Monitoring Morphological Changes in 2D Monolayer Semiconductors Using Atom-Thick Plasmonic Nanocavities

Daniel O. Sigle, Jan Mertens, Lars O. Herrmann, Richard W. Bowman, Sandrine Ithurria, Benoit Dubertret, Yumeng Shi, Hui Ying Yang, Christos Tserkezis, Javier Aizpurua, Jeremy J. Baumberg

Research output: Contribution to journalArticlepeer-review

97 Citations (SciVal)


Nanometer-sized gaps between plasmonically coupled adjacent metal nanoparticles enclose extremely localized optical fields, which are strongly enhanced. This enables the dynamic investigation of nanoscopic amounts of material in the gap using optical interrogation. Here we use impinging light to directly tune the optical resonances inside the plasmonic nanocavity formed between single gold nanoparticles and a gold surface, filled with only yoctograms of semiconductor. The gold faces are separated by either monolayers of molybdenum disulfide (MoS2) or two-unit-cell thick cadmium selenide (CdSe) nanoplatelets. This extreme confinement produces modes with 100-fold compressed wavelength, which are exquisitely sensitive to morphology. Infrared scattering spectroscopy reveals how such nanoparticle-on-mirror modes directly trace atomic-scale changes in real time. Instabilities observed in the facets are crucial for applications such as heat-assisted magnetic recording that demand long-lifetime nanoscale plasmonic structures, but the spectral sensitivity also allows directly tracking photochemical reactions in these 2-dimensional solids.
Original languageEnglish
Pages (from-to)825-830
Number of pages6
JournalACS Nano
Issue number1
Early online date15 Dec 2014
Publication statusPublished - 27 Jan 2015


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