Carbon nanotubes (CNTs), helically wrapped with single-stranded DNA, have recently emerged as a spin-filtering material. The inversion asymmetric helical potential of DNA creates a spin-filtering effect (commonly known as “chirality-induced spin selectivity” or CISS), which polarizes carrier spins in the nanotube. Thus, tuning of the DNA–CNT interaction is expected to affect carrier spins in nanotubes. The CISS effect induces spin polarization, which is coupled with the carrier’s momentum direction, and therefore, in one-dimensional systems, such as nanotubes, momentum flip must be accompanied by a simultaneous spin flip. This spin momentum locking can have a profound impact on charge transport in nanotubes as backscattering due to phonons and disorder will be suppressed as these mechanisms are spin-independent. Here, we report DNA–CNT spin filters in which CNTs have been functionalized with two different classes of sequences, exhibiting different degrees of interaction with the CNT. They induce different degrees of spin polarization in the channel, with significant impact on temperature-dependent charge transport and interference phenomena arising from carrier backscattering. This work raises the intriguing possibility of engineering charge transport in nanotubes via CISS-induced spin polarization by tailor-made DNA sequences.

Supramolecular short-peptide assemblies have been widely used for the development of biomaterials with potential biomedical applications. These peptides can self-assemble in a multitude of chiral hierarchical structures triggered by the application of different stimuli, such as changes in temperature, pH, solvent, etc. The self-assembly process is sensitive to the chemical composition of the peptides, being affected by specific amino acid sequence, type, and chirality. The resulting supramolecular chirality of these materials has been explored to modulate protein and cell interactions. Recently, significant attention has been focused on the development of chiral materials with potential spintronic applications, as it has been shown that transport of charge carriers through a chiral environment polarizes the carrier spins. This effect, named chiralityinduced spin selectivity or CISS, has been studied in different chiral organic molecules and materials, as well as carbon nanotubes functionalized with chiral molecules. Nevertheless, this effect has been primarily explored in homochiral systems in which the chirality of the medium, and hence the resulting spin polarization, is defined by the chirality of the molecule, with limited options for tunability. Herein, we have developed heterochiral carbon-nanotube−shortpeptide materials made by the combination of two different chiral sources: that is, homochiral peptides (L/D) + glucono-δlactone. We show that the presence of a small amount of glucono-δ-lactone with fixed chirality can alter the supramolecular chirality of the medium, thereby modulating the sign of the spin signal from "up" to "down" and vice versa. In addition, small amounts of glucono-δ-lactone can even induce nonzero spin polarization in an otherwise achiral and spin-inactive peptide− nanotube composite. Such "chiral doping" strategies could allow the development of complementary CISS-based spintronic devices and circuits on a single material platform.

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.

Helical molecules such as DNA have recently been found to behave as an efficient source and detector of spin-polarized charge carriers. This phenomenon, often dubbed as chirality-induced spin selectivity or CISS, could be used to significantly improve the performance of spintronic devices, which utilize carrier spins (rather than charge) to realize electronic and sensing functions. Recently, it has been reported that carbon nanotubes, helically wrapped with DNA, can also act as an efficient source and detector of spin-polarized carriers, by virtue of spin–orbit coupling originating from the helical potential. It has been postulated that spin polarization should increase with the length of the wrapped tubes. However, in literature, most fabrication processes yield tubes with submicron lengths, which can produce ∼70% spin polarization. In an effort to enhance this effect further, here, we report a fabrication process that can yield DNA-wrapped nanotubes of length ∼1–4 microns. Detailed characterization of these devices, using atomic force microscopy, Raman, UV–vis, and temperature-dependent transport, has been presented. Initial transport measurements indicate the presence of strong magnetoresistance in these tubes, which could be attributed to spin-dependent effects. Systematic fabrication of long DNA-wrapped nanotubes, which has hitherto not been reported, is expected to enable further investigation into the spin-dependent properties of these ultimate one-dimensional nanoscale hybrids and may have a significant impact on nanoscale spintronics.

Helical functionalization of carbon nanotubes using DNA strands can polarize carrier spins through chirality induced spin selectivity (or CISS) effect. Detection of this effect using transport experiments unravels an underlying magnetoresistance effect, origin of which is not well understood. In the present study, we investigate this effect, a fundamental understanding of which is crucial for the potential use of this system in spintronic devices. The conduction mechanism has been found to be in the strongly localized regime due to DNA functionalization, with the observed magnetoresistance originating from the interference effects between the forward and backward hopping paths. CISS-induced spin polarization has been estimated to increase the carrier localization length by an order of magnitude in the low temperature range and it affects the magnetoresistance effect in a non-trivial way that is not observed in conventional systems.