Tuning the Electronic and Magnetic Properties of Nitrogen-Functionalized Few-Layered Graphene Nanoflakes

Abstract

In this article, we report the modification of the electronic and magnetic properties of few-layered graphene (FLG) nanoflakes by nitrogen functionalization carried out using radio-frequency plasma-enhanced chemical vapor deposition (rf-PECVD) and electron cyclotron resonance (ECR) plasma processes. Even though the rf-PECVD N2 treatment led to higher N-doping levels in the FLG (4.06 atomic %) as compared to the ECR process (2.18 atomic %), the ferromagnetic behavior of the ECR FLG (118.62 × 10–4 emu/g) was significantly higher than that of the rf-PECVD FLG (0.39 × 10–4 emu/g) and pristine graphene (3.47 × 10–4 emu/g). Although both plasma processes introduce electron-donating N atoms into the graphene structure, distinct dominant nitrogen bonding configurations (pyridinic, pyrrolic) were observed for the two FLG types. Whereas the ECR plasma introduced more sp2-type nitrogen moieties, the rf-PECVD process led to the formation of sp3-coordinated nitrogen functionalities, as confirmed through Raman measurem...