| Abstract: | A distant-neighbor quantum-mechanical method is used to study the nonlinear optical wave mixing in graphene nanoflakes(GNFs),including sum-and difference-frequency generation,as well as four-wave mixing.Our analysis shows that molecular-scale GNFs support quantum plasmons in the visible spectrum region,and significant enhancement of nonlinear optical wave mixing is achieved.Specifically,the second-and third-order wave-mixing polarizabilities of GNFs are dramatically enhanced,provided that one(or more) of the input or output frequencies coincide with a quantum plasmon resonance.Moreover,by embedding a cavity into hexagonal GNFs,we show that one can break the structural inversion symmetry and enable otherwise forbidden second-order wave mixing,which is found to be enhanced by the quantum plasmon resonance too.This study reveals that the molecular-sized graphene could be used in the quantum regime for nanoscale nonlinear optical devices and ultrasensitive molecular sensors. |
