Electrochemically Gated Single Molecule FETs

Lead Research Organisation: University of Reading
Department Name: Chemistry

Abstract

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Publications

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Domingos SR (2015) Elucidating the Structure of Chiral Molecules by using Amplified Vibrational Circular Dichroism: From Theory to Experimental Realization. in Chemphyschem : a European journal of chemical physics and physical chemistry

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Domingos SR (2014) Switchable amplification of vibrational circular dichroism as a probe of local chiral structure. in Angewandte Chemie (International ed. in English)

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Osorio HM (2015) Electrochemical Single-Molecule Transistors with Optimized Gate Coupling. in Journal of the American Chemical Society

 
Description We have contributed strongly to the development of monitoring electrochemical (redox) reactions by diverse spectroscopic methods.
We have introduced a unique device (spectroelectrochemical cell) for probing redox reactions and improving detection limits of optically active compounds of importance in the fields of pharmaceutical research, DNA research, catalysis.
We have developed novel spectroelectrochemical cells for far infrared region and for monitoring redox reactions of compounds attached (chemisorbed, self-assembled) on electrode surfaces by infrared spectroscopy at variable temperature. These method further expand the existing portfolio of spectroelectrochemical methods.
Finally, we have introduced for the first time the highly interesting medium of ionic liquids to spectroelectrochemistry. Ionic liquids have played a significant role in working on the key target of the EPSRC project - studying gated electron transfer on a molecular level using a scanning tunnelling microscope (in collaboration with Prof. Richard Nichols in Liverpool).
Exploitation Route Direct application of our newly developed experimental (spectroelectrochemical) techniques in other research projects. Inspiration by the molecular wires investigated and methodologies applied in this collaborative project (Reading/Durham/Liverpool) and/or in the new partnership with CCNU Wuhan.
Sectors Chemicals,Electronics,Environment,Pharmaceuticals and Medical Biotechnology

 
Description Global Talent Plan 111
Amount ¥1,000,000 (CNY)
Organisation Central China Normal University 
Sector Academic/University
Country China
Start 12/2016 
End 12/2021
 
Title 2D-IR spectroelectrochemistry 
Description Pioneering application of in situ spectroelectrochemistry to monitor time-resolved vibrational relaxation of optically excited molecules in different oxidation states. 
Type Of Material Technology assay or reagent 
Provided To Others? No  
Impact This pioneering technique has a potential to be widely used by numerous research groups in diverse chemistry research fields - materials chemistry, molecular electronics, biochemistry and pharmacy, electrocatalysis, etc. 
 
Title Atenuated Total Reflectance (ATR) spectroelectroelectrochemical cell for Infra-Red monitoring of redox reactions at variable temperature. 
Description The cell allows to monitor specific redox reactions of compounds attached to the surface of a gold film electrode deposited to an ATR crystal. The development of this setup was one of the major goals of the EPSRC-funded project. The fabrication proved to be much more challenging than initially thought. The prototype has recently been completed. 
Type Of Material Technology assay or reagent 
Provided To Others? No  
Impact The introduction of this spectroelectrochemical tool will have a major impact on diverse areas of fundamental and applied research, e.g., materials chemistry, catalysis, molecular electronics. It can directly support studies of gated electron transfer on a molecular level. 
 
Title Spectroelectrochemistry in Far-InfraRed (FIR) region 
Description A unique spectroelectrochemical cell has been constructed and tested within the EPSRC project, which allows to investigate redox processes (including those related to the topic of the project) in the far infrared spectral region. This method will have a big impact on diverse research areas (e.g., pharmaceutical research). At present this method is solely available in Reading. 
Type Of Material Technology assay or reagent 
Provided To Others? No  
Impact A new area of spectroelectrochemical research is open by introducing this specific tool. 
 
Title Spectroelectrochemistry in ionic liquids. 
Description Monitoring of electrochemical reactions by molecular spectroscopic methods (infrared and UV-Visible spectroscopies) without the need of using supporting electrolyte. Directly related to the activities of the EPSRC network (gated electron transfer studied in Liverpool by Prof. Richard Nichols). 
Type Of Material Technology assay or reagent 
Year Produced 2015 
Provided To Others? Yes  
Impact This is a pioneering approach with much impact expected in the coming years. 
 
Title Vibrational circular dichroism (VCD) spectroelectrochemistry 
Description The combination of VCD and electrochemistry allows for significant enhancement of VCD signals. This methods is promising for investigation of structures of optically active molecules, including biologically active compounds. 
Type Of Material Technology assay or reagent 
Year Produced 2014 
Provided To Others? Yes  
Impact "Switchable Amplification of Vibrational Circular Dichroism as a Probe of Local Chiral Structure." S. R. Domingos, H. J. Sanders, F. Hartl*, W. J. Buma and S. Woutersen, Angew. Chem. Int. Ed., accepted for publication. DOI: 10.1002/anie.201407376 and 10.1002/ange.201407376. Strongly rising interest from diverse research groups (noticed at Research Gate). 
 
