Molecular
functionalization of CNTs is a routine procedure in the
field of nanotechnology. However, whether and how these molecules
affect the spin polarization of the charge carriers in CNTs are largely
unknown. In this work we demonstrate that spin polarization can indeed
be induced in two-dimensional (2D) CNT networks by “certain”
molecules and the spin signal routinely survives length scales significantly
exceeding 1 μm. This result effectively connects the area of
molecular spintronics with that of carbon-based 2D nanoelectronics.
By using the versatility of peptide chemistry, we further demonstrate
how spin polarization depends on molecular structural features such
as chirality as well as molecule–nanotube interactions. A chirality-independent effect was detected in addition to
the more common chirality-dependent effect, and the overall spin signal
was found to be a combination of both. Finally, the magnetic field
dependence of the spin signals has been explored, and the “chirality-dependent”
signal has been found to exist only in certain field angles.