Designing Hybrids of Graphene Oxide and Gold Nanoparticles for Nonlinear Optical Response

Nonlinear optical absorption of light by materials is weak due to its perturbative nature, although a strong nonlinear response is of crucial importance to applications in optical limiting and switching. Here we demonstrate experimentally and theoretically an extremely efficient scheme of excited-state absorption by charge transfer between donor and acceptor materials as a method to enhance the nonlinear absorption by orders of magnitude. With this idea, we demonstrate a strong excited-state absorption (ESA) in reduced graphene oxide that otherwise shows an increased transparency at high fluence and enhancement of ESA by one order of magnitude in graphene oxide by attaching gold nanoparticles (Au NP) in the tandem configuration that acts as an efficient charge-transfer pair when excited at the plasmonic wavelength. To explain the unprecedented enhancement, we develop a five-level rate-equation model based on the charge transfer between the two materials and numerically simulate the results. To understand the correlation of interfacial charge transfer with the concentration and type of the functional ligands attached to the graphene oxide sheet, we investigate the Au-NP-graphene oxide interface with various possible ligand configurations from first-principles calculations. By using the strong ESA of our hybrid materials, we fabricate liquid cell-based high-performance optical limiters with important device parameters better than that of the benchmark optical limiters.