Quantum plasmon enhanced nonlinear wave mixing in graphene nanoflakes

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.

Highly efficient continuous-wave mid-infrared generation based on intracavity difference frequency mixing

We report on a new scheme for efficient continuous-wave(CW)mid-infrared generation using difference frequency generation(DFG)inside a periodically poled lithium niobate(PPLN)-based optical parametric oscillator(OPO).The pump sources were two CW fiber lasers fixed at 1018 nm and 1080 nm.One worked as the assisted laser to build parametric oscillation and generate an oscillating signal beam while the other worked at low power(3 W)to induce DFG between it and the signal beam.The PPLN temperature was appropriately adjusted to enable OPO and DFG to synchronously meet phase-matching conditions.Finally,both low-power 1018 nm and 1080 nm pump beams were successfully converted to 3.1μm and 3.7μm idler beams,respectively.The conversion efficiencies of the 1018 nm and 1080 nm pumped DFG reached 20% and 15%,respectively,while their slope efficiencies reached 19.6% and 15%.All these data were comparable to the OPOs pumped by themselves and never realized before in traditional CW DFG schemes.The results reveal that high-efficiency frequency down-conversion can be achieved with a low-power nearinfrared pump source.