Conspectus
Organic semiconductors (OSCs) offer unique advantages
with respect
to mechanical flexibility, low-cost processing, and tunable properties.
The optical and electrical properties of devices based on OSCs can
be greatly improved when an OSC is coupled with graphene in a certain
manner. Our research group has focused on using graphene as a growth
template for OSCs and incorporating such high-quality heterostructures
into optoelectronic devices. The idea is that graphene’s atomically
flat surface with a uniform sp2 carbon network can serve
as a perfect quasi-epitaxial template for the growth of OSCs. In addition,
OSC–graphene heterostructures benefit from graphene’s
unique characteristics, such as its high charge-carrier mobility,
excellent optical transparency, and fascinating mechanical durability
and flexibility.
However, we have often found that OSC molecules
assemble on graphene
in unpredictable manners that vary from batch to batch. From observations
of numerous research systems, we elucidated the mechanism underlying
such poor repeatability and set out a framework to actually control
the template effect of graphene on OSCs. In this Account, we not only
present our scientific findings in this spectrum of areas but also
convey our research scheme to the readers so that similar heterostructure
complexes can be systematically studied.
We began with experiments
showing that the growth of OSCs on a
graphene surface was driven by van der Waals interactions and is therefore
sensitive to the cleanliness of the graphene surface. Nonetheless,
we noted that, even on similarly clean graphene surfaces, the OSC
thin film still varied with the underlying substrate. Thanks to the
graphene-transfer method and in situ gating methods that we developed,
we discovered that the decisive parameter for molecule–graphene
interaction (and, hence, for the growth of OSCs on graphene) is the
charge density in the graphene. Thus, to prepare a graphene template
for high-quality graphene–OSC heterostructures, we controlled
the charge density in the graphene to minimize the molecule–graphene
interaction. Moreover, the possible charge transfer between OSC molecules
and graphene, which induces additional molecule–graphene interactions,
should also be taken into account. Eventually, we demonstrated a wide
range of optoelectronic applications that benefitted from high-quality
OSC–graphene heterostructures fabricated using our proof-of-concept
systems.