Atomism | EPFL Graph Search

Atomism (from Greek ἄτομον, atomon, i.e. "uncuttable, indivisible") is a natural philosophy proposing that the physical universe is composed of fundamental indivisible components known as atoms. References to the concept of atomism and its atoms appeared in both ancient Greek and ancient Indian philosophical traditions. Leucippus is the earliest figure whose commitment to atomism is well attested and he is usually credited with inventing atomism. He and other ancient Greek atomists theorized that nature consists of two fundamental principles: atom and void. Clusters of different shapes, arrangements, and positions give rise to the various macroscopic substances in the world. The particles of chemical matter for which chemists and other natural philosophers of the early 19th century found experimental evidence were thought to be indivisible, and therefore were given by John Dalton the name "atom", long used by the atomist philosophy. Although the connection to histor

Etude par STM de la déposition d'agrégats d'or sur TiO2 et mesure de l'émission électronique secondaire induite par l'impact d'agrégats sur une surface

Pierre Convers

This thesis work focuses on impact and diffusion processes as well as equilibrium positions of a metal deposited on a surface. The metal is deposited in the form of clusters containing n atoms in a controlled way. Gold or silver clusters cations (Au+n and Ag+n ) are used. Their size (n ∈ [1, 9]), charge state and deposition energy (E = 10 - 4500 eV) are well defined. The surface being at room temperature during the deposition, can be annealed and transferred in a scanning tunnelling microscope (STM) after deposition. The variable temperature microscope was developed during this thesis. The approach of the tip is carried out by an axial motor, which renders the microscope very stable. The first part of this work treats of the evolution of gold deposited on a TiO2(110) surface. Position and size of gold islands created by cluster or atomic depositions are determined by STM. Compared to atomic deposition at the same energy (10 < E < 100 eV), the cluster deposition produces smaller islands with a large islands density after annealing at 800 K. Regardless the deposition conditions, gold atoms diffuse on the surface already at 300 K. The impact energy is the key parameter to reduce the diffusion by cluster or atomic implantation or defect creation. Upon a high energy deposition, part of the deposited gold is invisible to the STM. The fate of these gold atoms is unclear : they are either buried under the surface or ejected in vacuum at the impact. The control of the islands size should permit the creation of a stable system with an optimum catalytic activity (i. e. CO combustion). Research groups have shown that this activity is strongly influenced by the islands size. It is equal to zero if the diameter is greater than 5 nm. The second part of this work is devoted to the electron emission γ induced by the impact of silver clusters Ag+n on a Pt and HOPG surface. Measurements are made by varying the impact energy (and so the speed v) of size-selected clusters on a defined surface. Impact velocity ranges from 104 to 105 m/s, which is lower than the classical threshold. Nevertheless every cluster size produces an electron emission. A potential emission (γ(v=0) ≠ 0) is observed for the monomer on both surfaces, which is caused by excited ions in a metastable state. The γ(v) curves are increasing, and no mesurable oscillation are observed. This does not confirm earlier work by Meiwes-Broer et al. These authors found oscillations in γ on similar systems relating them to the electronic structure of the clusters and the surface. A model based on heating of the electron gas is developed. This model gives good agreements with the γ(v) curves. The electronic temperature is estimated to 3000-8000 K. Similar behavior on both surfaces (Pt and HOPG) depending of the cluster size is shown. This behavior is probably related to the geometrical structure of the clusters. Finally, a more pronounced molecular effect is observed for the HOPG : the number of electrons emitted by the impact of a Ag+n is up to 7 times higher than the number of electrons emitted by impacts of n independent atoms. This value is smaller than 2 for the Pt surface.

EPFL2005

An Experimental Setup for Heterogeneous Catalysis on Atomically Defined Metal Nanostructures

Jean-Guillaume De Groot

The main objective of this PhD thesis is to link the atomic scale structure to the catalytic properties of self-assembled nanostructures. The growth and characterization of these nanostructures was carried out in an ultra-high vacuum (UHV) chamber initially designed for the study of the kinetics of epitaxial growth of thin films and nanostructures by variable temperature scanning tunneling microscopy. During this PhD thesis, we built a very sensitive and selective gas detector based on a quadrupole mass spectrometer and adapted to the geometry of this UHV system. The proper functioning of the gas detector is confirmed by temperature programmed desorptions of Xe on Ag(100) which demonstrate the very high sensitivity of the device of about

