignment of the molecular rows with respect to the underlying metal lattice. These molecular domains always aggregated in groups of three, all of the same chirality, but with different rotational orientations, forming homochiral “tri‐lobe” ensembles. At a larger length scale, these tri‐lobe ensembles associated with nearest‐neighbor tri‐lobe units of opposite chirality at lower packing densities before forming an extended array of homochiral tri‐lobe ensembles at higher converges. This system displayed chirality at a variety of size scales from the molecular (≈1 nm) and domain (≈5 nm) to the tri‐lobe ensemble (≈10 nm) and extended array (>25 nm) levels. The chirality of the tri‐lobe ensembles dictated how the overall surface packing occurred and both homo‐ and heterochiral arrays could be reproducibly and reversibly formed and interchanged as a function of surface coverage. Finally, these chirally templated surfaces displayed remarkable enantiospecificity for naphtho[2,3‐a]pyrene molecules adsorbed in the second layer. Given its simplicity, reversibility, and rich degree of order, this system represents an ideal test bed for the investigation of symmetry breaking and the hierarchical transmission of chirality through multiple length scales. 相似文献
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Iski EV Johnston BF Florence AJ Sykes EC Urquhart AJ 《Chemical communications (Cambridge, England)》2011,47(34):9627-9629
High-resolution STM imaging of the structures formed by carbamazepine molecules adsorbed onto a pseudo-ordered carbamazepine monolayer on Au(111) shows the formation of previously unreported 1-dimensional supramolecular assemblies. 相似文献
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Subham Majumdar EV Sampathkumaran St Berger M Della Mea H Michor E Bauer M Brando J Hemberger A Loidl 《Pramana》2002,58(5-6):777-782
Recently, the solid solution Ce2Au1−
x
Co
xSi3 has been shown to exhibit many magnetic anomalies associated with the competition between magnetic ordering and the Kondo
effect. Here we report high pressure electrical resistivity of Ce2AuSi3, ac susceptibility (X) and magnetoresistance of various alloys of this solid solution in order to gain better knowledge of the magnetism of these
alloys. High pressure resistivity behavior is consistent with the proposal that Ce2AuSi3 lies at the left-hand side of the maximum in Doniach’s magnetic phase diagram. The ac X data reveal that there are in fact two magnetic transitions, one at 2 K and the other at 3 K for this compound, both of which
are spin-glass-like. However, as the Co concentration is increased, antiferromagnetism is stabilized for intermediate compositions
before attaining non-magnetism for the Co end member. 相似文献
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Erin V. Iski April D. Jewell Heather L. Tierney Georgios Kyriakou E. Charles H. Sykes 《Surface science》2012,606(3-4):536-541
Organic thin films composed of naphtho[2,3-a]pyrene, a very promising multifunctional polyaromatic hydrocarbon for use in optoelectronic devices, are demonstrated to restructure the pristine Au(111) 22 × √3 surface. The perturbation of the herringbone reconstruction was used to gauge the interaction strength of the organic molecule with the substrate through a series of controlled adsorption and annealing treatments. The overall behavior of the system is interpreted as an interplay between thermodynamic and kinetic factors, dictated by the temperature of the sample and the surface coverage of the molecules. The restructuring mechanism involves the exchange of Au atoms from the herringbone reconstruction to the step edges. Our results reveal that the molecular and substrate equilibrium structure is only achieved after annealing the system to > 470 K. This infers that caution should be taken when organic–metal interfaces are constructed by low or room temperature deposition, as they may not correspond to the equilibrium structures, and therefore, may misrepresent the adlayer structure which exists at the realistic working conditions of devices. 相似文献
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We have grown single crystals of the psuedo-one-dimensional compound Sr3CuIrO6, a K4CdCl6-derived monoclinic structure with Cu-Ir chains along the [101] direction. We present the ac and dc magnetization behavior
of the single crystals in comparison with that of the polycrystalline form reported earlier. There is a distinct evidence
for at least two magnetic transitions, at 5 K (T
1) and 19 K (T
2), with different relative magnitudes in the single and polycrystals. The low temperature magnetic relaxation behavior of
both the forms is found to be widely different, exhibiting unexpected time dependence. 相似文献
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Baber AE Jensen SC Iski EV Sykes EC 《Journal of the American Chemical Society》2006,128(48):15384-15385
We describe how the presence of styrene, a weakly adsorbed molecule, dramatically restructures the Au{111} surface at temperatures as low as 80 K. The restructuring manifests itself both in mobility of step-edge atoms, as well as changes in the position of the herringbone reconstruction over time. These effects are explained in terms of the preferential adsorption sites of styrene allowing it to assist in atom detachment from step edges, as well as lowering of the energetic barrier for movement of the herringbone reconstruction. This work has important consequences for studies in which Au is used as a support for or as an electrical contact to molecules. 相似文献
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