scholarly journals A Chemically Soldered Polyoxometalate Single-Molecule Transistor

Author(s):  
Chuanli Wu ◽  
Xiaohang Qiao ◽  
Craig M. Robertson ◽  
Simon Higgins ◽  
Chenxin Cai ◽  
...  

Polyoxometalates have been proposed in the literature as promising components for nanoelectronic applications, where they could offer key advantages with their structural versatility and rich electrochemistry. Apart from a few studies on their ensemble behaviour (for instance, as monolayers or thin films) this potential remains largely unexplored. We synthesised a pyridyl-capped Anderson-Evans polyoxometalate and used it to fabricate single-molecule junctions, by using the organic termini to chemically “solder” a single metal oxide cluster to two nanoelectrodes through coordination bonds. Operating the device in an electrochemical environment allowed us to probe charge transport through different oxidation states of the polyoxometalate, and we report here an efficient three-state transistor behaviour. Conductance data fits a quantum tunnelling transport mechanism, with charge having different tunnelling probabilities through different oxidation states of the polyoxometalate. Our results show the promise of such compounds in nanoelectronics, and are, to our best knowledge, the first report on the single-entity electrochemical behaviour of polyoxometalates.<p></p>

2020 ◽  
Author(s):  
Chuanli Wu ◽  
Xiaohang Qiao ◽  
Craig M. Robertson ◽  
Simon Higgins ◽  
Chenxin Cai ◽  
...  

Polyoxometalates have been proposed in the literature as promising components for nanoelectronic applications, where they could offer key advantages with their structural versatility and rich electrochemistry. Apart from a few studies on their ensemble behaviour (for instance, as monolayers or thin films) this potential remains largely unexplored. We synthesised a pyridyl-capped Anderson-Evans polyoxometalate and used it to fabricate single-molecule junctions, by using the organic termini to chemically “solder” a single metal oxide cluster to two nanoelectrodes through coordination bonds. Operating the device in an electrochemical environment allowed us to probe charge transport through different oxidation states of the polyoxometalate, and we report here an efficient three-state transistor behaviour. Conductance data fits a quantum tunnelling transport mechanism, with charge having different tunnelling probabilities through different oxidation states of the polyoxometalate. Our results show the promise of such compounds in nanoelectronics, and are, to our best knowledge, the first report on the single-entity electrochemical behaviour of polyoxometalates.<p></p>


2020 ◽  
Author(s):  
Chuanli Wu ◽  
Xiaohang Qiao ◽  
Craig M. Robertson ◽  
Simon Higgins ◽  
Chenxin Cai ◽  
...  

Polyoxometalates have been proposed in the literature as promising components for nanoelectronic applications, where they could offer key advantages with their structural versatility and rich electrochemistry. Apart from a few studies on their ensemble behaviour (for instance, as monolayers or thin films) this potential remains largely unexplored. We synthesised a pyridyl-capped Anderson-Evans polyoxometalate and used it to fabricate single-molecule junctions, by using the organic termini to chemically “solder” a single metal oxide cluster to two nanoelectrodes through coordination bonds. Operating the device in an electrochemical environment allowed us to probe charge transport through different oxidation states of the polyoxometalate, and we report here an efficient three-state transistor behaviour. Conductance data fits a quantum tunnelling transport mechanism, with charge having different tunnelling probabilities through different oxidation states of the polyoxometalate. Our results show the promise of such compounds in nanoelectronics, and are, to our best knowledge, the first report on the single-entity electrochemical behaviour of polyoxometalates.<p></p>


2021 ◽  
Vol 7 (10) ◽  
pp. eabe4365
Author(s):  
Zihao Liu ◽  
Xingxing Li ◽  
Hiroshi Masai ◽  
Xinyi Huang ◽  
Susumu Tsuda ◽  
...  

One of the ultimate goals of analytic chemistry is to efficiently discriminate between amino acids. Here we demonstrate this ability using a single-molecule electrical methodology based on molecular nanocircuits formed from stable graphene-molecule-graphene single-molecule junctions. These molecular junctions are fabricated by covalently bonding a molecular machine featuring a permethylated-β-cyclodextrin between a pair of graphene point contacts. Using pH to vary the type and charge of the amino acids, we find distinct multimodal current fluctuations originating from the different host-guest interactions, consistent with theoretical calculations. These conductance data produce characteristic dwell times and shuttling rates for each amino acid, and allow accurate, statistical real-time, in situ measurements. Testing four amino acids and their enantiomers shows the ability to distinguish between them within a few microseconds, thus paving a facile and precise way to amino acid identification and even single-molecule protein sequencing.


2020 ◽  
Author(s):  
María Camarasa-Gómez ◽  
Daniel Hernangómez-Pérez ◽  
Michael S. Inkpen ◽  
Giacomo Lovat ◽  
E-Dean Fung ◽  
...  

Ferrocenes are ubiquitous organometallic building blocks that comprise a Fe atom sandwiched between two cyclopentadienyl (Cp) rings that rotate freely at room temperature. Of widespread interest in fundamental studies and real-world applications, they have also attracted<br>some interest as functional elements of molecular-scale devices. Here we investigate the impact of<br>the configurational degrees of freedom of a ferrocene derivative on its single-molecule junction<br>conductance. Measurements indicate that the conductance of the ferrocene derivative, which is<br>suppressed by two orders of magnitude as compared to a fully conjugated analog, can be modulated<br>by altering the junction configuration. Ab initio transport calculations show that the low conductance is a consequence of destructive quantum interference effects that arise from the hybridization of metal-based d-orbitals and the ligand-based π-system. By rotating the Cp rings, the hybridization, and thus the quantum interference, can be mechanically controlled, resulting in a conductance modulation that is seen experimentally.<br>


2018 ◽  
Author(s):  
Kun Wang ◽  
Andrea Vezzoli ◽  
Iain Grace ◽  
Maeve McLaughlin ◽  
Richard Nichols ◽  
...  

We have used scanning tunneling microscopy to create and study single molecule junctions with thioether-terminated oligothiophene molecules. We find that the conductance of these junctions increases upon formation of charge transfer complexes of the molecules with tetracyanoethene, and that the extent of the conductance increase is greater the longer is the oligothiophene, i.e. the lower is the conductance of the uncomplexed molecule in the junction. We use non-equilibrium Green's function transport calculations to explore the reasons for this theoretically, and find that new resonances appear in the transmission function, pinned close to the Fermi energy of the contacts, as a consequence of the charge transfer interaction. This is an example of a room temperature quantum interference effect, which in this case boosts junction conductance in contrast to earlier observations of QI that result in diminished conductance.<br>


Nano Letters ◽  
2012 ◽  
Vol 12 (3) ◽  
pp. 1643-1647 ◽  
Author(s):  
Sriharsha V. Aradhya ◽  
Jeffrey S. Meisner ◽  
Markrete Krikorian ◽  
Seokhoon Ahn ◽  
Radha Parameswaran ◽  
...  

Nanoscale ◽  
2021 ◽  
Vol 13 (8) ◽  
pp. 4685-4686
Author(s):  
Hervé Dekkiche ◽  
Andrea Gemma ◽  
Fatemeh Tabatabaei ◽  
Andrei S. Batsanov ◽  
Thomas Niehaus ◽  
...  

Correction for ‘Electronic conductance and thermopower of single-molecule junctions of oligo(phenyleneethynylene) derivatives’ by Hervé Dekkiche et al., Nanoscale, 2020, 12, 18908–18917, DOI: 10.1039/D0NR04413J.


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