Electric-field control of single-molecule tautomerization

Shai Mangel; Maxim Skripnik; Katharina Polyudov; Christian Dette; Tobias Wollandt; Paul Punke; Dongzhe Li; Roberto Urcuyo; Fabian Pauly; Soon Jung Jung; Klaus Kern

doi:10.1039/c9cp06868f

Electric-field control of single-molecule tautomerization

Shai Mangel, Maxim Skripnik, Katharina Polyudov, Christian Dette, Tobias Wollandt, Paul Punke, Dongzhe Li, Roberto Urcuyo, Fabian Pauly, Soon Jung Jung, Klaus Kern

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

The electric field is an important parameter to vary in a single-molecule experiment, because it can directly affect the charge distribution around the molecule. Yet, performing such an experiment with a well-defined electric field for a model chemical reaction at an interface has proven to be extremely difficult. Here, by combining a graphene field-effect transistor and a gate-tunable scanning tunneling microscope (STM), we reveal how this strategy enables the intramolecular H atom transfer of a metal-free macrocycle to be controlled with an external field. Experiments and theory both elucidate how the energetic barrier to tautomerization decreases with increasing electric field. The consistency between the two results demonstrates the potential in using electric fields to engineer molecular switching mechanisms that are ubiquitous in nanoscale electronic devices.

Original language	English
Pages (from-to)	6370-6375
Number of pages	6
Journal	Physical Chemistry Chemical Physics
Volume	22
Issue number	11
DOIs	https://doi.org/10.1039/c9cp06868f
State	Published - 21 Mar 2020
Externally published	Yes

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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Cite this

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abstract = "The electric field is an important parameter to vary in a single-molecule experiment, because it can directly affect the charge distribution around the molecule. Yet, performing such an experiment with a well-defined electric field for a model chemical reaction at an interface has proven to be extremely difficult. Here, by combining a graphene field-effect transistor and a gate-tunable scanning tunneling microscope (STM), we reveal how this strategy enables the intramolecular H atom transfer of a metal-free macrocycle to be controlled with an external field. Experiments and theory both elucidate how the energetic barrier to tautomerization decreases with increasing electric field. The consistency between the two results demonstrates the potential in using electric fields to engineer molecular switching mechanisms that are ubiquitous in nanoscale electronic devices.",

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AU - Mangel, Shai

AU - Skripnik, Maxim

AU - Polyudov, Katharina

AU - Dette, Christian

AU - Wollandt, Tobias

AU - Punke, Paul

AU - Li, Dongzhe

AU - Urcuyo, Roberto

AU - Pauly, Fabian

AU - Jung, Soon Jung

AU - Kern, Klaus

PY - 2020/3/21

Y1 - 2020/3/21

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AB - The electric field is an important parameter to vary in a single-molecule experiment, because it can directly affect the charge distribution around the molecule. Yet, performing such an experiment with a well-defined electric field for a model chemical reaction at an interface has proven to be extremely difficult. Here, by combining a graphene field-effect transistor and a gate-tunable scanning tunneling microscope (STM), we reveal how this strategy enables the intramolecular H atom transfer of a metal-free macrocycle to be controlled with an external field. Experiments and theory both elucidate how the energetic barrier to tautomerization decreases with increasing electric field. The consistency between the two results demonstrates the potential in using electric fields to engineer molecular switching mechanisms that are ubiquitous in nanoscale electronic devices.

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Electric-field control of single-molecule tautomerization

Abstract

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