The origin of high-resolution IETS-STM images of organic molecules with functionalized tips

Recently, the family of high-resolution scanning probe imaging techniques using decorated tips has been complimented by a method based on inelastic electron tunneling spectroscopy (IETS). The new technique resolves the inner structure of organic molecules by mapping the vibrational energy of a single carbonmonoxide (CO) molecule positioned at the apex of a scanning tunnelling microscope (STM) tip. Here, we explain high-resolution IETS imaging by extending the model developed earlier for STM and atomic force microscopy (AFM) imaging with decorated tips. In particular, we show that the tip decorated with CO acts as a nanoscale sensor that changes the energy of the CO frustrated translation in response to the change of the local curvature of the surface potential. In addition, we show that high resolution AFM, STM and IETS-STM images can deliver information about intramolecular charge transfer for molecules deposited on a~surface. To demonstrate this, we extended our numerical model by taking into the account the electrostatic force acting between the decorated tip and surface Hartree potential.Comment: 5 pages, 4 figure

The mechanism of high-resolution STM/AFM imaging with functionalized tips

High resolution Atomic Force Microscopy (AFM) and Scanning Tunnelling Microscopy (STM) imaging with functionalized tips is well established, but a detailed understanding of the imaging mechanism is still missing. We present a numerical STM/AFM model, which takes into account the relaxation of the probe due to the tip-sample interaction. We demonstrate that the model is able to reproduce very well not only the experimental intra- and intermolecular contrasts, but also their evolution upon tip approach. At close distances, the simulations unveil a significant probe particle relaxation towards local minima of the interaction potential. This effect is responsible for the sharp sub-molecular resolution observed in AFM/STM experiments. In addition, we demonstrate that sharp apparent intermolecular bonds should not be interpreted as true hydrogen bonds, in the sense of representing areas of increased electron density. Instead they represent the ridge between two minima of the potential energy landscape due to neighbouring atoms

Scanning Quantum Dot Microscopy

Interactions between atomic and molecular objects are to a large extent defined by the nanoscale electrostatic potentials which these objects produce. We introduce a scanning probe technique that enables three-dimensional imaging of local electrostatic potential fields with sub-nanometer resolution. Registering single electron charging events of a molecular quantum dot attached to the tip of a (qPlus tuning fork) atomic force microscope operated at 5 K, we quantitatively measure the quadrupole field of a single molecule and the dipole field of a single metal adatom, both adsorbed on a clean metal surface. Because of its high sensitivity, the technique can record electrostatic potentials at large distances from their sources, which above all will help to image complex samples with increased surface roughness.Comment: main text: 5 pages, 4 figures, supplementary information file: 4 pages, 2 figure

How cold is the junction of a millikelvin scanning tunnelling microscope?

We employ a scanning tunnelling microscope (STM) cooled to millikelvin temperatures by an adiabatic demagnetization refrigerator (ADR) to perform scanning tunnelling spectroscopy (STS) on an atomically clean surface of Al(100) in a superconducting state using normal-metal and superconducting STM tips. Varying the ADR temperatures between 30 mK and 1.2 K, we show that the temperature of the STM junction $T$ is decoupled from the temperature of the surrounding environment $T_{\mathrm{env}}$. Simulating the STS data with the $P(E)$ theory, we determine that $T_{\mathrm{env}} \approx 1.5$ K, while the fitting of the superconducting gap spectrum yields the lowest $T=77$ mK.Comment: 12 pages, 10 figure

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A millikelvin scanning tunneling microscope in ultra-high vacuum with adiabatic demagnetization refrigeration

We present the design and performance of an ultra-high vacuum (UHV) scanning tunneling microscope (STM) that uses adiabatic demagnetization of electron magnetic moments for controlling its operating temperature in the range between 30 mK and 1 K with the accuracy of up to 7 $\mu$K. The time available for STM experiments at 50 mK is longer than 20 h, at 100 mK about 40 h. The single-shot adiabatic demagnetization refrigerator (ADR) can be regenerated automatically within 7 hours while keeping the STM temperature below 5 K. The whole setup is located in a vibrationally isolated, electromagnetically shielded laboratory with no mechanical pumping lines penetrating through its isolation walls. The 1K pot of the ADR cryostat can be operated silently for more than 20 days in a single-shot mode using a custom-built high-capacity cryopump. A high degree of vibrational decoupling together with the use of a specially-designed minimalistic STM head provides an outstanding mechanical stability, demonstrated by the tunneling current noise, STM imaging, and scanning tunneling spectroscopy measurements all performed on atomically clean Al(100) surface.Comment: 12 pages, 15 figure

Electrostatic potentials of atomic nanostructures at metal surfaces quantified by scanning quantum dot microscopy

The discrete and charge-separated nature of matter — electrons and nuclei — results in local electrostatic fields that are ubiquitous in nanoscale structures and relevant in catalysis, nanoelectronics and quantum nanoscience. Surface-averaging techniques provide only limited experimental access to these potentials, which are determined by the shape, material, and environment of the nanostructure. Here, we image the potential over adatoms, chains, and clusters of Ag and Au atoms assembled on Ag(111) and quantify their surface dipole moments. By focusing on the total charge density, these data establish a benchmark for theory. Our density functional theory calculations show a very good agreement with experiment and allow a deeper analysis of the dipole formation mechanisms, their dependence on fundamental atomic properties and on the shape of the nanostructures. We formulate an intuitive picture of the basic mechanisms behind dipole formation, allowing better design choices for future nanoscale systems such as single-atom catalysts

Quantum transport through STM-lifted single PTCDA molecules

Using a scanning tunneling microscope we have measured the quantum conductance through a PTCDA molecule for different configurations of the tip-molecule-surface junction. A peculiar conductance resonance arises at the Fermi level for certain tip to surface distances. We have relaxed the molecular junction coordinates and calculated transport by means of the Landauer/Keldysh approach. The zero bias transmission calculated for fixed tip positions in lateral dimensions but different tip substrate distances show a clear shift and sharpening of the molecular chemisorption level on increasing the STM-surface distance, in agreement with experiment.Comment: accepted for publication in Applied Physics