Volume 250, 2024

Singlet fission is incoherent in pristine orthorhombic single crystals of rubrene: no evidence of triplet-pair emission

Abstract

Singlet fission (SF) and its inverse, triplet–triplet annihilation (TTA), are promising strategies for enhancing photovoltaic efficiencies. However, detailed descriptions of the processes of SF/TTA are not fully understood, even in the most well-studied systems. Reports of the photophysics of crystalline rubrene, for example, are often inconsistent. Here we attempt to resolve these inconsistencies using time-resolved photoluminescence and transient absorption spectroscopy of ‘pristine’ rubrene orthorhombic single crystals. We find the reported time-resolved photoluminescence behaviour that hinted at triplet-pair emission is found only at specific sites on the crystals and likely arises from surface defects. Using transient absorption spectroscopy of the same crystals, we also observe no evidence of instantaneous generation of triplet-pair population with ∼100 fs excitation, independent of excitation wavelength (532 nm, 495 nm) or excitation angle. Our results suggest that SF occurs incoherently on a relatively slow (picosecond) timescale in rubrene single crystals, as expected from the original theoretical calculations. We conclude that the sub-100 fs formation of triplet pairs in crystalline rubrene films is likely to be due to static disorder.

Graphical abstract: Singlet fission is incoherent in pristine orthorhombic single crystals of rubrene: no evidence of triplet-pair emission

Associated articles

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Article information

Article type
Paper
Submitted
08 Sep 2023
Accepted
20 Sep 2023
First published
26 Sep 2023
This article is Open Access
Creative Commons BY license

Faraday Discuss., 2024,250, 162-180

Singlet fission is incoherent in pristine orthorhombic single crystals of rubrene: no evidence of triplet-pair emission

D. G. Bossanyi, M. Matthiesen, R. Jayaprakash, S. Bhattacharya, J. Zaumseil and J. Clark, Faraday Discuss., 2024, 250, 162 DOI: 10.1039/D3FD00150D

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