A kinetic Monte Carlo study of desorption of H2 from graphite (0001)

The formation of H2 in the interstellar medium proceeds on the surfaces of silicate or carbonaceous particles. To get a deeper insight of its formation on the latter substrate, this letter focuses on H2 desorption from graphite (0001) in Temperature-Programmed-Desorption Monte-Carlo simulations. The results are compared to experimental results which show two main peaks and an intermediate shoulder for high initial coverage. The simulation program includes barriers obtained by ab-initio methods and is further optimised to match two independent experimental observations. The simulations reproduce the two experimental observed desorption peaks. Additionally, a possible origin of the intermediate peak is given.Comment: 9 pages, 5 figures, Chem. Phys. Lett. in pres

Adsorption and STM imaging of polycyclic aromatic hydrocarbons on graphene

International audienceThe structural characterization of polycyclic aromatic hydrocarbon molecules adsorbed on graphene is of fundamental importance in view of the use of graphene or graphene nanoribbons for electronic applications. Before reaching this point, one has to determine the structure of the adsorbed molecules. Here, we study the case of benzene, coronene, and hexabenzocoronene on a graphene layer. First, the adsorption properties of single molecules are calculated using first-principles calculations at the level of density functional theory. We benefit from a recent scheme, particularly adapted for weakly adsorbed molecules, allowing us to precisely calculate the van der Waals contribution. Then, scanning tunneling microscopy (STM) is used to produce images of self-assembled molecules comparing different theoretical approaches to experimental observations. Finally, we consider the imaging of isolated molecules, and we show how the STM tip influences the molecule position by soft mechanical interaction during the scanning process

Mobility of D atoms on porous amorphous water ice surfaces under interstellar conditions

Aims. The mobility of H atoms on the surface of interstellar dust grains at low temperature is still a matter of debate. In dense clouds, the hydrogenation of adsorbed species (i.e., CO), as well as the subsequent deuteration of the accreted molecules depend on the mobility of H atoms on water ice. Astrochemical models widely assume that H atoms are mobile on the surface of dust grains even if controversy still exists. We present here direct experimental evidence of the mobility of H atoms on porous water ice surfaces at 10 K. Methods. In a UHV chamber, O2 is deposited on a porous amorphous water ice substrate. Then D atoms are deposited onto the surface held at 10 K. Temperature-Programmed Desorption (TPD) is used and desorptions of O2 and D2 are simultaneously monitored. Results. We find that the amount of O2 that desorb during the TPD diminishes if we increase the deposition time of D atoms. O2 is thus destroyed by D atoms even though these molecules have previously diffused inside the pores of thick water ice. Our results can be easily interpreted if D is mobile at 10 K on the water ice surface. A simple rate equation model fits our experimental data and best fit curves were obtained for a D atoms diffusion barrier of 22(+-)2 meV. Therefore hydrogenation can take place efficiently on interstellar dust grains. These experimental results are in line with most calculations and validate the hypothesis used in several models.Comment: 4 pages (Submitted to A&A

Spatially-resolved potential measurement with ion crystals

We present a method to measure potentials over an extended region using one-dimensional ion crystals in a radio frequency (RF) ion trap. The equilibrium spacings of the ions within the crystal allow the determination of the external forces acting at each point. From this the overall potential, and also potentials due to specific trap features, are calculated. The method can be used to probe potentials near proximal objects in real time, and can be generalized to higher dimensions.Comment: 7 pages (double spaced), 3 figure

Ab initio simulations of the kinetic properties of the hydrogen monomer on graphene

The understanding of the kinetic properties of hydrogen (isotopes) adatoms on graphene is important in many fields. The kinetic properties of hydrogen-isotope (H, D and T) monomers were simulated using a composite method consisting of density functional theory, density functional perturbation theory and harmonic transition state theory. The kinetic changes of the magnetic property and the aromatic $\pi$ bond of the hydrogenated graphene during the desorption and diffusion of the hydrogen monomer was discussed. The vibrational zero-point energy corrections in the activation energies were found to be significant, ranging from 0.072 to 0.205 eV. The results obtained from quantum-mechanically modified harmonic transition state theory were compared with the ones obtained from classical-limit harmonic transition state theory over a wide temperature range. The phonon spectra of hydrogenated graphene were used to closely explain the (reversed) isotope effects in the prefactor, activation energy and jump frequency of the hydrogen monomer. The kinetic properties of the hydrogen-isotope monomers were simulated under conditions of annealing for 10 minutes and of heating at a constant rate (1.0 K/s). The isotope effect was observed; that is, a hydrogen monomer of lower mass is desorbed and diffuses more easily (with lower activation energies). The results presented herein are very similar to other reported experimental observations. This study of the kinetic properties of the hydrogen monomer and many other involved implicit mechanisms provides a better understanding of the interaction between hydrogen and graphene.Comment: Accepted by J. Phys. Chem.

All-Optical Broadband Excitation of the Motional State of Trapped Ions

We have developed a novel all-optical broadband scheme for exciting, amplifying and measuring the secular motion of ions in a radio frequency trap. Oscillation induced by optical excitation has been coherently amplified to precisely control and measure the ion's secular motion. Requiring only laser line-of-sight, we have shown that the ion's oscillation amplitude can be precisely controlled. Our excitation scheme can generate coherent motion which is robust against variations in the secular frequency. Therefore, our scheme is ideal to excite the desired level of oscillatory motion under conditions where the secular frequency is evolving in time. Measuring the oscillation amplitude through Doppler velocimetry, we have characterized the experimental parameters and compared them with a molecular dynamics simulation which provides a complete description of the system.Comment: 8 pages, 10 figure

Molecular Dynamics Simulation of Sympathetic Crystallization of Molecular Ions

It is shown that the translational degrees of freedom of a large variety of molecules, from light diatomic to heavy organic ones, can be cooled sympathetically and brought to rest (crystallized) in a linear Paul trap. The method relies on endowing the molecules with an appropriate positive charge, storage in a linear radiofrequency trap, and sympathetic cooling. Two well--known atomic coolant species, ${}^9{\hbox{Be}}^+$ and ${}^{137}{\hbox{Ba}}^+$, are sufficient for cooling the molecular mass range from 2 to 20,000 amu. The large molecular charge required for simultaneous trapping of heavy molecules and of the coolant ions can easily be produced using electrospray ionization. Crystallized molecular ions offer vast opportunities for novel studies.Comment: Accepted for publication in Phys. Rev.

Quantum Computing with Trapped Ion Hyperfine Qubits

We discuss the basic aspects of quantum information processing with trapped ions, including the principles of ion trapping, preparation and detection of hyperfine qubits, single-qubit operations and multi-qubit entanglement protocols. Recent experimental advances and future research directions are outlined.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/45527/1/11128_2004_Article_489417.pd