TY - JOUR
T1 - Cocrystalline Polymer Films Exhibiting Second-Order Nonlinear Optical Properties
AU - Xu, Yifan
AU - Zu, Rui
AU - Yennawar, Neela H.
AU - Gopalan, Venkatraman
AU - Hickey, Robert J.
N1 - Funding Information:
This work is supported by the Air Force Office of Scientific Research (AFOSR) under the Young Investigator Prize (Award: 18RT0680). R.Z. and V.G. were primarily supported as part of the center for 3D Ferroelectric Microelectronics (3DFeM), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences under Award Number DE-SC002111, for the optical SHG measurements. The AFM and WAXS measurements were taken at the Materials Characterization Lab (MCL) in the Materials Research Institute (MRI) at Penn State University. We thank Nichole Wonderling for her help on X-ray scattering measurements and discussion.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/10/19
Y1 - 2021/10/19
N2 - Tailored polymer materials exhibiting high-glass transition temperatures, cross-linked matrices, and/or strong intermolecular interactions containing electric-field poled nonlinear optical (NLO) chromophores are promising materials for applications in optical telecommunication, high-performance computing, and data transmission. Although the current design parameters have led to significant advances in NLO materials, we introduce an alternative, yet highly effective, approach in which a NLO chromophore is cocrystallized with a polymer, forming a noncentrosymmetric hybrid host-guest complex. Specifically, poly(ethylene oxide) (PEO) and 2-chloro-4-nitroaniline (CNA) will cocrystallize and exhibit second harmonic generation (SHG) activity due to the formation of a noncentrosymmetric cocrystalline unit cell where the chromophore exhibits acentric alignment. Furthermore, the hybrid PEO/CNA films exhibit interesting SHG activity at elevated temperature in which SHG intensity decreases to zero when the cocrystal orientation randomizes due to sample melting. Aligning and maintaining a cocrystalline domain orientation via the formation of hybrid host-guest complexes, while imparting SHG properties, is an innovative approach for creating materials exhibiting SHG properties.
AB - Tailored polymer materials exhibiting high-glass transition temperatures, cross-linked matrices, and/or strong intermolecular interactions containing electric-field poled nonlinear optical (NLO) chromophores are promising materials for applications in optical telecommunication, high-performance computing, and data transmission. Although the current design parameters have led to significant advances in NLO materials, we introduce an alternative, yet highly effective, approach in which a NLO chromophore is cocrystallized with a polymer, forming a noncentrosymmetric hybrid host-guest complex. Specifically, poly(ethylene oxide) (PEO) and 2-chloro-4-nitroaniline (CNA) will cocrystallize and exhibit second harmonic generation (SHG) activity due to the formation of a noncentrosymmetric cocrystalline unit cell where the chromophore exhibits acentric alignment. Furthermore, the hybrid PEO/CNA films exhibit interesting SHG activity at elevated temperature in which SHG intensity decreases to zero when the cocrystal orientation randomizes due to sample melting. Aligning and maintaining a cocrystalline domain orientation via the formation of hybrid host-guest complexes, while imparting SHG properties, is an innovative approach for creating materials exhibiting SHG properties.
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U2 - 10.1021/acsmacrolett.1c00345
DO - 10.1021/acsmacrolett.1c00345
M3 - Article
C2 - 35549037
AN - SCOPUS:85116697838
SN - 2161-1653
VL - 10
SP - 1216
EP - 1222
JO - ACS Macro Letters
JF - ACS Macro Letters
IS - 10
ER -