Controlled synthetic chirality in macroscopic assemblies of carbon nanotubes

TL;DR

This paper presents two simple, scalable methods to create wafer-scale chiral carbon nanotube assemblies with tunable and record-high circular dichroism, enabling new opportunities in chiral photonics and electronics.

Contribution

It introduces straightforward fabrication techniques for macroscopic chiral CNT structures with controllable handedness and giant optical activity, without complex nanofabrication.

Findings

Achieved record-high deep-ultraviolet ellipticity of 40 mdeg/nm.

Theoretical simulations predict ellipticity up to 150 mdeg/nm with optimized thickness.

Created wafer-scale chiral CNT assemblies with tunable optical properties.

Abstract

There is an emerging recognition that successful utilization of chiral degrees of freedom can bring new scientific and technological opportunities to diverse research areas. Hence, methods are being sought for creating artificial matter with controllable chirality in an uncomplicated and reproducible manner. Here, we report the development of two straightforward methods for fabricating wafer-scale chiral architectures of ordered carbon nanotubes (CNTs) with tunable and giant circular dichroism (CD). Both methods employ simple approaches, (i) mechanical rotation and (ii) twist-stacking, based on controlled vacuum filtration and do not involve any sophisticated nanofabrication processes. We used a racemic mixture of CNTs as the starting material, so the intrinsic chirality of chiral CNTs is not responsible for the observed chirality. In particular, by controlling the stacking angle and handedness in (ii), we were able to maximize the CD response and achieve a record-high deep-ultraviolet ellipticity of 40 $\pm$ 1 mdeg/nm. Our theoretical simulations using the transfer matrix method reproduce the salient features of the experimentally observed CD spectra and further predict that a film of twist-stacked CNTs with an optimized thickness will exhibit an ellipticity as high as 150 mdeg/nm. The created wafer-scale objects represent a new class of synthetic chiral matter consisting of ordered quantum wires whose macroscopic properties are governed by nanoscopic electronic signatures such as van Hove singularities. These artificial structures with engineered chirality will not only provide playgrounds for uncovering new chiral phenomena but also open up new opportunities for developing high-performance chiral photonic and optoelectronic devices.