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2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim (1 of 7) 1400378 wileyonlinelibrary.com
Formation of Air Stable Graphene p–n–p Junctions Using
an Amine-Containing Polymer Coating
Hossein Sojoudi, Jose Baltazar, Laren Tolbert, Clifford Henderson, and Samuel Graham*
Dr. H. Sojoudi, Prof. S. Graham
Woodruff School of Mechanical Engineering
Georgia Institute of Technology
Atlanta, Georgia 30332, USA
E-mail: sgraham@gatech.edu
Dr. J. Baltazar, Prof. C. Henderson
School of Chemical & Biomolecular Engineering
Georgia Institute of Technology
Atlanta, Georgia 30332, USA
Prof. L. Tolbert
School of Chemistry & Biochemistry
Georgia Institute of Technology
Atlanta, Georgia 30332, USA
DOI: 10.1002/admi.201400378
of graphene junctions have used multiple
electrostatic gates,
[7,8]
electrical stress-
induced doping,
[9]
chemical treatment by
gas exposure,
[10]
molecular modifications
on top of the graphene,
[11–13]
ionic liquid
gating,
[14]
local doping by focused laser
irradiation
[15]
and deep UV radiation,
[16]
and modification of the substrate by
changing the local electrostatic potential
in the vicinity of one of the contacts.
[17,18]
However, these methods might not be
stable and can degrade carrier mobility by
introducing defects. A low-temperature
method was recently developed to fabri-
cate junctions in graphene by modifying
the interface between graphene and its
support substrate with covalently bonded
self-assembled monolayers (SAMs).
[19,20]
P- and n-type SAMs were patterned on
a field effect transistor (FET) device, resulting in thermally
stable graphene junctions while minimizing the introduction of
defects.
[19,20]
However, these junctions are not stable upon expo-
sure to air requiring hermetic packaging and multiple lithog-
raphy steps to pattern a graphene FET channel.
Here, we utilize an ultrathin layer of a polymer containing
simple aliphatic amine groups, polyethylenimine ethoxylated
(PEIE), on a back-gated FET device to obtain graphene p–n–p
junctions. Recently, PEIE was employed as a universal method
to lower the work function (WF) of conductors including metals,
transparent conductive metal oxides, conducting polymers, and
graphene.
[21]
Amine-terminated compounds were shown to be
effective molecules to control doping in graphene films.
[19,20]
In
contrast to π-conjugated amine-containing small molecules and
polymers, PEIE is an insulator, and it should not be regarded
as a charge injection layer but rather as a surface modifier. The
intrinsic molecular dipole moments associated with the neu-
tral amine groups contained in such an insulating polymer
layer, and the charge-transfer character of their interaction with
the conductor surface, together reduce the WF of graphene.
[21]
In contrast, gold, a well-known electron acceptor,
[22]
results in
p-doping of graphene. Charge transfer at a metal–graphene
interface results in doping of the graphene sheet due to differ-
ences in the WFs.
[23–27]
In physisorption interfaces such as those
in graphene/gold contact, Fermi level pinning and Pauli-exclu-
sion-induced energy-level shifts are shown to be two primary fac-
tors determining graphene’s doping types and densities.
[17,28–30]
Thus, adding a layer of PEIE on a back-gated graphene FET
device with gold contacts results in formation of graphene
regions with n- and p-type characteristics on a single FET device.
An ultrathin layer of a polymer containing simple aliphatic amine groups,
polyethylenimine ethoxylated (PEIE), is deposited on a back-gated field effect
graphene device to form graphene p–n–p junctions. Characteristic I–V curves
indicate the superposition of two separate Dirac points, which confirms an
energy separation of neutrality points within the complementary regions. This
is a simple approach for making graphene p–n–p junctions without a need
for multiple lithography steps or electrostatic gates and, unlike, the destruc-
tive techniques such as substitutional doping or covalent functionalization, it
induces a minor defect, if any, as there is no discernible D peak in the Raman
spectra of the graphene films after creating junctions and degradation in the
charge carrier mobilities of the graphene devices. This method can be easily
processed from dilute solutions in environmentally-friendly solvents such as
water or methoxyethanol and does not suffer any change upon exposure to
air or heating at temperatures below 100 °C.
1. Introduction
Graphene has many unique electrical properties, including
its nearly linear energy dispersion relation, which results in
electric-field-induced generation of electrons and holes in the
material. These electrons theoretically travel as massless Dirac
fermions with very high velocities.
[1–5]
Due to the zero-gap in
single-layer graphene, both carrier type and concentration can
be controlled through an electrostatic gate, making graphene
a promising material for semiconductor applications.
[1,3]
Gra-
phene junctions in which exciting phenomena such as Klein
tunneling
[6]
and fractional quantum Hall transport
[7]
have been
studied and observed, can be formed using this electrostatic
gating. Most of the studies reported so far on the formation
Adv. Mater. Interfaces 2014, 1400378
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