Structurally Homogeneous Hybrid Carbon Superstructures Enable Nanoscale Control of Energy, Charge, and Spin

Abstract

The rapid expansion of computationally demanding technologies, such as artificial intelligence, has created unprecedented demand for miniaturized, lightweight, high performance, and low-power electronic systems. Such technologies increasingly rely on electrical architectures capable of precisely controlling particles and quasiparticles that bear energy, charge, and spin at the nanoscale. Rigorous nanoscale control of such carriers, and their dynamic trajectories, however, is fundamentally hindered by quantum uncertainty, tunneling phenomena, and scattering processes that randomize transport and induce decoherence. This dissertation presents structurally homogeneous and electronically tunable hybrid carbon superstructures based on (i) single walled carbon nanotubes (SWNTs) and (ii) twisted multilayer graphene (tMLG), as next-generation platforms for controlling energy, charge, and spin at the nanoscale. Specifically, this work explores (i) the use of polymer wrapped SWNTs as light harvesting systems: unveiling previously unresolved excited state reaction trajectories involving multibody mediated charge transfer reactions and defect-localized trap states, (ii) the development of SWNT inks to fabricate semiconducting channels in thin film transistors: displaying compatibility with green, printing-based fabrication and exhibiting high on/off ratios with large on- currents, and (iii) the generation of highly homogeneous and morphologically controlled SWNTs and tMLG as conductive quantum phase-coherent spin channels: demonstrating long coherence lengths and molecularly tunable quantum interference phenomena.