Break junctions are important in generating nanosensors and single molecular devices. The mechanically con- trollable break junction is the most widely used method for a break junction due to its simplicity and stabil...Break junctions are important in generating nanosensors and single molecular devices. The mechanically con- trollable break junction is the most widely used method for a break junction due to its simplicity and stability. However, the bandwidths of traditional devices are limited to about a few hertz. Moreover, when using traditional methods it is hard to allow independent control of more than one junction. Here we propose on-chip thermally controllable break junctions to overcome these challenges. This is verified by using finite element analysis. Adopting microelectromechanical systems produces features of high bandwidth and independent controllability to this new break junction system. The proposed method will have a wide range of applications on on-chip high speed independent controllable and highly integrated single molecule devices.展开更多
We report an electrochemically assisted mechanically controllable break junction (EC-MCBJ) approach to investigating single molecule conductance. Electrode pairs connected with a gold nanobridge were fabricated by e...We report an electrochemically assisted mechanically controllable break junction (EC-MCBJ) approach to investigating single molecule conductance. Electrode pairs connected with a gold nanobridge were fabricated by electrochemical deposition and then mounted on a homebuilt MCBJ platform. A large number of Au- molecule-Au junctions were produced sequentially by repeated breaking and reconnecting of the gold nanobridge. In order to measure their single molecule conductance, statistical conductance histograms were generated for benzene-l,4-dithiol (BDT) and 4,4'-bipyridine (BPY). The values extracted from these histograms were found to be in the same range as values previously reported in the literature. Our method is distinct from the ones used to acquire these previously reported literature values, however, in that it is faster, simpler, more cost-effective, and changing the electrode material is more convenient.展开更多
In this article, we report on the characterization of various molecular junctions' current-voltage characteristics (Ⅰ-Ⅴ curves) evolution under mechanical modulations, by employing a novel electrochemically assis...In this article, we report on the characterization of various molecular junctions' current-voltage characteristics (Ⅰ-Ⅴ curves) evolution under mechanical modulations, by employing a novel electrochemically assisted-mechanically controllable break junction (EC-MCBJ) method. For 1,4-benzenedithiol, the Ⅰ-Ⅴ curves measured at constant electrode pair separation show excellent reproducibility, indicating the feasibility of our EC-MCBJ method for fabricating molecular junctions. For ferrocene-bisvinylphenylmethyl dithiol (Fc-VPM), an anomalous type of Ⅰ-Ⅴ curve was observed by the particular control over the stepping motor. This phenomenon is rationalized assuming a model of atomic contact evolution with the presence of molecular junctions. To test this hypothesized model, a molecule with a longer length, 1,3-butadiyne-linked dinuclear ruthenium(H) complex (Ru-1), was implemented, and the Ⅰ-Ⅴ curve evolution was investigated under similar circumstances. Compared with Fc-VPM, the observed Ⅰ-Ⅴ curves show close analogy and minor differences, and both of them fit the hypothesized model well.展开更多
The quantum interference effect in the charge transport through single-phenyl molecules received intensive interests from theory but remained as an experimental challenge. In this paper, we investigated the charge tra...The quantum interference effect in the charge transport through single-phenyl molecules received intensive interests from theory but remained as an experimental challenge. In this paper, we investigated the charge transport through single-molecule benzene dithiol (BDT) junction with different connectivities using mechanically controllable break.junction (MCB]) technique. By further improving the mechanical stability and the electronic measuring component of the MCBJ set-up, we obtained the conductance histograms of BDT molecules (BDTs) from the statistical analysis of conductance-distance traces without data selection. By tuning the connectivity, the conductance of BDTs is determined to be 10-12Go, 10-22Go and 10-10Go for pcra, meta, and ortho connectivity, following the trend that ortfio-BDT 〉 para-BDT 〉 meta-BDT. Furthermore, the displacements of the junctions followed the trend that para 〉 meta 〉 ortho, suggesting the charge transport through the molecules via the gold-thiol bond. The different trends between conductance and displacement for different connectivities suggests the presence of destructive quantum interference effect on meta-BDT, which provides the experimental evidence for the quantum interference effect through single-phenyl molecular junctions.展开更多
Plasmonic optical manipulation has emerged as an affordable alternative to manipulate single chemical and biological molecules in nanoscience.Although the theoretical models of sub-5 nm single-molecule trapping have b...Plasmonic optical manipulation has emerged as an affordable alternative to manipulate single chemical and biological molecules in nanoscience.Although the theoretical models of sub-5 nm single-molecule trapping have been considered promising,the experimental strategies remain a challenge due to the Brownian motions and weak optical gradient forces with significantly reduced molecular polarizability.Herein,we address direct trapping and in situ sensing of single molecules with unprecedented size,down to∼5Åin solution,by employing an adjustable plasmonic optical nanogap and single-molecule conductance measurement.The theoretical simulations demonstrate that local fields with a high enhancement factor,over 103,were generated at such small nanogaps,resulting in optical forces as large as several piconewtons to suppress the Brownian motion and trap a molecule of length sub-1 nm.This work demonstrates a strategy for directly manipulating the small molecule units,promising a vast multitude of applications in chemical,biological,and materials sciences at the single-molecule level.展开更多
基金Supported by the National Key Basic Research Program of China under Grant No 2013CB921800the National Natural Science Foundation of China under Grant Nos 11227901,91021005,11274299,11104262 and 10834005the Strategic Priority Research Program(B)of the Chinese Academy of Sciences under Grant No XDB01030400
文摘Break junctions are important in generating nanosensors and single molecular devices. The mechanically con- trollable break junction is the most widely used method for a break junction due to its simplicity and stability. However, the bandwidths of traditional devices are limited to about a few hertz. Moreover, when using traditional methods it is hard to allow independent control of more than one junction. Here we propose on-chip thermally controllable break junctions to overcome these challenges. This is verified by using finite element analysis. Adopting microelectromechanical systems produces features of high bandwidth and independent controllability to this new break junction system. The proposed method will have a wide range of applications on on-chip high speed independent controllable and highly integrated single molecule devices.
