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>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 χ(2) grating with 280 nm periodicity, which is the shortest reported to date.
%0 Journal Article
%1 yan2017sub-wavelength
%A Yan, Yixin
%A Yuan, Yakun
%A Wang, Baomin
%A Gopalan, Venkatraman
%A Giebink, Noel C.
%D 2017
%I Nature Publishing Group
%J Nature Communications
%K additionally ct-state organic
%P 14269
%R 10.1038/ncomms14269
%T Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films
%U /brokenurl#http:https://dx.doi.org/10.1038/ncomms14269
%V 8
%X 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>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 χ(2) grating with 280 nm periodicity, which is the shortest reported to date.
@article{yan2017sub-wavelength,
abstract = {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>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 χ(2) grating with 280 nm periodicity, which is the shortest reported to date.},
added-at = {2017-02-16T14:03:35.000+0100},
author = {Yan, Yixin and Yuan, Yakun and Wang, Baomin and Gopalan, Venkatraman and Giebink, Noel C.},
biburl = {https://www.bibsonomy.org/bibtex/24d4ee411da89d8217ea9aa5b362b1af4/bretschneider_m},
doi = {10.1038/ncomms14269},
interhash = {bee1caf71ecadcb542953ab74586c9b2},
intrahash = {4d4ee411da89d8217ea9aa5b362b1af4},
issn = {2041-1723},
journal = {Nature Communications},
keywords = {additionally ct-state organic},
month = {1},
pages = 14269,
publisher = {Nature Publishing Group},
timestamp = {2017-02-16T14:03:35.000+0100},
title = {Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films},
url = {/brokenurl#http:https://dx.doi.org/10.1038/ncomms14269},
volume = 8,
year = 2017
}