Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms14269
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Funding
- Air Force Office of Scientific Research Young Investigator Program [FA-9550-14-1-0301]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0012365]
- U.S. Department of Energy [DE-SC0012375]
- U.S. Department of Energy (DOE) [DE-SC0012365, DE-SC0012375] Funding Source: U.S. Department of Energy (DOE)
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Modulating the second-order nonlinear optical susceptibility (chi((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 chi((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)>10 pm V-1, when incorporated in a non-centrosymmetric DA multilayer stack. Using grating-shadowed oblique-angle deposition to laterally structure the DA interface distribution in such multilayers subsequently enables the demonstration of a chi((2)) grating with 280 nm periodicity, which is the shortest reported to date.
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