Hayakawa, Ryoma

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Single-charge transport through hybrid core-shell Au-ZnS quantum dot : A comprehensive analysis from the modified energy structure

2021-03-07, Basu, Tuhin Shuvra, Diesch, Simon, Hayakawa, Ryoma, Wakayama, Yutaka, Scheer, Elke

We examine the modified electronic structure and single-carrier transport of individual hybrid core-shell metal-semiconductor Au-ZnS quantum dots (QDs) by a scanning tunnel microscope. Nearly monodisperse ultra-small QDs are achieved by a facile wet chemical route. The exact energy structures are evaluated by scanning tunneling spectroscopy (STS) measurements at 300 mK for the individual nanoobjects starting from the main building block Au nanocrystals (NCs) to the final Au-ZnS QDs. The study divulges the evolution of the energy structure and the charge transport from the single metallic building block core to the core-shell metal-semiconductor QD. Further, we successfully determine the contributions related to the quantum-confinement-induced excitonic band structure of the ZnS nano-shell and the charging energy of the system by applying a semi-empirical approach considering a double barrier tunnel junction (DBTJ) arrangement. We detect strong conductance peaks in an Au-ZnS QD due to the overlapping of the energy structure of the Au nano-core and the discrete energy states of the semiconductor ZnS nano-shell. Our findings will help to understand the electronic properties of metal-semiconductor QDs. The outcomes, therefore, have the potential to fabricate tailored metal-semiconductor QDs for single-electron devices.

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Shot Noise of 1,4-Benzenedithiol Single-Molecule Junctions

2016-03-09, Karimi, Mohammad Amin, Bahoosh, Safa G., Herz, Markus, Hayakawa, Ryoma, Pauly, Fabian, Scheer, Elke

We report measurements of the shot noise on single-molecule Au-1,4-benzenedithiol-Au junctions, fabricated with the mechanically controllable break junction (MCBJ) technique at 4.2 K in a wide range of conductance values from 10(-2) to 0.24 conductance quanta. We introduce a simple measurement scheme using a current amplifier and a spectrum analyzer and that does not imply special requirements regarding the electrical leads. The experimental findings provide evidence that the current is carried by a single conduction channel throughout the whole conductance range. This observation suggests that the number of channels is limited by the Au-thiol bonds and that contributions due to direct tunneling from the Au to the π-system of the aromatic ring are negligible also for high conductance. The results are supported by quantum transport calculations using density functional theory.

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P-type polymer-based Ag2S atomic switch for “tug of war” operation

2017, Lutz, Carolin, Hasegawa, Tsuyoshi, Tsuchiya, Takashi, Adelsberger, Christoph, Hayakawa, Ryoma, Chikyow, Toyohiro

The Ag2S gap-type atomic switch based "tug of war" device is a promising element for building a new type of CMOS free neuromorphic computer-hardware. Since Ag+ cations are reduced during operation of the device, it was thought that the gap-material should be a n-type polymer. In this study, we revealed that the polymer bithiophene–oligoethyleneoxide (BTOE) doped poly(ethylene oxide) (PEO), which was used as gap-material in the first demonstration of the "tug of war", is a p-type polymer. For this we used impedance spectroscopy and transistor measurements. We elaborate on how the electrochemical processes in the "tug of war" devices could be explained in the case of p-type conductive gap-materials.

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Large Magnetoresistance in Single-Radical Molecular Junctions

2016-08-10, Hayakawa, Ryoma, Karimi, Mohammad Amin, Wolf, Jannic, Huhn, Thomas, Zöllner, Martin Sebastian, Herrmann, Carmen, Scheer, Elke

Organic radicals are promising building blocks for molecular spintronics. Little is known about the role of unpaired electrons for electron transport at the single-molecule level. Here, we examine the impact of magnetic fields on electron transport in single oligo(p-phenyleneethynylene) (OPE)-based radical molecular junctions, which are formed with a mechanically controllable break-junction technique at a low temperature of 4.2 K. Surprisingly huge positive magnetoresistances (MRs) of 16 to 287% are visible for a magnetic field of 4 T, and the values are at least 1 order of magnitude larger than those of the analogous pristine OPE (2-4%). Rigorous analysis of the MR and of current-voltage and inelastic electron-tunneling spectroscopy measurements reveal an effective reduction of the electronic coupling between the current-carrying molecular orbital and the electrodes with increasing magnetic field. We suggest that the large MR for the single-radical molecular junctions might be ascribed to a loss of phase coherence of the charge carriers induced by the magnetic field. Although further investigations are required to reveal the mechanism underlying the strong MR, our findings provide a potential approach for tuning charge transport in metal-molecule junctions with organic radicals.