Nonlinear plasmon-exciton coupling enhances sum-frequency generation from a hybrid metal/semiconductor nanostructure

Jin Hui Zhong, Jan Vogelsang, Jue Min Yi, Dong Wang, Lukas Wittenbecher, Sara Mikaelsson, Anke Korte, Abbas Chimeh, Cord L. Arnold, Peter Schaaf, Erich Runge, Anne L’ Huillier, Anders Mikkelsen, Christoph Lienau

Research output: Contribution to journalArticlepeer-review


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.

Original languageEnglish
Article number1464
JournalNature Communications
Issue number1
Publication statusPublished - 2020

Subject classification (UKÄ)

  • Atom and Molecular Physics and Optics


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