RESUMEN
We outline calibrated measurements of the microwave reflection coefficient from the tunnel junction of an ultra-high vacuum low temperature scanning tunneling microscope. The microwave circuit design is described in detail, including an interferometer for an enhanced signal-to-noise ratio and a demodulation scheme for lock-in detection. A quantitative, in situ procedure for impedance calibration based on the numerical three-error-term model is presented. Our procedure exploits the response of the microwave reflection signal due to the change of the tunneling conductance caused by sub-nm variation of the tunneling distance. Experimental calibration is achieved by a least-squares numerical fit of simultaneously measured conductance and microwave reflection retraction curves at finite conductance. Our method paves the way for nanoscale microscopy and spectroscopy of dielectric surface properties at GHz frequencies and cryogenic temperatures. This opens a promising pathway even for dielectric fingerprinting at the single molecule limit.
RESUMEN
Diverse spectroscopic methods operating at radio frequency depend on a reliable calibration to compensate for the frequency dependent damping of the transmission lines. Calibration may be impeded by the existence of a sensitive interdependence of two or more experimental parameters. Here, we show by combined scanning tunnelling microscopy measurements and numerical simulations how a frequency-dependent conductance response is affected by different DC conductance behaviours of the tunnel junction. Distinct and well-defined DC-conductance behaviour is provided by our experimental model systems, which include C60 molecules on Au(111), exhibiting electronic configurations distinct from the well-known dim and bright C60's reported so far. We investigate specific combinations of experimental parameters. Variations of the modulation amplitude as small as only a few percent may result in systematic conductance deviations as large as one order of magnitude. We provide practical guidelines for calibrating respective measurements, which are relevant to RF spectroscopic measurements.
RESUMEN
Dielectric relaxation lies at the heart of well-established techniques of dielectric spectroscopy essential to diverse fields of research and technology. We report an experimental route for increasing the sensitivity of dielectric spectroscopy ultimately towards the scale of a single molecule. We use the method of radio frequency scanning tunneling microscopy to excite a single molecule junction based on a polar substituted helicene molecule by an electric field oscillating at 2-5 GHz. We detect the dielectric relaxation of the single molecule junction indirectly via its effect of power dissipation, which causes lateral displacement. From our data we determine a corresponding relaxation time of about 300 ps-consistent with literature values of similar helicene derivatives obtained by conventional methods of dielectric spectroscopy.
RESUMEN
Radio-frequency (rf) scanning tunneling microscopy has recently been advanced to methods such as single-atom spin resonance. Such methods benefit from a frequency-independent rf voltage amplitude across the tunnel junction, which is challenging to achieve due to the strong frequency dependence of the rf attenuation in a transmission line. Two calibration methods for the rf amplitude have been reported to date. In this Note, we present an alternative method to achieve a frequency-independent rf voltage amplitude across the tunnel junction and show the results of this calibration. The presented procedure is applicable to devices that can deliver rf voltage to a tunnel junction.
RESUMEN
Active optical control over matter is desirable in many scientific disciplines, with prominent examples in all-optical magnetic switching1,2, light-induced metastable or exotic phases of solids3-8 and the coherent control of chemical reactions9,10. Typically, these approaches dynamically steer a system towards states or reaction products far from equilibrium. In solids, metal-to-insulator transitions are an important target for optical manipulation, offering ultrafast changes of the electronic4 and lattice11-16 properties. The impact of coherences on the efficiencies and thresholds of such transitions, however, remains a largely open subject. Here, we demonstrate coherent control over a metal-insulator structural phase transition in a quasi-one-dimensional solid-state surface system. A femtosecond double-pulse excitation scheme17-20 is used to switch the system from the insulating to a metastable metallic state, and the corresponding structural changes are monitored by ultrafast low-energy electron diffraction21,22. To govern the transition, we harness vibrational coherence in key structural modes connecting both phases, and observe delay-dependent oscillations in the double-pulse switching efficiency. Mode-selective coherent control of solids and surfaces could open new routes to switching chemical and physical functionalities, enabled by metastable and non-equilibrium states.
RESUMEN
An on-surface bimolecular system is described, comprising a simple divalent bis(imidazolyl) molecule that is shown to "walk" at room temperature via an inchworm mechanism along a specific pathway terminated at each end by oligomeric "fences" constructed on a monocrystalline copper surface. Scanning tunneling microscopy shows that the motion of the walker occurs along the [110] direction of the Cu surface with remarkably high selectivity and is effectively confined by the orthogonal construction of covalent porphyrin oligomers along the [001] surface direction, which serve as barriers. Density functional theory shows that the mobile molecule walks by attaching and detaching the nitrogen atoms in its imidazolyl "legs" to and from the protruding close-packed rows of the metal surface and that it can transit between two energetically equivalent extended and contracted conformations by overcoming a small energy barrier.
