Abstract
The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters. The ultrafast optical dynamics of such hybrid plasmon–emitter systems have rarely been explored. Here, we study those dynamics by interferometrically probing nonlinear optical emission from individual porous gold nanosponges infiltrated with zinc oxide (ZnO) emitters. Few-femtosecond time-resolved photoelectron emission microscopy reveals multiple long-lived localized plasmonic hot spot modes, at the surface of the randomly disordered nanosponges, that are resonant in a broad spectral range. The locally enhanced plasmonic near-field couples to the ZnO excitons, enhancing sum-frequency generation from individual hot spots and boosting resonant excitonic emission. The quantum pathways of the coupling are uncovered from a two-dimensional spectrum correlating fundamental plasmonic excitations to nonlinearly driven excitonic emissions. Our results offer new opportunities for enhancing and coherently controlling optical nonlinearities by exploiting nonlinear plasmon-quantum emitter coupling.
Highlights
The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters
Many studies have been performed on various combinations of plasmonic nanoantennas and semiconductors in the frequency domain, considerably less is known about their ultrafast optical dynamics
We show that the coupling between plasmonic hot spot fields and excitonic quantum emitters, via SF quantum channels, boosts nonlinear excitonic emission from zinc oxide (ZnO)
Summary
The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters. The enhancement of nonlinear emission often results from the coupling of fundamental plasmonic fields to higher-energy, electronic[7] or excitonic[9,14,15] transitions of quantum emitters. Many studies have been performed on various combinations of plasmonic nanoantennas and semiconductors in the frequency domain, considerably less is known about their ultrafast optical dynamics Accessing such dynamics is important to understand the microscopic origin of the coupling and the mechanism of nonlinear signal enhancement, and necessary for full coherent control of coupled nanosystems[3]. The results are valuable for improving and controlling optical nonlinearity via nonlinear plasmon–quantum emitter coupling[20]
Sign-in/Register to view highlights & summary Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
