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Title: Sub-wavelength modulation of χ (2) optical nonlinearity in organic thin films

Modulating the second-order nonlinear optical susceptibility (χ (2)) of materials at the nanoscale represents an ongoing technological challenge for a variety of integrated frequency conversion and nonlinear nanophotonic applications. Here we exploit the large hyperpolarizability of intermolecular charge transfer states, naturally aligned at an organic semiconductor donor–acceptor (DA) interface, as a means to control the magnitude and sign of χ (2) at the nanoscale. Focusing initially on a single pentacene-C 60 DA interface, we confirm that the charge transfer transition is strongly aligned orthogonal to the heterojunction and find that it is responsible for a large interfacial nonlinearity probed via second harmonic generation that is sufficient to achieve d 33 > 10pm V –1, when incorporated in a non-centrosymmetric DA multilayer stack. Lastly, using grating-shadowed oblique-angle deposition to laterally structure the DA interface distribution in such multilayers subsequently enables the demonstration of a χ (2) grating with 280 nm periodicity, which is the shortest reported to date.
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  1. The Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Grant/Contract Number:
SC0012365; SC0012375
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Nature Publishing Group
Research Org:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
36 MATERIALS SCIENCE; metamaterials; nonlinear optics; surface patterning
OSTI Identifier: