skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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-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:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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. doi:10.1038/ncomms14269.
Yan, Yixin, Yuan, Yakun, Wang, Baomin, Gopalan, Venkatraman, and Giebink, Noel C. Fri . "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 = {Fri Jan 27 00:00:00 EST 2017},
month = {Fri Jan 27 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1work
Citation information provided by
Web of Science

Save / Share:
  • Cited by 38
  • Both the linear and nonlinear optical properties of Bi{sub 3.15}Nd{sub 0.85}Ti{sub 3}O{sub 12} (BNT{sub 0.85}) ferroelectric thin films deposited on quartz substrates were investigated. The fundamental optical constants were determined as a function of light wavelength by optical transmittance measurements. By performing single-beam Z-scan experiments with femtosecond laser pulses at a wavelength of 800 nm, the two-photon absorption (TPA) coefficient β and third-order nonlinear refraction index γ were measured to be 1.15 × 10{sup 2 }cm/GW and −8.15 × 10{sup −3} cm{sup 2}/GW, respectively. The large TPA is attributed to an indirect transition process via the intermediate energy levels and the large refractive nonlinearity is themore » result of the electronic polarization and ferroelectric polarization arisen from the femtosecond midinfrared radiation. The results indicate that the BNT{sub 0.85} thin film is a promising candidate for applications in nonlinear photonic devices.« less
  • The nonlinear susceptibility of thin stannum dichloride phthalocyanine (SnCl{sub 2}Pc) films was studied by the method of degenerate four-wave mixing (DFWM) using the second-harmonic 532-nm, 10-ns pulses from a single-mode, TEM{sub 00}, 1.5-mJ Nd{sup 3+}:YAG laser and by the method of nonlinear lens (the Z-scan method). The intensity of the first-order self-diffraction upon the DFWM on dynamic gratings induced in SnCl{sub 2}Pc films has a cubic dependence on the recording-beam intensity, indicating to the third-order nonlinear response of the films. The value of the nonlinear susceptibility {chi}{sup (3)}({omega};{omega},-{omega},{omega})=(4.4 {+-} 0.5) x 10{sup -7} esu noticeably exceeds this value for phthalocyaninesmore » known in the literature. The mechanisms that can be responsible for the nonlinear response of the new synthesised material are discussed. (nonlinear optical phenomena)« less
  • We compare the superlattice modulation, microstructure, and epitaxy of Tl/sub 2/Ba/sub 2/Ca/sub 2/Cu/sub 3/O/sub 10/ thin films grown on MgO (100) and SrTiO/sub 3/ (100) substrates by dc diode sputtering. Films grown on MgO were found to be quite clean with the c axis perpendicular to the substrate. However, no in-plane orientational relationship to the substrate was found. Films grown on SrTiO/sub 3/, on the other hand, showed very good epitaxy to the substrate despite the presence of second phases. Films grown on MgO also exhibited a longer coherence length of the superlattice modulation than those grown on SrTiO/sub 3/more » under identical conditions.« less
  • Very large third-order optical nonlinearity, {chi}{sup (3)}{approximately}2.5{times}10{sup {minus}6} esu, measured by a degenerate four wave mixing method using a short pulse (70 picosecond) laser, has been found in the rapid-thermal annealed Au:SiO{sub 2} composite films at concentrations below the Au percolation threshold. The dependence of the {chi}{sup (3)} on Au concentration, p, follows a cubic power law. The maximum figure of merit, {chi}{sup (3)}/{alpha} (with {alpha} being the absorption coefficient) is about 10{sup {minus}11} esu cm. We explain this result as due to local field enhancement arising from the Mie resonance of the Au nanoclusters, with strong interaction between themore » nanoclusters further promoting the effect. {copyright} {ital 1997 American Institute of Physics.}« less