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

Yan, Yixin; Yuan, Yakun; Wang, Baomin; Gopalan, Venkatraman; Giebink, Noel C.

doi:10.1038/ncomms14269

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

Journal Article · Fri Jan 27 00:00:00 EST 2017 · Nature Communications

DOI:https://doi.org/10.1038/ncomms14269· OSTI ID:1347383

Yan, Yixin ^[1]; Yuan, Yakun ^[1]; Wang, Baomin ^[1]; Gopalan, Venkatraman ^[1];

^[1]

The Pennsylvania State Univ., University Park, PA (United States)

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-C₆₀ 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 d₃₃ > 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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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012365; SC0012375

OSTI ID:: 1347383

Journal Information:: Nature Communications, Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 8 works

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