title: High-Efficiency Second-Harmonic Generation from Hybrid Light-Matter States.
abstract: We report a novel approach to modify the second order nonlinear optical (NLO) susceptibility of organic nanofiber crystals by hybridization with the optical modes of microcavities in the strong coupling regime. The wavelength dependence of the SHG efficiency displays two intense peaks corresponding to the so-formed light-matter hybrid states. Our results demonstrate an enhancement of the resonant SHG efficiency of the lower polariton by 2 orders of magnitude for the collectively coupled molecules as compared to that of the same material outside the microcavity. This study is a proof of principle that opens a new direction for NLO of organic materials in subwavelength resonators.
authors.affiliation: ISIS and icFRC, University of Strasbourg and CNRS , 8 allée Gaspard Monge, 67000 Strasbourg, France.
authors.forename: Thibault
authors.initials: T
authors.lastname: Chervy
authors.affiliation: School of Chemical Engineering and Technology, Tianjin University , Yaguan Road 135, 300350 Tianjin, People's Republic of China.|Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.
authors.forename: Jialiang
authors.initials: J
authors.lastname: Xu
authors.affiliation: Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.
authors.forename: Yulong
authors.initials: Y
authors.lastname: Duan
authors.affiliation: ISIS and icFRC, University of Strasbourg and CNRS , 8 allée Gaspard Monge, 67000 Strasbourg, France.
authors.forename: Chunliang
authors.initials: C
authors.lastname: Wang
authors.affiliation: IPCMS, University of Strasbourg and CNRS , 23 rue du Loess, 67034 Strasbourg, France.
authors.forename: Loïc
authors.initials: L
authors.lastname: Mager
authors.affiliation: Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.
authors.forename: Maurice
authors.initials: M
authors.lastname: Frerejean
authors.affiliation: Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.
authors.forename: Joris A W
authors.initials: JA
authors.lastname: Münninghoff
authors.affiliation: Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.
authors.forename: Paul
authors.initials: P
authors.lastname: Tinnemans
authors.affiliation: ISIS and icFRC, University of Strasbourg and CNRS , 8 allée Gaspard Monge, 67000 Strasbourg, France.
authors.forename: James A
authors.initials: JA
authors.lastname: Hutchison
authors.affiliation: ISIS and icFRC, University of Strasbourg and CNRS , 8 allée Gaspard Monge, 67000 Strasbourg, France.
authors.forename: Cyriaque
authors.initials: C
authors.lastname: Genet
authors.affiliation: Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.|Australian Institute for Bioengineering and Nanotechnology (AIBN), The University of Queensland , Brisbane, Queensland 4072, Australia.
authors.forename: Alan E
authors.initials: AE
authors.lastname: Rowan
authors.affiliation: Institute for Molecules and Materials (IMM), Radboud University , Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.
authors.forename: Theo
authors.initials: T
authors.lastname: Rasing
authors.affiliation: ISIS and icFRC, University of Strasbourg and CNRS , 8 allée Gaspard Monge, 67000 Strasbourg, France.
authors.forename: Thomas W
authors.initials: TW
authors.lastname: Ebbesen
keywords: Second harmonic generation; cavity; polariton state; self-assembly; strong coupling