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Protein sensing beyond the Debye Length Using Graphene Field-effect Transistors
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.ORCID iD: 0000-0003-3843-7198
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
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2018 (English)In: IEEE Sensors Journal, ISSN 1530-437X, E-ISSN 1558-1748, Vol. 18, no 16, p. 6497-6503Article in journal (Refereed) Published
Abstract [en]

Sensing biomolecules in electrolytes of high ionic strength has been a difficult challenge for field-effect transistor-based sensors. Here, we present a graphene-based transistor sensor that is capable of detection of antibodies against protein p53 in electrolytes of physiological ionic strength without dilution. As these molecules are much larger than the Debye screening length at physiological ionic strengths, this paper proves the concept of detection beyond the Debye length. The measured signal associated with the expected specific binding of the antibodies to p53 is concluded to result from resistance changes at the graphene-electrolyte interface, since a sensor responding to resistance changes rather than charge variations is not limited by Debye screening. The conclusion with changes in interface resistance as the underlying phenomena that lead to the observed signal is validated by impedance spectroscopy, which indeed shows an increase of the total impedance in proportion to the amounts of bound antibodies. This finding opens up a new route for electrical detection of large-size and even neutral biomolecules for biomedical detection applications with miniaturized sensors.

Place, publisher, year, edition, pages
Institute of Electrical and Electronics Engineers (IEEE), 2018. Vol. 18, no 16, p. 6497-6503
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering
Research subject
Engineering Science with specialization in Electronics
Identifiers
URN: urn:nbn:se:uu:diva-317088DOI: 10.1109/JSEN.2018.2849006ISI: 000439966100003OAI: oai:DiVA.org:uu-317088DiVA, id: diva2:1080394
Funder
Knut and Alice Wallenberg Foundation, 2011.0113 2011.0082Swedish Foundation for Strategic Research , SE13-0061Swedish Research Council, 2014-5591 2014-5588Available from: 2017-03-10 Created: 2017-03-10 Last updated: 2018-11-12Bibliographically approved
In thesis
1. On the Road to Graphene Biosensors
Open this publication in new window or tab >>On the Road to Graphene Biosensors
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Biosensors are devices that detect biological elements and then transmit a readable signal. Biosensors can automatize diagnostics that would otherwise have to be performed by a physician or perhaps not be possible to perform at all. Current biosensors are however either limited to particular diseases or prohibitively expensive. In order to further the field, sensors capable of many parallel measurements at a lower cost need to be developed. Field effect transistor (FET) based sensors are possible candidates for delivering this, mainly by allowing miniaturization. Smaller sensors could be cheaper, and enable parallel measurements.

Graphene is an interesting material to use as the channel of FET-sensors. The low electrochemical reactivity of its plane makes it possible to have graphene in direct contact with the sample liquid, which enhances the signal from impedance changes. Graphene-FET based impedance sensors should be able to sense almost all possible analytes and allow for scaling without losing sensitivity.

In this work the steps needed to make graphene based biosensors are presented. An improved graphene transfer is described which by using low pressure to dry the graphene removes most contamination. A method to measure the contamination of graphene by surface enhanced Raman scattering is presented. Methods to produce double gated and electrolyte gated graphene transistors on a large scale in an entirely photolithographic process are detailed. The deposition of 1-pyrenebutyric acid (PBA) on graphene is studied. It is shown that at high surface concentrations the PBA stands up on graphene and forms a dense self-assembled monolayer. A new process of using Raman spectroscopy data to quantify adsorbents was developed in order to quantify the molecule adsorption. Biosensing has been performed in two different ways. Graphene FETs have been used to read the signal generated by a streaming potential setup. Using FETs in this context enables a more sensitive readout than what would be possible without them. Graphene FETs have been used to directly sense antibodies in high ionic strength. This sensing was done by measuring the impedance of the interface between the FET and the electrolyte.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2017. p. 68
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1488
Keywords
Graphene, Biosensors, Microprocessing, Photolithography, Surface Physics, Raman Spectroscopy, Transistors
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering
Research subject
Engineering Science with specialization in Electronics
Identifiers
urn:nbn:se:uu:diva-317092 (URN)978-91-554-9845-0 (ISBN)
Public defence
2017-04-28, Polhemssalen/10134, Ångströmslaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:00 (English)
Opponent
Supervisors
Funder
Knut and Alice Wallenberg Foundation, 2011.0113Swedish Research Council, VR, No.621-2014-5591
Available from: 2017-04-07 Created: 2017-03-10 Last updated: 2017-04-21

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Hinnemo, MalkolmMakaraviciute, AstaAhlberg, PatrikOlsson, JörgenZhang, ZhenZhang, Shi-LiZhang, Zhi-Bin

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