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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.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1]
  1. The Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Grant/Contract Number:
SC0012365; SC0012375
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
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
Language:
English
Subject:
36 MATERIALS SCIENCE; metamaterials; nonlinear optics; surface patterning
OSTI Identifier:
1347383

Yan, Yixin, Yuan, Yakun, Wang, Baomin, Gopalan, Venkatraman, and Giebink, Noel C. Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films. United States: N. p., Web. doi:10.1038/ncomms14269.
Yan, Yixin, Yuan, Yakun, Wang, Baomin, Gopalan, Venkatraman, & Giebink, Noel C. Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films. United States. doi:10.1038/ncomms14269.
Yan, Yixin, Yuan, Yakun, Wang, Baomin, Gopalan, Venkatraman, and Giebink, Noel C. 2017. "Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films". United States. doi:10.1038/ncomms14269. https://www.osti.gov/servlets/purl/1347383.
@article{osti_1347383,
title = {Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films},
author = {Yan, Yixin and Yuan, Yakun and Wang, Baomin and Gopalan, Venkatraman and Giebink, Noel C.},
abstractNote = {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.},
doi = {10.1038/ncomms14269},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {1}
}