Tailoring light-matter-spin interactions in colloidal hetero-nanostructures

The interplay between light and matter is the basis of many fundamental processes and various applications(1). Harnessing light-matter interactions in principle allows operation of solid state devices under new physical principles: for example, the a. c. optical Stark effect (OSE) has enabled coherent quantum control schemes of spins in semiconductors, with the potential for realizing quantum devices based on spin qubits(2-5). However, as the dimension of semiconductors is reduced, light-matter coupling is typically weakened, thus limiting applications at the nanoscale. Recent experiments have demonstrated significant enhancement of nanoscale light-matter interactions, albeit with the need for a high-finesse cavity(6,7), ultimately preventing device down-scaling and integration. Here we report that a sizable OSE can be achieved at substantial energy detuning in a cavity-free colloidal metal-semiconductor core-shell hetero-nanostructure, in which the metal surface plasmon is tuned to resonate spectrally with a semiconductor exciton transition. We further demonstrate that this resonantly enhanced OSE exhibits polarization dependence and provides a viable mechanism for coherent ultrafast spin manipulation within colloidal nanostructures. The plasmon-exciton resonant nature further enables tailoring of both OSE and spin manipulation by tuning plasmon resonance intensity and frequency. These results open a pathway for tailoring light-matter-spin interactions through plasmon-exciton resonant coupling in a judiciously engineered nanostructure, and offer a basis for future applications in quantum information processing at the nanoscale. More generally, integrated nanostructures with resonantly enhanced light-matter interactions should serve as a test bed for other emerging fields, including nano-biophotonics and nano-energy(8,9).