Charge‐carrier transport through an individually contacted bipyridyl‐dinitro oligophenylene‐ethynylene dithiol molecule (BPDN‐DT, see picture) and through a BP‐DT molecule was studied using the mechanically controllable break‐junction technique. BPDN‐DT exhibits a voltage‐induced switching between two distinct conductive states, in contrast to BP‐DT.
We present a statistical approach that combines comprehensive current-voltage data acquisition during the controlled manipulation of a molecular junction with subsequent statistical analysis. Thereby the most probable transport characteristics can be determined. The excellent sensitivity of this impartial approach to even subnanometer-long molecules is illustrated by benzene-1,4-dithiol and 4,4"-bis(acetylthiol)-2,2',5',2"-tetramethyl-[1,1';4',1"] terphenyl results.
The weak interlayer binding in two-dimensional layered materials such as graphite gives rise to poorly understood low-friction characteristics. Accurate measurements of the adhesion forces governing the overall mechanical stability have also remained elusive. We report on the direct mechanical measurement of line tension and friction forces acting in sheared mesoscale graphite structures. We show that the friction is fundamentally stochastic in nature and is attributable to the interaction between the incommensurate interface lattices. We also measured an adhesion energy of 0.227 ± 0.005 joules per square meter, in excellent agreement with theoretical models. In addition, bistable all-mechanical memory cell structures and rotational bearings have been realized by exploiting position locking, which is provided solely by the adhesion energy.
Charge transport through single molecules can be influenced by the charge and spin states of redox-active metal centres placed in the transport pathway. These molecular intrinsic properties are usually addressed by varying the molecule's electrochemical and magnetic environment, a procedure that requires complex setups with multiple terminals. Here we show that oxidation and reduction of organometallic compounds containing either Fe, Ru or Mo centres can solely be triggered by the electric field applied to a two-terminal molecular junction. Whereas all compounds exhibit bias-dependent hysteresis, the Mo-containing compound additionally shows an abrupt voltage-induced conductance switching, yielding high-to-low current ratios exceeding 1000 at voltage stimuli of less than 1.0 V. DFT calculations identify a localized, redox-active molecular orbital that is weakly coupled to the electrodes and closely aligned with the Fermi energy of the leads because of the spin-polarised ground state unique to the Mo centre. This situation opens an additional slow and incoherent hopping channel for transport, triggering a transient charging effect of the entire molecule and a strong hysteresis with unprecedented high low-to-high current ratios.
Charge transport through single diblock dipyrimidinyl diphenyl molecules consisting of a donor and acceptor moiety was measured in the low-bias regime and as a function of bias at different temperatures using the mechanically controllable break-junction technique. Conductance histograms acquired at 10 mV reveal two distinct peaks, separated by a factor of 1.5, representing the two orientations of the single molecule with respect to the applied bias. The current-voltage characteristics exhibit a temperature-independent rectification of up to a factor of 10 in the temperature range between 300 and 50 K with single-molecule currents of 45-70 nA at ±1.5 V. The current-voltage characteristics are discussed using a semiempirical model assuming a variable coupling of the molecular energy levels as well as a nonsymmetric voltage drop across the molecular junction, thus shifting the energy levels accordingly. The excellent agreement of the data with the proposed model suggests that the rectification originates from an asymmetric Coulomb blockade in combination with an electric-field-induced level shifting.
Graphene and layered materials in general exhibit rich physics and application potential owing to their exceptional electronic properties, which arise from the intricate π-orbital coupling and the symmetry breaking in twisted bilayer systems. Here, we report room-temperature experiments to study electrical transport across a bilayer graphene interface with a well-defined rotation angle between the layers that is controllable in situ. This twisted interface is artificially created in mesoscopic pillars made of highly oriented pyrolytic graphite by mechanical actuation. The overall measured angular dependence of the conductivity is consistent with a phonon-assisted transport mechanism that preserves the electron momentum of conduction electrons passing the interface. The most intriguing observations are sharp conductivity peaks at interlayer rotation angles of 21.8° and 38.2°. These angles correspond to a commensurate crystalline superstructure leading to a coherent two-dimensional (2D) electronic interface state. Such states, predicted by theory, form the basis for a new class of 2D weakly coupled bilayer systems with hitherto unexplored properties and applications.
Many efficient light-emitting devices and photodetectors are based on semiconductors with, respectively, a direct or indirect bandgap configuration. The less known pseudodirect bandgap configuration can be found in wurtzite (WZ) semiconductors: here electron and hole wave-functions overlap strongly but optical transitions between these states are impaired by symmetry. Switching between bandgap configurations would enable novel photonic applications but large anisotropic strain is normally needed to induce such band structure transitions. Here we show that the luminescence of WZ GaAs nanowires can be switched on and off, by inducing a reversible direct-to-pseudodirect band structure transition, under the influence of a small uniaxial stress. For the first time, we clarify the band structure of WZ GaAs, providing a conclusive picture of the energy and symmetry of the electronic states. We envisage a new generation of devices that can simultaneously serve as efficient light emitters and photodetectors by leveraging the strain degree of freedom.
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