文摘We report an electrochemically assisted mechanically controllable break junction (EC-MCBJ) approach to investigating single molecule conductance. Electrode pairs connected with a gold nanobridge were fabricated by electrochemical deposition and then mounted on a homebuilt MCBJ platform. A large number of Au- molecule-Au junctions were produced sequentially by repeated breaking and reconnecting of the gold nanobridge. In order to measure their single molecule conductance, statistical conductance histograms were generated for benzene-l,4-dithiol (BDT) and 4,4'-bipyridine (BPY). The values extracted from these histograms were found to be in the same range as values previously reported in the literature. Our method is distinct from the ones used to acquire these previously reported literature values, however, in that it is faster, simpler, more cost-effective, and changing the electrode material is more convenient.
基金This work was supported by the National Basic Research Program of China (Nos. 2011YQ030124, 2014CB845603, and 2015CB932301), National Natural Science Foundation of China (Nos. 91427304, 21321062, 21303114, 21403181, and 21503179), Natural Science Foundation of Fujian Province (No. 2012J05034), and by CNRS UMR 8640 PASTEUR and LIA CNRS NanoBioCatEchem.
文摘In this article, we report on the characterization of various molecular junctions' current-voltage characteristics (Ⅰ-Ⅴ curves) evolution under mechanical modulations, by employing a novel electrochemically assisted-mechanically controllable break junction (EC-MCBJ) method. For 1,4-benzenedithiol, the Ⅰ-Ⅴ curves measured at constant electrode pair separation show excellent reproducibility, indicating the feasibility of our EC-MCBJ method for fabricating molecular junctions. For ferrocene-bisvinylphenylmethyl dithiol (Fc-VPM), an anomalous type of Ⅰ-Ⅴ curve was observed by the particular control over the stepping motor. This phenomenon is rationalized assuming a model of atomic contact evolution with the presence of molecular junctions. To test this hypothesized model, a molecule with a longer length, 1,3-butadiyne-linked dinuclear ruthenium(H) complex (Ru-1), was implemented, and the Ⅰ-Ⅴ curve evolution was investigated under similar circumstances. Compared with Fc-VPM, the observed Ⅰ-Ⅴ curves show close analogy and minor differences, and both of them fit the hypothesized model well.
基金supported by the Ministry of Science and Technology of China(No. SQ2017YFJC020081)the National Natural Science Foundation of China(Nos. 21673195,21503179)+2 种基金Fundamental Research Funds for the Central Universities in China (Xiamen University: No. 20720170035)Natural Science Foundation of Fujian Province(No. 2016J05162)the Young Thousand Talent Project of China
文摘The quantum interference effect in the charge transport through single-phenyl molecules received intensive interests from theory but remained as an experimental challenge. In this paper, we investigated the charge transport through single-molecule benzene dithiol (BDT) junction with different connectivities using mechanically controllable break.junction (MCB]) technique. By further improving the mechanical stability and the electronic measuring component of the MCBJ set-up, we obtained the conductance histograms of BDT molecules (BDTs) from the statistical analysis of conductance-distance traces without data selection. By tuning the connectivity, the conductance of BDTs is determined to be 10-12Go, 10-22Go and 10-10Go for pcra, meta, and ortho connectivity, following the trend that ortfio-BDT 〉 para-BDT 〉 meta-BDT. Furthermore, the displacements of the junctions followed the trend that para 〉 meta 〉 ortho, suggesting the charge transport through the molecules via the gold-thiol bond. The different trends between conductance and displacement for different connectivities suggests the presence of destructive quantum interference effect on meta-BDT, which provides the experimental evidence for the quantum interference effect through single-phenyl molecular junctions.
基金supported by the National Natural Science Foundation of China(grant nos.T2222002,21973079,22032004,92161118,12174324,21991130,and 21905238)the Ministry of Science and Technology of the People’s Republic of China(grant no.2021YFA1201502)the Natural Science Foundation of Fujian Province(grant no.2021J06008).
文摘Plasmonic optical manipulation has emerged as an affordable alternative to manipulate single chemical and biological molecules in nanoscience.Although the theoretical models of sub-5 nm single-molecule trapping have been considered promising,the experimental strategies remain a challenge due to the Brownian motions and weak optical gradient forces with significantly reduced molecular polarizability.Herein,we address direct trapping and in situ sensing of single molecules with unprecedented size,down to∼5Åin solution,by employing an adjustable plasmonic optical nanogap and single-molecule conductance measurement.The theoretical simulations demonstrate that local fields with a high enhancement factor,over 103,were generated at such small nanogaps,resulting in optical forces as large as several piconewtons to suppress the Brownian motion and trap a molecule of length sub-1 nm.This work demonstrates a strategy for directly manipulating the small molecule units,promising a vast multitude of applications in chemical,biological,and materials sciences at the single-molecule level.