Sub-wavelength modulation of χ(2) optical nonlinearity in organic thin films
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 > 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:
-
- The Pennsylvania State Univ., University Park, PA (United States)
- Publication Date:
- Research Org.:
- Pennsylvania State Univ., University Park, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1347383
- Grant/Contract Number:
- SC0012365; SC0012375
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 8; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; metamaterials; nonlinear optics; surface patterning
Citation Formats
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., 2017.
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. https://doi.org/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. https://doi.org/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},
url = {https://www.osti.gov/biblio/1347383},
journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 8,
place = {United States},
year = {Fri Jan 27 00:00:00 EST 2017},
month = {Fri Jan 27 00:00:00 EST 2017}
}
Web of Science
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Works referencing / citing this record:
Designing Hybrids of Graphene Oxide and Gold Nanoparticles for Nonlinear Optical Response
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