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Register a new userElectroluminescence from a polythiophene molecular wire suspended in a plasmonic scanning tunneling microscope junction
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The electroluminescence of a polythiophene wire suspended between two metallic electrodes is probed using a scanning tunneling microscope. Under positive sample voltage, the spectral and voltage dependencies of the emitted light are consistent with the fluorescence of the wire junction mediated by localized plasmons. This emission is strongly attenuated for the opposite polarity. Both emission mechanism and polarity dependence are similar to what occurs in organic light emitting diodes (OLED) but at the level of a single molecular wire.
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The coupling between molecular exciton and gap plasmons plays a key role in single molecular electroluminescence induced by a scanning tunneling microscope (STM). But it has been difficult to clarify the complex experimental phenomena. By employing the nonequilibrium Greens function method, we propose a general theoretical model to understand the light emission spectrum from single molecule and gap plasmons from an energy transport point of view. The coherent interaction between gap plasmons and molecular exciton leads to a prominent Fano resonance in the emission spectrum. We analyze the dependence of the Fano line shape on the system parameters, based on which we provide a unified account of several recent experimental observations. Moreover, we highlight the effect of the tip-molecule electronic coupling on the spectrum, which has hitherto not been considered.
We present the main features of a home-built scanning tunneling microscope that has been attached to the mixing chamber of a dilution refrigerator. It allows scanning tunneling microscopy and spectroscopy measurements down to the base temperature of the cryostat, T approx. 30mK, and in applied magnetic fields up to 13T. The topography of both highly-ordered pyrolytic graphite (HOPG) and the dichalcogenide superconductor NbSe2 have been imaged with atomic resolution down to T approx. 50mK as determined from a resistance thermometer adjacent to the sample. As a test for a successful operation in magnetic fields, the flux-line lattice of superconducting NbSe2 in low magnetic fields has been studied. The lattice constant of the Abrikosov lattice shows the expected field dependence B^{-0.5} and measurements in the STS mode clearly show the superconductive density of states with Andreev bound states in the vortex core.
Experimental advances allow for the inclusion of multiple probes to measure the transport properties of a sample surface. We develop a theory of dual-probe scanning tunnelling microscopy using a Greens Function formalism, and apply it to graphene. Sampling the local conduction properties at finite length scales yields real space conductance maps which show anisotropy for pristine graphene systems and quantum interference effects in the presence of isolated impurities. The spectral signatures of the Fourier transform of real space conductance maps include characteristics that can be related to different scattering processes. We compute the conductance maps of graphene systems with different edge geometries or height fluctuations to determine the effects of non-ideal graphene samples on dual-probe measurements.
The detection of fluorescence with submolecular resolution enables the exploration of spatially varying photon yields and vibronic properties at the single-molecule level. By placing individual polycyclic aromatic hydrocarbon molecules into the plasmon cavity formed by the tip of a scanning tunneling microscope and a NaCl-covered Ag(111) surface, molecular light emission spectra are obtained that unravel vibrational progression. In addition, light spectra unveil a signature of the molecule even when the tunneling current is injected well separated from the molecular emitter. This signature exhibits a distance-dependent Fano profile that reflects the subtle interplay between inelastic tunneling electrons, the molecular exciton and localized plasmons in at-distance as well as on-molecule fluorescence. The presented findings open the path to luminescence of a different class of molecules than investigated before and contribute to the understanding of single-molecule luminescence at surfaces in a unified picture.
We have performed low-temperature scanning tunneling spectroscopy measurements on suspended single-wall carbon nanotubes with a gate electrode allowing three-terminal spectroscopy measurements. These measurements show well-defined Coulomb diamonds as well as side peaks from phonon-assisted tunneling. The side peaks have the same gate voltage dependence as the main Coulomb peaks, directly proving that they are excitations of these states.
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