Linear and Third‐Order Nonlinear Optical Properties of Chalcogenopyrylium‐Terminated Heptamethine Dyes with Rigid, Bulky Substituents. (1st October 2018)

• Record Type: Journal Article
• Authors: Getmanenko, Yulia A.; Allen, Taylor G.; Kim, Hyeongeu; Hales, Joel M.; Sandhu, Bhupinder; Fonari, Marina S.; Suponitsky, Kyrill Yu.; Zhang, Yadong; Khrustalev, Victor N.; Matichak, Jonathan D.; Timofeeva, Tatiana V.; Barlow, Stephen; Chi, San‐Hui; Perry, Joseph W.; Marder, Seth R.
• Is Part Of: Advanced functional materials. Volume 28:Number 46(2018)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2018-10-01
• Subjects: aggregation -- cyanine -- nonlinear optics -- polymethine; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.201804073
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract: The aggregation of chalcogenopyrylium‐terminated heptamethine dyes in high‐chromophore density films can be substantially suppressed by attachment of rigid, bulky substituents that project out of the plane of the conjugated π‐system of the dye, allowing the retention in the solid state of favorable linear and nonlinear optical properties relevant to all‐optical signal processing (AOSP). Dye structures are systematically engineered with a range of out‐of‐plane substituents to investigate the impacts on the optical properties at 1550 nm in the solid state. Large magnitudes of the third‐order susceptibility are obtained for solid films. Very high values of the two‐photon figure‐of‐merit (2PA‐FOM), an important parameter for AOSP, are observed in dilute solutions of seleno‐ and telluropyrylium dyes (in several cases >30). In the case of the telluropyrylium dye, the 2PA‐FOM is not measureable for 50 wt% blends with polymers. Blends of the selenopyrylium examples exhibit 2PA‐FOM values that, although decreased substantially relative to the solution values, in some cases meet the requirements for AOSP. Abstract : Systematic engineering of chalcogenopyrylium heptamethines gives insight into the impacts of the chalcogen and of rigid, bulky, out‐of‐plane substituents on their linear and nonlinear optical properties in neat films and 50 wt% blends with polymers. Some of these films meet the requirements for all‐optical signal processing at 1550 nm.