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A straightforward method to generate both atomic-scale sharp and atomic-scale planar electrodes is reported. The atomic-scale sharp electrodes are generated by precisely stretching a suspended nanowire, while the atomic-scale planar electrodes are obtained via mechanically controllable interelectrodes compression followed by a thermal-driven atom migration process. Notably, the gap size between the electrodes can be precisely controlled at subangstrom accuracy with this method. These two types of electrodes are subsequently employed to investigate the properties of single molecular junctions. It is found, for the first time, that the conductance of the amine-linked molecular junctions can be enhanced ≈50% as the atomic-scale sharp electrodes are used. However, the atomic-scale planar electrodes show great advantages to enhance the sensitivity of Raman scattering upon the variation of nanogap size. The underlying mechanisms for these two interesting observations are clarified with the help of density functional theory calculation and finite-element method simulation. These findings not only provide a strategy to control the electron transport through the molecule junction, but also pave a way to modulate the optical response as well as to improve the stability of single molecular devices via the rational design of electrodes geometries.

Electronic switches with nanoscale dimensions satisfy an urgent demand for further device miniaturization. A recent heavily investigated approach for nanoswitches is the use of molecular junctions that employ photochromic molecules that toggle between two distinct isoforms. In contrast to the reports on this approach, we demonstrate that the conductance switch behavior can be realized with only a bare metallic contact without any molecules under light illumination. We demonstrate that the conductance of bare metallic quantum contacts can be reversibly switched over eight orders of magnitude, which substantially exceeds the performance of molecular switches. After the switch process, the gap size between two electrodes can be precisely adjusted with subangstrom accuracy by controlling the light intensity or polarization. Supported by simulations, we reveal a more general and straightforward mechanism for nanoswitching behavior, i.e., atomic switches can be realized by the expansion of nanoelectrodes due to plasmonic heating.

To reduce the size of optoelectronic devices, it is essential to understand the crystal size effect on the carrier transport through microscale materials. Here, we show a soft contact method to probe the properties of irregularly shaped microscale perovskite crystals by employing a movable liquid metal electrode to form a self-adaptative deformable electrode−perovskite−electrode junction. Accordingly, we demonstrate that (1) the photocurrents of perovskite quantum dot films and microplatelets show profound differences regarding both the on/off ratio and the response time upon light illumination; and (2) small-size perovskite (<50 μm) junctions may show negative differential resistance (NDR) behavior, whereas the NDR phenomenon is absent in large-size perovskite junctions within the same bias regime. Our studies provide a method for studying arbitrary-shaped crystals without mechanical damage, assisting the understanding of the photogenerated carriers transport through microscale crystals.

We develop a method based on the mechanically controllable break junction technique to investigate the electron transport properties of single molecular junctions upon fiber waveguided light. In our strategy, a...