Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions

Understanding the mechanisms of charge transport (CT) across biomolecules in solid-state devices is imperative to realize biomolecular electronic devices in a predictive manner. Although it is well-accepted that biomolecule-electrode interactions play an essential role, it is often overlooked. This...

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Main Authors: Gupta, Nipun Kumar, Karuppannan, Senthil Kumar, Pasula, Rupali Reddy, Vilan, Ayelet, Martin, Jens, Xu, Wentao, May, Esther Maria, Pike, Andrew R., Astier, Hippolyte P. A. G., Salim, Teddy, Lim, Sierin, Nijhuis, Christian A.
Other Authors: School of Chemical and Biomedical Engineering
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/168625
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Institution: Nanyang Technological University
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spelling sg-ntu-dr.10356-1686252023-12-29T06:52:51Z Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions Gupta, Nipun Kumar Karuppannan, Senthil Kumar Pasula, Rupali Reddy Vilan, Ayelet Martin, Jens Xu, Wentao May, Esther Maria Pike, Andrew R. Astier, Hippolyte P. A. G. Salim, Teddy Lim, Sierin Nijhuis, Christian A. School of Chemical and Biomedical Engineering Engineering::Chemical engineering Biomolecular Electronics Graphene Understanding the mechanisms of charge transport (CT) across biomolecules in solid-state devices is imperative to realize biomolecular electronic devices in a predictive manner. Although it is well-accepted that biomolecule-electrode interactions play an essential role, it is often overlooked. This paper reveals the prominent role of graphene interfaces with Fe-storing proteins in the net CT across their tunnel junctions. Here, ferritin (AfFtn-AA) is adsorbed on the graphene by noncovalent amine-graphene interactions confirmed with Raman spectroscopy. In contrast to junctions with metal electrodes, graphene has a vanishing density of states toward its intrinsic Fermi level ("Dirac point"), which increases away from the Fermi level. Therefore, the amount of charge carriers is highly sensitive to temperature and electrostatic charging (induced doping), as deduced from a detailed analysis of CT as a function of temperature and iron loading. Remarkably, the temperature dependence can be fully explained within the coherent tunneling regime due to excitation of hot carriers. Graphene is not only demonstrated as an alternative platform to study CT across biomolecular tunnel junctions, but it also opens rich possibilities in employing interface electrostatics in tuning CT behavior. Ministry of Education (MOE) Published version We acknowledge the Ministry of Education (MOE) for supporting this research under award no. MOE2019-T2-1-137. 2023-06-12T06:57:42Z 2023-06-12T06:57:42Z 2022 Journal Article Gupta, N. K., Karuppannan, S. K., Pasula, R. R., Vilan, A., Martin, J., Xu, W., May, E. M., Pike, A. R., Astier, H. P. A. G., Salim, T., Lim, S. & Nijhuis, C. A. (2022). Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions. ACS Applied Materials & Interfaces, 14(39), 44665-44675. https://dx.doi.org/10.1021/acsami.2c11263 1944-8244 https://hdl.handle.net/10356/168625 10.1021/acsami.2c11263 36148983 2-s2.0-85139367576 39 14 44665 44675 en MOE2019-T2-1-137 ACS Applied Materials & Interfaces © 2022 The Authors. Published by American Chemical Society. This is an open-access article distributed under the terms of the Creative Commons Attribution License. application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Chemical engineering
Biomolecular Electronics
Graphene
spellingShingle Engineering::Chemical engineering
Biomolecular Electronics
Graphene
Gupta, Nipun Kumar
Karuppannan, Senthil Kumar
Pasula, Rupali Reddy
Vilan, Ayelet
Martin, Jens
Xu, Wentao
May, Esther Maria
Pike, Andrew R.
Astier, Hippolyte P. A. G.
Salim, Teddy
Lim, Sierin
Nijhuis, Christian A.
Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
description Understanding the mechanisms of charge transport (CT) across biomolecules in solid-state devices is imperative to realize biomolecular electronic devices in a predictive manner. Although it is well-accepted that biomolecule-electrode interactions play an essential role, it is often overlooked. This paper reveals the prominent role of graphene interfaces with Fe-storing proteins in the net CT across their tunnel junctions. Here, ferritin (AfFtn-AA) is adsorbed on the graphene by noncovalent amine-graphene interactions confirmed with Raman spectroscopy. In contrast to junctions with metal electrodes, graphene has a vanishing density of states toward its intrinsic Fermi level ("Dirac point"), which increases away from the Fermi level. Therefore, the amount of charge carriers is highly sensitive to temperature and electrostatic charging (induced doping), as deduced from a detailed analysis of CT as a function of temperature and iron loading. Remarkably, the temperature dependence can be fully explained within the coherent tunneling regime due to excitation of hot carriers. Graphene is not only demonstrated as an alternative platform to study CT across biomolecular tunnel junctions, but it also opens rich possibilities in employing interface electrostatics in tuning CT behavior.
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Gupta, Nipun Kumar
Karuppannan, Senthil Kumar
Pasula, Rupali Reddy
Vilan, Ayelet
Martin, Jens
Xu, Wentao
May, Esther Maria
Pike, Andrew R.
Astier, Hippolyte P. A. G.
Salim, Teddy
Lim, Sierin
Nijhuis, Christian A.
format Article
author Gupta, Nipun Kumar
Karuppannan, Senthil Kumar
Pasula, Rupali Reddy
Vilan, Ayelet
Martin, Jens
Xu, Wentao
May, Esther Maria
Pike, Andrew R.
Astier, Hippolyte P. A. G.
Salim, Teddy
Lim, Sierin
Nijhuis, Christian A.
author_sort Gupta, Nipun Kumar
title Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
title_short Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
title_full Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
title_fullStr Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
title_full_unstemmed Temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
title_sort temperature-dependent coherent tunneling across graphene-ferritin biomolecular junctions
publishDate 2023
url https://hdl.handle.net/10356/168625
_version_ 1787136761381519360