We-Hyo Soe

Manipulating molecular quantum states with classical metal atom inputs: demonstration of a single molecule NOR logic gate.

Quantum states of a trinaphthylene molecule were manipulated by putting its naphthyl branches in contact with single Au atoms. One Au atom carries 1-bit of classical information input that is converted into quantum information throughout the molecule. The Au-trinaphthylene electronic interactions give rise to measurable energy shifts of the molecular electronic states demonstrating a NOR logic gate functionality. The NOR truth table of the single molecule logic gate was characterized by means of scanning tunnelling spectroscopy.

Mapping the Excited States of Single Hexa-peri-benzocoronene Oligomers

Electronic states of a molecule are usually analyzed via their decomposition in linear superposition of multielectronic Slater determinants built up from monoelectronics molecular orbitals. It is generally believed that a scanning tunneling microscope (STM) is able to map those molecular orbitals. Using a low-temperature ultrahigh vacuum (LT-UHV) STM, the dI/dV conductance maps of large single hexabenzocoronene (HBC) monomer, dimer, trimer, and tetramer molecules were recorded. We demonstrate that the attribution of a tunnel electronic resonance to a peculiar π molecular orbital of the molecule (or σ intermonomer chemical bond) in the STM junction is inappropriate. With an STM weak-measurement-like procedure, a dI/dV resonance results from the conductance contribution of many molecular states whose superposition makes it difficult to reconstruct an apparent molecular orbital electron probability density map.

Conformation Manipulation and Motion of a Double Paddle Molecule on an Au(111) Surface

The molecular conformation of a bisbinaphthyldurene (BBD) molecule is manipulated using a low-temperature ultrahigh-vacuum scanning tunneling microscope (LT-UHV STM) on an Au(111) surface. BBD has two binaphthyl groups at both ends connected to a central durene leading to anti/syn/flat conformers. In solution, dynamic nuclear magnetic resonance indicated the fast interexchange between the anti and syn conformers as confirmed by density functional theory calculations. After deposition in a submonolayer on an Au(111) surface, only the syn conformers were observed forming small islands of self-assembled syn dimers. The syn dimers can be separated into syn monomers by STM molecular manipulations. A flat conformer can also be prepared by using a peculiar mechanical unfolding of a syn monomer by STM manipulations. The experimental STM dI/dV and theoretical elastic scattering quantum chemistry maps of the low-lying tunneling resonances confirmed the flat conformer BBD molecule STM production. The key BBD electronic states for a step-by-step STM inelastic excitation lateral motion on the Au(111) are presented requiring no mechanical interactions between the STM tip apex and the BBD. On the BBD molecular board, selected STM tip apex positions for this inelastic tunneling excitation enable the flat BBD to move controllably on Au(111) by a step of 0.29 nm per bias voltage ramp.

Mapping the first electronic resonances of a Cu phthalocyanine STM tunnel junction

Using a low temperature, ultrahigh vacuum scanning tunneling microscope (STM), dI/dV differential conductance maps were recorded at the tunneling resonance energies for a single Cu phthalocyanine molecule adsorbed on an Au(111) surface. We demonstrated that, contrary to the common assumption, such maps are not representative of the molecular orbital spatial expansion, but rather result from their complex superposition captured by the STM tip apex with a superposition weight which generally does not correspond to the native weight used in the standard Slater determinant basis set. Changes in the molecule conformation on the Au(111) surface further obscure the identification between dI/dV conductance maps and the native molecular orbital electronic probability distribution in space.

High Voltage STM Imaging of Single Copper Phthalocyanine

In this chapter experiments done to investigate the scanning tunneling microscope (STM) imaging at near field emission voltages of single Copper Phthalocyanine (CuPc) molecules deposited on Au(111) are presented. An imaging bias voltage range is explored exceeding the standard tunneling imaging conditions going from the threshold of the tunneling junction barrier up to −10.0 V. At this voltage regime current transmitted through the tip-molecule–substrate junction is made not only of tunneling electrons but also of electrons overcoming the tunneling barrier and behaving like free electrons. Our interpretation of the process, enabling the visualization of the electronic cloud of single organic molecules under these conditions, is presented.

Nanogears Mechanics: From a Single Molecule to Solid-State Nanogears on a Surface

The first experimental demonstration of a controllable rotating molecule gear is presented. A scanning tunneling microscope (STM) is used to construct, manipulate, and observe the rotation of the molecule gear. The appropriate combination of molecule design, molecule manipulation protocol, and surface atomic structure selection leads to the functioning of the molecule gear. Rotation of the molecule gear is done step-by-step and totally under control. The fabrication of solid-state SiO2 nanogears with diameters ranging from 30 nm up to 1 μm and their manipulation using an atomic force microscope tip on a graphite surface is also presented. Ranging in sizes from few tens of nanometers up to submicron diameters, they are going to enable the transmission of mechanical motion from functional mechanical molecule machineries to larger submicron or micron-sized devices through series of solid-state gears and mechanical components compatible with the semiconductor and electronics industry technology.

Mapping the Electronic Resonances of Single Molecule STM Tunnel Junctions

In this chapter is presented how the electron probability distributions of molecular states are imaged in real space using scanning tunneling microscopy. Differential tunneling conductance images of selected single molecules taken at voltages corresponding to resonances near the substrate Fermi level were found to be very close to their respective mono-electronic molecular orbitals. In contrast, high-order resonance states images were composed of molecular orbitals components from many states, even though those states lie in a lower energy range.