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The donor-acceptor interaction of a charge-coupled heterostructureencompassing a metal and an amorphous semiconductor subjected to a laser fieldhas many potential applications in the realm of nonlinear optics. In this work,we fabricate an electron donor gold nanoparticle (AuNP) and acceptor amorphousGe24Se76 heterostructure on a quartz substrate using a sequential thermalevaporation technique. In this charge-coupled heterostructure, we demonstratethe ultrafast third-order nonlinear absorptive and refractive response andtheir sign reversal compared to pristine Ge24Se76. Enhanced opticalnonlinearity in these heterostructures of varying plasmonic wavelengths is dueto charge transfer, verified by the Raman spectroscopy. Further, the ultrafasttransient absorption measurements support the thesis of charge transfer in theAuNP/Ge24Se76 heterostructure. These findings open up exciting opportunitiesfor developing novel device technologies with far-reaching applications innonlinear optics.

Ultrafast Third-Order Nonlinear Optical Response of Charge Coupled Gold Nanoparticle-Ge24Se76 Heterostructure