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Asymmetric dye-filled carbon nanotubes for nonlinear optics

Cambré, Sofie (University of Antwerp, Antwerp, BEL); Campo, Jochen (University of Antwerp, Antwerp, BEL); Van Bezouw, Stein (University of Antwerp, Antwerp, BEL); Van Werveke, wouter (University of Antwerp, Antwerp, BEL); Beirnaert, Charlie (University of Antwerp, Antwerp, BEL); C. Verlackt, Christof (University of Antwerp, Antwerp, BEL); Cool, Pegie (University of Antwerp, Antwerp, BEL); Wenseleers, Wim (University of Antwerp, Antwerp, BEL)

Asymmetric dipolar molecules with a large second-order nonlinear optical (NLO) response, find applications in ultrafast electro-optic switches and in wavelength conversion of lasers.1 In 3D bulk materials, however, such dipolar molecules tend to align in a pairwise anti-parallel way, thus cancelling each other’s NLO responses. Here we show that by encapsulating such molecules in the 1D internal channel of single-wall carbon nanotubes (SWCNTs), Coulomb interactions naturally favor a polar head-to-tail alignment, leading to a coherent addition of their second-order NLO responses.2 Fluorescence-excitation3 and resonance Raman4 experiments evidence the dye-encapsulation. Wavelength-dependent hyper-Rayleigh scattering5,6 experiments effectively show that these organic-SWCNT nanohybrids possess giant NLO responses (~50-70 identically aligned dyes). Their equally giant dipole moment and size promises a stable alignment in a polymer film, opening an entirely new route to the rational design of solution-processible yet stable NLO materials. This work has received funding from the ERC under Horizon 2020 (679841: ORDERin1D) and the FWOVlaanderen.

[1] E. Goovaerts et al. In Handbook of advanced electronic and photonic Materials and Devices, Vol. 9: Nonlinear optical materials, Academic Press, San Diego 2001, 127-191.

[2] S. Cambré et al., Nature Nanotechnol. 2015, 10, 248

[3] S. Cambré et al., ACS nano 2012, 6 ,2649.

[4] W. Wenseleers et al., Adv. Mater. 2007, 19, 2274.

[5] J. Campo et al., Optics Expr. 2009, 17, 4587. [6] J. Campo et al., J. Phys. Chem. Lett . 2012, 3, 2248.

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