Noble metals functionalized reduced graphene oxide as an efficient optical limiter: a combined experimental and theoretical investigation

Abstract

Copper, silver, and gold-reduced graphene oxide nanocomposite (Cu-rGO, Ag-rGO, and Au-rGO) were fabricated via the hydrothermal method, which shows unique physiochemical properties. Environment friendly electromagnetic radiation was employed to synthesize rGO from GO. The nonlinear optical phenomenon of noble metal decorated rGO is predominantly due to excited state absorption, which arises from surface plasmon resonance and increases in defects at the surface due to Cu, Ag, and Au incorporation. It is found that the third-order nonlinear absorption coefficient was in the order of 10⁻¹⁰ m/W, with notable enhancements in the third-order properties of Au-rGO compared to other nanocomposites and their respective counterparts. Functionalizing rGO induces defect states (sp³), increasing NLO response. Cu, Ag, and Au exhibit higher Surface-Enhanced Raman Scattering (SERS) activity due to rGO-induced structural modifications. SERS signals are influenced by dominant signals from Au nanorods. The electronic structures for pure and doped rGO were investigated through Density Functional Theory (DFT). The computed partial density of states (PDOS) confirms the enhancement of the state in Au-doped rGO is due to the charge transference from Au to C 2p orbital. The optical absorption spectra and PDOS reveal the possibility of free carrier absorption enhancement in Au which validates experimentally observed higher two-photon absorption (β) value of Au-doped rGO. The tuning of nonlinear optical and SERS behaviour with variation in the noble metal upon rGO provides an easy way to attain tuneable properties which are exceedingly required in both optoelectronics and photonics applications.