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Title: Bis(4-dialkylaminophenyl)heteroarylamino donor chromophores exhibiting exceptional hyperpolarizabilities
Organic electro-optic (EO) materials incorporated into silicon-organic hybrid and plasmonic-organic hybrid devices have enabled new records in EO modulation performance. We report a new series of nonlinear optical chromophores engineered by theory-guided design, utilizing bis(4-dialkylaminophenyl)heteroarylamino donor moieties to greatly enhance molecular hyperpolarizabilities. Hyperpolarizabilities predicted using density functional theory were validated by hyper-Rayleigh scattering measurements, showing strong prediction/experiment agreement and >2-fold advancement in static hyperpolarizability over the best prior chromophores. Electric field poled thin films of these chromophores showed significantly enhanced EO coefficients ( r 33 ) and poling efficiencies ( r 33 / E p ) at low chromophore concentrations compared with state-of-the-art chromophores such as JRD1 . The highest performing blend, containing just 10 wt% of the novel chromophore BTP7 , showed a 12-fold enhancement in poling efficiency per unit concentration vs. JRD1 . Our results suggest that further improvement in chromophore hyperpolarizability is feasible without unacceptable tradeoffs with optical loss or stability.  more » « less
Award ID(s):
2036514
NSF-PAR ID:
10378636
Author(s) / Creator(s):
; ; ; ; ; ; ;
Date Published:
Journal Name:
Journal of Materials Chemistry C
Volume:
9
Issue:
8
ISSN:
2050-7526
Page Range / eLocation ID:
2721 to 2728
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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