Description Molecular electronics 
Organisation Central China Normal University
Country China 
Sector Academic/University 
PI Contribution Spectroelectrochemistry of diverse organometallic molecular wires.
Collaborator Contribution Synthesis, characterisation and theoretical studies of diverse organometallic molecular wires.
Impact 1. "Bridge-Localized HOMO-Binding Character of Divinylanthracene-Bridged Dinuclear Ruthenium Carbonyl Complexes: Spectroscopic, Spectroelectrochemical, and Computational Studies." Y.-P. Ou, J. Zhang, M. Xu, J. Xia, F. Hartl, J. Yin, G.-A. Yu and S.H. Liu, Chem. Asian J., 9 (2014) 1152-1160. 2. "Diruthenium Complexes with Bridging Diethynyl Polyaromatic Ligands: Synthesis, Spectroelectrochemistry and Theoretical Calculations." J. Zhang, M. Zhang, C. Sun, M. Xu, F. Hartl*, J. Yin, G. Yu, L. Rao, and S. Liu, Organometallics 34 (2015) 3967-3978. 3. "Asymmetric Oxidation of Bridging Vinyl- and Ethynyl Terthiophene Ligands in Triruthenium Complexes". J. Zhang, C.-F. Sun, M.-X. Zhang, F. Hartl*, J. Yin, G.-A. Yu, L.Rao and S.H. Li, Dalton Trans. 45 (2016) 768-782. 4. "Notable Differences between Oxidized Diruthenium Complexes Bridged by Four Isomeric Diethynyl Benzodithiophene Ligands". Y.-P. Ou, J. Zhang, F. Zhang, D. Kuang, F. Hartl*, L. Rao, S. H. Liu, Dalton Trans. 45 (2016) 6503-6516. 5. "Mononuclear Piano-Stool Iron 2-Ethynylbenzo[b]thiophene Complex: Crystal Structure and Reversible Oxidation Studied by Spectro-electrochemical and DFT Methods." Y.-P. Ou, J. Zhang, D. Kuang, F. Zhang, J. Yu, X. Zhu, S. H. Liu, F. Hartl*, J. Coord. Chem., 70 (2017) 722-733. 6. "Multistep Oxidation of Diethynyl Oligophenylamine-Bridged Diruthenium and Diiron Complexes." J. Zhang, S.-Z. Guo, Y.-B. Dong, L. Rao, J. Yin, G.-A. Yu, F. Hartl* and S. H. Liu, Inorg. Chem. 56 (2017) 1001-1015.
Start Year 2013
 
Description Molecular wires 
Organisation University of Reading
Department Department of Meteorology
Country United Kingdom 
Sector Academic/University 
PI Contribution Spectro-electrochemical investigation of new compounds envisaged as candidates for molecular wires - oligoviologen derivatives, transition metal complexes with cyanodiazenide and oxodiazolyldiazenide bridges.
Collaborator Contribution Synthesis and characterisation, including crystal structure determinations.
Impact "Efficient Access to Conjugated 4,4'-Bipyridinium Oligomers Using the Zincke Reaction: Synthesis, Spectroscopic and Electrochemical Properties." L. Chen, H. Wilcock, C.J. Wedge, F. Hartl, H. M. Colquhoun and B. W. Greenland, Org. Biomol. Chem., 14 (2016) 980-988. "Prediction of E1/2(1) and E1/2(2) Values for Viologen-containing Conjugated Unimers and Dimers from Calculated pKb Values of the Substituents." L. Chen, F. Hartl, H. M. Colquhoun and B. W. Greenland, Tetrahedron Lett., submitted.
Start Year 2014
 
Description Electronic Structure of Redox Active Linear and Cross-Conjugated Compounds for Molecular Devices 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Type Of Presentation keynote/invited speaker
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Keynote lecture at ISEMN 2014, Wuhan, China, April 18-21, 2014.

The impact of the lecture can be seen in established new links to research groups in the UK and China, which will promote collaboration and joint project activities in the future.
Year(s) Of Engagement Activity 2014
 
Description Invited keynote conference lecture at Electrochem 2014, Loughborough, September 2014 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Rich discussion after the talk. Interest in continued and new collaborations.

Continued collaboration with Molecular Photonics at the University of Amsterdam. New research activities within my new BBSRC project (Co-I).
Year(s) Of Engagement Activity 2014
 
Description Versatile Spectroelectrochemistry Serving Wide Electroanalytical Community 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Invited lecture at the 15th International Symposium of Electroanalytical Chemistry, Changchun, PR China, August 2015.
Year(s) Of Engagement Activity 2015