10^{-6}

~monolayer (ML). The zero-order desorption parameters obtained for the first monolayer of Xe adsorbed on Ag(100) are

E_d=0.22-0.23

~eV with a prefactor

\nu_0

between

4\times10^{12}

^{-1}

and

1 \times10^{13}

^{-1}

. An exchange process between Fe adatoms and Ag atoms from the Ag(100) surface is identified by means of temperature programmed desorption of N

_2

. Desorption spectra suggest that the exchange is complete from an annealing temperature of 140~K. Our study of the catalytic activity of metal nanostructures focuses on the ability of passivated Fe clusters to adsorb N

_2

molecules without dissociating them, which is a fundamental step in the bio-inspired heterogeneous catalysis of ammonia. The first system investigated for the growth of Fe clusters is MgO/Ag(100). Diffusion of Fe adatoms deposited on a MgO monolayer is observed from an annealing temperature of 280~K onwards. Fe clusters with an average size of

12.1\pm 0.5

~atoms are obtained on a MgO monolayer by thermal ripening of 0.072~ML of Fe deposited at 40~K. No sign of N

_2

adsorption was observed on these clusters by thermal programmed desorption investigation. The second system chosen for the growth of Fe clusters is graphene/Ir(111) obtained by chemical vapor deposition. The deposition of 0.3 and 0.4 ML of Fe on a graphene/Ir(111) sample at 50~K, followed by annealing at 300~K, generates a superlattice of Fe clusters which matches the periodicity of the moiré formed by graphene/Ir(111). The theoretically expected mean cluster size is 26 atoms for 0.3~ML of Fe, and 35 atoms for 0.4~ML of Fe. The temperature stability of the clusters obtained with 0.4~ML Fe is investigated from 300~K to 600~K. It is established that Smoluchowski ripening takes place as the annealing temperature increases and the superlattice structure has completely disappeared after annealing at 600~K. Temperature programmed desorption of molecularly adsorbed N

_2

at 50~K on a sample with 0.4~ML of Fe deposited on graphene/Ir(111) reveals 3 desorption peaks at 120~K, 92~K, and 60~K. In addition, slow dissociation of nitrogen molecules at 50~K adsorbed on the higher energy adsorption sites is demonstrated.

EPFL2021

Monte Carlo Modeling of Crystal Channeling at High Energies

Philippe Jean Schoofs

Charged particles entering a crystal close to some preferred direction can be trapped in the electromagnetic potential well existing between consecutive planes or strings of atoms. This channeling effect can be used to extract beam particles if the crystal is bent beforehand. Crystal channeling is becoming a reliable and efficient technique for collimating beams and removing halo particles. At the European Organization for Nuclear Research (CERN), the installation of silicon crystals in the Large Hadron Collider (LHC) is under scrutiny by the UA9 collaboration with the goal of investigating if they are a viable option for the collimation system upgrade. This thesis describes a new Monte Carlo model of planar channeling which has been developed from scratch in order to be implemented in the FLUKA code simulating particle transport and interactions. Crystal channels are described through the concept of continuous potential taking into account thermal motion of the lattice atoms and using Moliere screening function. The energy of the particle transverse motion determines whether or not it is trapped between the crystal planes while single Coulomb scattering on lattice atoms can lead to dechanneling. The volume capture and reflection applying to quasi-channeled particles are also modeled. Analogously to dechanneling, single scattering is used to determine the occurrence of volume capture. The parameters of the crystals, such as torsion or miscut, are described as well. For channeled particles, the suppression of electromagnetic and nuclear collisions is implemented. It is stronger for particles oscillating close to the center of the channel and is crucial for a correct evaluation of the rate of dechanneling without having recourse to the use of a macroscopic dechanneling length. The UA9-H8 experiment conducted at CERN aims at investigating new crystal physics as well as characterizing crystals that can be of interest in view of the implementation of crystal collimation at CERN, including in the LHC. This experiment uses silicon strip detectors situated on both sides of the crystal. Putting together upstream and downstream tracks in coincidence and matching at an identical fitted location on the crystal, it yields information about the deflections given to the beam population. Several runs from the UA9-H8 experiment are analyzed and compared to the model results. Channeling and dechanneling rates, as well as angular distributions at crystal exit are shown to be in a very encouraging agreement both for strip and quasi-mosaic crystals.

EPFL2014