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Title: Efficient Singlet Fission and Triplet-Pair Emission in a Family of Zethrene Diradicaloids
Authors: Lukman, S
Richter, J.M
Yang, L
Hu, P 
Wu, J 
Greenham, N.C
Musser, A.J
Keywords: Binding energy
Quantum entanglement
Absorbed photons
Chromophore design
Excited state absorption
Photochemical properties
Thermally activated
Thermodynamic limits
Triplet excitons
Tunable materials
Excited states
Issue Date: 2017
Citation: Lukman, S, Richter, J.M, Yang, L, Hu, P, Wu, J, Greenham, N.C, Musser, A.J (2017). Efficient Singlet Fission and Triplet-Pair Emission in a Family of Zethrene Diradicaloids. Journal of the American Chemical Society 139 (50) : 18376-18385. ScholarBank@NUS Repository.
Abstract: Singlet fission offers the potential to overcome thermodynamic limits in solar cells by converting the energy of a single absorbed photon into two distinct triplet excitons. However, progress is limited by the small family of suitable materials, and new chromophore design principles are needed. Here, we experimentally vindicate the design concept of diradical stabilization in a tunable family of functionalized zethrenes. All molecules in the series exhibit rapid formation of a bound, spin-entangled triplet-pair state TT. It can be dissociated by thermally activated triplet hopping and exhibits surprisingly strong emission for an optically "dark" state, further enhanced with increasing diradical character. We find that the TT excited-state absorption spectral shape correlates with the binding energy between constituent triplets, providing a new tool to understand this unusual state. Our results reveal a versatile new family of tunable materials with excellent optical and photochemical properties for exploitation in singlet fission devices. © 2017 American Chemical Society.
Source Title: Journal of the American Chemical Society
ISSN: 0002-7863
DOI: 10.1021/jacs.7b10762
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