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Inelastic Electron Tunneling Spectroscopy (IETS) with the Scanning Tunneling Microscope (STM) is a novel vibrational spectroscopy technique that permits to characterize very subtle properties of molecules adsorbed on metallic surfaces. Its proposed symmetry-based propensity selection rules, however, fail to fully capture its exact mechanism and influencing factors; are not directly retraceable to an adsorbate property and are cumbersome. In this thesis, a theoretical approach was taken to improve them. An IETS simulation protocol has been developed, parameterized and benchmarked, and consequently used to calculate IETS spectra for a set of systematically related small molecules on copper surfaces. Extending IETS principles were deduced that refer to the tunneling state's vacuum extension, the selective activating/quenching of certain types of modes due to the moieties' electronic properties, and the applicability of a sum rule of IETS signals. Also, fingerprinting IETS-signals that enable discrimination between adsorbate orientations, the chemical nature of atoms and structural isomers were determined and a strategy using straightforward electronic density distribution properties of the isolated molecule to predict IETS activity without (large) computational cost was developed. This expertise was used to rationalize and interpret experimentally measured IETS spectra for adsorbed metalloporphyrins and metallophthalocyanines, being the first IETS studies of this large size. This experimental approach permitted to determine the current limitations of IETS-simulations. The associated identification shortcomings were resolved by conducting complementary STM-image simulations.
Electron tunnelling spectroscopy as a research tool has strongly advanced understanding of superconductivity. This book explains the physics and instrumentation behind the advances illustrated in beautiful images of atoms, rings of atoms and exotic states in high temperature superconductors, and summarizes the state of knowledge that has resulted.
This work describes the experimental study of electron-boson interactions in superconductors by means of inelastic electron tunneling spectroscopy performed with a scanning tunneling microscope (STM) at temperatures below 1 K. This new approach allows the direct measurement of the Eliashberg function of conventional superconductors as demonstrated on lead (Pb) and niobium (Nb). Preparative experiments on unconventional iron-pnictides are presented in the end.
Inelastic Electron Tunneling Spectroscop~ or lETS, provides a unique technique for electronically monitoring the vibrational modes of molecul (;5 adsorbed on a metal oxide surface. Since the discovery of the phenomena by JAKLEVIC and LM1BE in 1966, lETS has been developed by a number of scientists as a method for studying the surface chemistry of molecular species adsorbed on aluminum oxide. Recent applications of lETS include investigations of physical and chemical adsorption of hydrocarbons, studies of catalysis by metal particles, detection and identification of trace substances in air and water, and studies of biological molecules and electron damage to such molecules. lETS has been employed to investigate adhesive materials, and studies are currently in prog ress to investigate corrosion species and corrosion inhibitors on aluminum and its alloys. Electronic transitions of molecules have also been studied by lETS. The recent development of the "external doping" technique, whereby molecu lar species can be introduced into fabricated tunnel junctions, opens the door for a vast new array of surface chemical studies by lETS. lETS is rap idly becoming an important tool for the study of surface and interface phe nomena. In addition to its role in surface studies, inelastic tunneling has proved extremely valuable for the study of the electronic properties of thin metallic films, and the recent discovery of light emission from inelastic tunneling promises to be of some importance in the area of device physics.
This work describes the experimental study of electron-boson interactions in superconductors by means of inelastic electron tunneling spectroscopy performed with a scanning tunneling microscope (STM) at temperatures below 1 K. This new approach allows the direct measurement of the Eliashberg function of conventional superconductors as demonstrated on lead (Pb) and niobium (Nb). Preparative experiments on unconventional iron-pnictides are presented in the end. This work was published by Saint Philip Street Press pursuant to a Creative Commons license permitting commercial use. All rights not granted by the work's license are retained by the author or authors.
Scanning tunneling microscopy has achieved remarkable progress and become the key technology for surface science. This book predicts the future development for all of scanning probe microscopy (SPM). Such forecasts may help to determine the course ultimately taken and may accelerate research and development on nanotechnology and nanoscience, as well as all in SPM-related fields in the future.
The power of rotational spectroscopy has long been demonstrated in the frequency domain by microwave spectroscopy, but its application in real space has been limited. Using a scanning tunneling microscope (STM) and inelastic electron tunneling spectroscopy (IETS), we were able to conduct real-space measurements of rotational transitions of gaseous hydrogen molecules physisorbed on surfaces at 10 K. The j=0 to j=2 rotational transition for para-H 2 and HD were observed by STM-IETS. It is also found that the rotational energy is very sensitive to its local environment, we could precisely investigate how the environmental coupling modifies the structure, including the bond length, of a single molecule with sub-Angstrom resolution. Due to this high sensitivity, the spatial variation in the potential energy surface can be quantified by the rotational and vibrational energies of the trapped H 2. The ability of the tip to drag along a hydrogen molecule as it scans over another adsorbed molecule combined with the sensitivity of the hydrogen rotational excitation recorded by IETS to its immediate environment lead to the implementation of rotational spectromicroscopy. Hydrogen rotational spectroscopy and microscopy provides novels approach toward visualizing and quantifying the intermolecular interaction as well as the intermediate processes of chemical reactions.
Work with individual atoms and molecules aims to demonstrate that miniaturized electronic, optical, magnetic, and mechanical devices can operate ultimately even at the level of a single atom or molecule. As such, atomic and molecular manipulation has played an emblematic role in the development of the field of nanoscience. New methods based on the use of the scanning tunnelling microscope (STM) have been developed to characterize and manipulate all the degrees of freedom of individual atoms and molecules with an unprecedented precision. In the meantime, new concepts have emerged to design molecules and substrates having specific optical, mechanical and electronic functions, thus opening the way to the fabrication of real nano-machines. Manipulation of individual atoms and molecules has also opened up completely new areas of research and knowledge, raising fundamental questions of "Optics at the atomic scale", "Mechanics at the atomic scale", Electronics at the atomic scale", "Quantum physics at the atomic scale", and "Chemistry at the atomic scale". This book aims to illustrate the main aspects of this ongoing scientific adventure and to anticipate the major challenges for the future in "Atomic and molecular manipulation" from fundamental knowledge to the fabrication of atomic-scale devices. Provides a broad overview of the field to aid those new and entering into this research area Presents a review of the historical development and evolution of the field Offers a clear personalized view of current scanning probe microscopy research from world experts