Chemical Vapor Deposition Mechanism of Graphene-Encapsulated Au Nanoparticle Heterostructures and Their Plasmonics

Direct encapsulation of graphene shells on noble metal nanoparticles via chemical vapor deposition (CVD) has been recently reported as a unique way to design and fabricate new plasmonic heterostructures. But currently, the fundamental nature of the growth mechanism of graphene layers on metal nanostructures is still unknown. Herein, we report a systematic investigation on the CVD growth of graphene-encapsulated Au nanoparticles (Au PG) by combining an experimental parameter study and theoretical modeling. We studied the effect of growth temperature, duration, hydrocarbon precursor concentration, and extent of reducing (H 2 ) environment on the morphology of the products. In addition, the influence of plasma oxidation conditions for the surface oxidation of gold nanoparticles on the graphene shell growth is evaluated in combination with thermodynamic calculations. We find that these parameters critically aid in the evolution of graphene shells around gold nanoparticles and allow for controlling shell thickness, graphene shell quality and morphology, and hybrid nanoparticle diameter. An optimized condition including the growth temperature of similar to 675 degrees C, duration of 30 min, and xylene feed rate of similar to 10 mL/h with 10% H-2/Ar carrier gas was finally obtained for the best morphology evolution. We further performed finite-element analysis (FEA) simulations to understand the equivalent von Mises stress distribution and discrete dipolar approximation (DDA) calculation to reveal the optical properties of such new core-shell heterostructures. This study brings new insight to the nature of CVD mechanism of Au@G and might help guiding their controlled growth and future design and application in plasmonic applications.

Automated summary

This study investigates the CVD growth of graphene-encapsulated Au nanoparticles (Au PG) through experimental parameter studies and theoretical modeling to understand the growth mechanism and control the morphology evolution. Optimized conditions for the best morphology evolution are identified, providing new insights for the design and application of such core-shell heterostructures in plasmonic applications.