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NANO MICRO
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2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Functionalized Graphdiyne Nanowires: On-Surface
Synthesis and Assessment of Band Structure, Flexibility,
and Information Storage Potential
Florian Klappenberger,* Raphael Hellwig, Ping Du, Tobias Paintner, Martin Uphoff,
Liding Zhang, Tao Lin, Bahare Abedin Moghanaki, Mateusz Paszkiewicz, Ivana Vobornik,
Jun Fujii, Olaf Fuhr, Yi-Qi Zhang, Francesco Allegretti, Mario Ruben, and Johannes V. Barth
DOI: 10.1002/smll.201704321
(CNTs),
[1]
graphene sheets,
[2]
and gra-
phene nanoribbons.
[3,4]
Recently, sig-
nificant interest in their graphyne and
graphdiyne-related counterparts incorpo-
rating both sp
2
- and sp-hybridized carbon
atoms is quickly emerging.
[5–8]
Notably,
theoretical investigations predict prom-
ising characteristics suitable for a broad
variety of applications including molecular
electronics, energy storage, gas filtering,
and light harvesting.
[9–13]
However, the
experimental realization of the targeted
materials remains challenging and, so
far, solution-based synthesis approaches
only afforded multilayered materials with
significant amounts of impurities and
unknown structural properties.
[14]
Various routes to the fabrication of
high-quality carbon materials are cur-
rently being investigated,
[15]
of which the
epitaxial growth on well-defined metal
substrates under ultrahigh vacuum (UHV)
conditions is considered one of the most
promising. Combining it with the cova-
lent on-surface synthesis from rationally
designed organic precursors
[16]
paved the
way to the engineering of stable
[17]
and
atom-precise nanostructures,
[18]
amongst
them various types of conjugated polymer wires
[19–21]
and gra-
phene nanoribbons.
[4,18,22,23]
In this context, the homocoupling reaction of terminal
alkyne tectons has raised great hopes for the construction of
graphdiyne-related nanostructures.
[8,24,25]
However, the intricate
Carbon nanomaterials exhibit extraordinary mechanical and electronic proper-
ties desirable for future technologies. Beyond the popular sp
2
-scaffolds, there
is growing interest in their graphdiyne-related counterparts incorporating both
sp
2
and sp bonding in a regular scheme. Herein, we introduce carbonitrile-
functionalized graphdiyne nanowires, as a novel conjugated, one-dimensional
(1D) carbon nanomaterial systematically combining the virtues of covalent
coupling and supramolecular concepts that are fabricated by on-surface
synthesis. Specifically, a terphenylene backbone is extended with reactive
terminal alkyne and polar carbonitrile (CN) moieties providing the required
functionalities. It is demonstrated that the CN functionalization enables highly
selective alkyne homocoupling forming polymer strands and gives rise to
mutual lateral attraction entailing room-temperature stable double-stranded
assemblies. By exploiting the templating effect of the vicinal Ag(455) surface,
40 nm long semiconducting nanowires are obtained and the first experimental
assessment of their electronic band structure is achieved by angle-resolved
photoemission spectroscopy indicating an effective mass below 0.1m
0
for the
top of the highest occupied band. Via molecular manipulation it is showcased
that the novel oligomer exhibits extreme mechanical flexibility and opens
unexplored ways of information encoding in clearly distinguishable CN-phenyl
trans–cis species. Thus, conformational data storage with density of
0.36 bit nm
-2
and temperature stability beyond 150 K comes in reach.
Carbon Materials
Dr. F. Klappenberger, Dr. R. Hellwig, T. Paintner, M. Uphoff, L. Zhang,
Dr. T. Lin, B. Abedin Moghanaki, M. Paszkiewicz, Dr. Y.-Q. Zhang,
Dr. F. Allegretti, Prof. J. V. Barth
Physik-Department E20
Technische Universität München
85748 Garching, Germany
E-mail: florian.klappenberger@tum.de
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/smll.201704321.
Dr. P. Du, Dr. O. Fuhr, Prof. M. Ruben
Institute für Nanotechnologie
Karlsruher Institut für Technologie (KIT)
76344 Eggenstein-Leopoldshafen, Germany
Dr. I. Vobornik, Dr. J. Fujii
Istituto Officina dei Materiali (IOM)-CNR
Laboratorio TASC
Area Science Park, I-34149 Trieste, Italy
Prof. M. Ruben
IPCMS-CNRS
Université de Strasbourg
F-67034 Strasbourg, France
Carbon-based materials exhibit extraordinary mechanical and
electronic properties. They are a central research topic in the
21st century and promising candidates for future nanotech-
nology applications. A plethora of nanomaterials is based on
established sp
2
-hybridized scaffolds such as carbon nanotubes
Small 2018, 14, 1704321