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Roman Fasel

Publications and source records attributed to Roman Fasel.

9 recordsLinked to original sources

Formation of a regular fullerene nanochain lattice.

A vicinal Au(11 12 12) surface, naturally patterned into a rectangular superlattice, has been used as a template to prepare C60 nanostructures with long-range order and uniform size. At a coverage of 0.1 monolayer and at room temperature, a two-dimensional long-range ordered superlattice of molecular nanochains is achieved, which perfectly replicates the periodicity of the template surface. The fullerene nanochains are found to be located exclusively on the face-centered cubic stacking domains at the lower step edges. Our experiments demonstrate that highly periodic molecular nanochains can be fabricated through a site-selective anchoring method.

Letter↗

Surface chirality of CuO thin films.

We present X-ray photoelectron spectroscopy (XPS) and X-ray photoelectron diffraction (XPD) investigations of CuO thin films electrochemically deposited on an Au(001) single-crystal surface from a solution containing chiral tartaric acid (TA). The presence of enantiopure TA in the deposition process results in a homochiral CuO surface, as revealed by XPD. On the other hand, XPD patterns of films deposited with racemic tartaric acid or the "achiral" meso-tartaric acid are completely symmetric. A detailed analysis of the experimental data using single scattering cluster calculations reveals that the films grown with l(+)-TA exhibit a CuO(1) orientation, whereas growth in the presence of d(-)-TA results in a CuO(11) surface orientation. A simple bulk-truncated model structure with two terminating oxygen layers reproduces the experimental XPD data. Deposition with alternating enantiomers of tartaric acid leads to CuO films of alternating chirality. Enantiospecifity of the chiral CuO surfaces is demonstrated by further deposition of CuO from a solution containing racemic tartaric acid. The pre-deposited homochiral films exhibit selectivity toward the same enantiomeric deposition pathway.

Copper↗

Self-assembly of extended polycyclic aromatic hydrocarbons on Cu111.

We present a low-temperature scanning tunneling microscopy study on the self-assembly of extended polycyclic aromatic hydrocarbons with different symmetries on the Cu111 surface. All molecules show a commensurate monolayer structure, with significant structural differences with respect to the unit cell of the molecular lattice and the orientational ordering. We find that the molecular lattice and the molecular orientation are largely dominated by molecule-substrate interactions, whereas molecule-molecule interactions determine the molecular packing density via steric repulsion. Moreover, we show that the structure of the monolayer is transferred to the second layer via molecule-molecule interaction.

Journal Article↗

Amplification of chirality in two-dimensional enantiomorphous lattices.

The concept of chirality dates back to 1848, when Pasteur manually separated left-handed from right-handed sodium ammonium tartrate crystals. Crystallization is still an important means for separating chiral molecules into their two different mirror-image isomers (enantiomers), yet remains poorly understood. For example, there are no firm rules to predict whether a particular pair of chiral partners will follow the behaviour of the vast majority of chiral molecules and crystallize together as racemic crystals, or as separate enantiomers. A somewhat simpler and more tractable version of this phenomenon is crystallization in two dimensions, such as the formation of surface structures by adsorbed molecules. The relatively simple spatial molecular arrangement of these systems makes it easier to study the effects of specific chiral interactions; moreover, chiral assembly and recognition processes can be observed directly and with molecular resolution using scanning tunnelling microscopy. The enantioseparation of chiral molecules in two dimensions is expected to occur more readily because planar confinement excludes some bulk crystal symmetry elements and enhances chiral interactions; however, many surface structures have been found to be racemic. Here we show that the chiral hydrocarbon heptahelicene on a Cu111 surface does not undergo two-dimensional spontaneous resolution into enantiomers, but still shows enantiomorphism on a mesoscopic length scale that is readily amplified. That is, we observe formation of racemic heptahelicene domains with non-superimposable mirror-like lattice structures, with a small excess of one of the heptahelicene enantiomers suppressing the formation of one domain type. Similar to the induction of homochirality in achiral enantiomorphous monolayers by a chiral modifier, a small enantiomeric excess suffices to ensure that the entire molecular monolayer consists of domains having only one of two possible, non-superimposable, mirror-like lattice structures.

Journal Article↗

Homochiral conglomerates and racemic crystals in two dimensions: tartaric acid on Cu(110).

Two-dimensional lattice structures formed by racemic tartaric acid on a single crystalline Cu(110) surface have been studied and compared with the enantiopure lattices. At low coverage, the doubly deprotonated bitartrate species is separated into two-dimensional conglomerates showing opposite enantiomorphism. At higher coverage, however, a singly deprotonated monotartrate species forms a heterochiral, racemic crystal lattice. While the enantioseparated bitartrate system undergoes decomposition at the same temperature as the enantiopure system, the racemic monotartrate lattice has a lower thermal stability than the enantiopure lattice of identical periodicity and surface density. At monolayer saturation coverage, the pure enantiomers form a denser lattice than the racemate. This is in contrast to the three-dimensional tartaric acid crystals, where the racemate crystallizes in a lattice of higher density, which is also more thermally stable than the enantiopure tartaric acid crystals.

Journal Article↗

Chiral recognition in surface explosion.

The vast majority of chiral compounds crystallize into racemic crystals. It has been predicted and was experimentally established as a rule that chiral molecules on surfaces are more easily separated into homochiral domains due to confinement into a plane and lower entropic contributions. We investigated the formation and stability of two-dimensional tartrate crystals on a Cu(110) surface for the racemic mixture for the first time by means of temperature-programmed desorption (TPD), low-energy electron diffraction (LEED), and X-ray photoelectron spectroscopy (XPS). At low coverage, a bitartrate species becomes separated into homochiral domains, while at high coverage a monotartrate species forms a racemic mixture. At the same coverage and lateral arrangement, the thermally induced autocatalytic decomposition reaction occurs for the monotartrate racemate at a lower temperature than for the pure enantiomers. The stereochemistry in this so-called "surface explosion" reaction is explained by a higher stability of the enantiopure lattice due to lateral hydrogen-bond formation. The higher stability of the enantiopure two-dimensional lattice is in contrast to the higher stability of racemic three-dimensional tartaric acid crystals but is consistent with the observation that homochirality is preferred in hydrogen-bonded self-assembled biomolecular structures.

Journal Article↗

Temperature dependence of electron-to-lattice energy transfer in single-wall carbon nanotube bundles.

The electron-phonon coupling strength in single-wall carbon nanotube (SWNT) bundles has been studied directly in the time domain by femtosecond time-resolved photoelectron spectroscopy. We have measured the dependence of H(Te, Tl), the rate of energy transfer between the electronic system and the lattice as a function of electron and lattice temperatures Te and Tl. The experiments are consistent with a T5 dependence of H on the electron and lattice temperatures, respectively. The results can be related to the e-ph mass enhancement parameter lambda. The experimentally obtained value of for lambda/[symbol: see text] D2, where [symbol: see text] D is the Debye temperature, suggests that e-ph scattering times at the Fermi level of SWNT bundles can be exceptionally long, exceeding 1.5 ps at room temperature.

Computer Simulation↗