
1.College of Advanced Interdisciplinary Studies, National University of Defense Technology, 410073 Changsha, China
2.Key Laboratory of Micro- and Nano-Photonic Structures (Ministry of Education), and State Key Laboratory of Surface Physics, Department of Physics, Fudan University, 200433 Shanghai, China
3.State Key Laboratory of High Performance Computing, College of Computer, National University of Defense Technology, 410073 Changsha, China
4.Beijing Institute for Advanced Study, National University of Defense Technology, 100000 Beijing, China
Lei Shi (lshi@fudan.edu.cn)
Tian Jiang (tjiang@nudt.edu.cn)
Published:31 May 2022,
Published Online:14 April 2022,
Received:13 December 2021,
Revised:24 February 2022,
Accepted:25 February 2022
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Tang, Y. X. et al. Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor. Light: Science & Applications, 11, 877-887 (2022).
Tang, Y. X. et al. Interacting plexcitons for designed ultrafast optical nonlinearity in a monolayer semiconductor. Light: Science & Applications, 11, 877-887 (2022). DOI: 10.1038/s41377-022-00754-3.
Searching for ideal materials with strong effective optical nonlinear responses is a long-term task enabling remarkable breakthroughs in contemporary quantum
and nonlinear optics. Polaritons
hybridized light-matter quasiparticles
are an appealing candidate to realize such nonlinearities. Here
we explore a class of peculiar polaritons
named plasmon–exciton polaritons (plexcitons)
in a hybrid system composed of silver nanodisk arrays and monolayer tungsten-disulfide (WS
2
)
which shows giant room-temperature nonlinearity due to their deep-subwavelength localized nature. Specifically
comprehensive ultrafast pump–probe measurements reveal that plexciton nonlinearity is dominated by the saturation and higher-order excitation-induced dephasing interactions
rather than the well-known exchange interaction in traditional microcavity polaritons. Furthermore
we demonstrate this giant nonlinearity can be exploited to manipulate the ultrafast nonlinear absorption properties of the solid-state system. Our findings suggest that plexcitons are intrinsically strongly interacting
thereby pioneering new horizons for practical implementations such as energy-efficient ultrafast all-optical switching and information processing.
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