Efficient second harmonic generation by para-nitroaniline embedded in electro-spun polymeric nanofibres

Intense well polarized second harmonic light was generated by poly(methyl methacrylate) nanofibres with embedded para-nitroaniline nanocrystals. Subwavelength diameter fibres were electro-spun using a 1.2 weight ratio of chromophore to polymer. Analysis of the generated second harmonic light indicates that the para-nitroaniline molecules, which nominally crystalize in the centrosymmetric space group, were organized into noncentrosymmetric structures leading to a second order susceptibility dominated by a single tensor element. Under the best deposition conditions, the nanofibrers display an effective nonlinear optical susceptibility approximately two orders of magnitude greater than that of potassium dihydrogen phosphate. Generalizing this approach to a broad range of organic molecules with strong individual molecular second order nonlinear responses, but which nominally form centrosymmetric organic crystals, could open a new pathway for the fabrication of efficient sub-micron sized second harmonic light generators.Hugo Goncalves thanks the Portuguese Foundation for Science and Technology (FCT) for the support under grant PD/BD/111873/2015. The equipment used to characterize the second harmonic response of the electro-spun fibres was acquired within the framework of the Portuguese National Program for Scientific Re-equipment, contract REEQ-25/FIS/2005 with funds from POCI 2010 (FEDER) and FCT. The Raman microscope was acquired through the project nSTeP Nanostructured Systems for Tailored Performance, NORTE-07-0124-FEDER-000039, ON. 2. This work was in part developed in the scope of the projects CICECO-Aveiro Institute of Materials (UID/CTM/50011/2013), financed by national funds through the Fundacao para a Ciencia e a Tecnologia/Ministerio da Educacao e Ciencia (FCT/MEC) and co-financed by FEDER under the PT2020 Partnership Agreement. The authors are grateful to A M P Botas (University of Aveiro) for help in acquiring the hyperspectral microscopy data.