Exciton dynamics in planar dumbbell-shaped electron-donor molecules for organic optoelectronics
Jiang Jing, Emilie Steveler, Amira Mounya Gharbi, Sébastien Marbach, Pascal Didier, Gilles Ulrich, Ibrahim Bulut, Nicolas Leclerc, Wilfried Uhring,
Jérémie Léonard, Benoît Heinrich, Patrick Lévêque and Thomas Heiser
Exciton dynamics play a crucial role in determining the efficiency of organic photovoltaic devices and photo-detectors. However, establishing clear correlations between molecular structure and exciton diffusion length remains a significant challenge, limiting the rational design of more efficient materials. In this study, we investigate exciton transport in thin films of a planar dumbbell-shaped electron donor composed of discotic triazatruxene end-groups and an electron-deficient central unit. These molecules self-assemble into unique bridged-columnar structures, which are known to support efficient charge transport, although their impact on exciton dynamics had not yet been explored. Using a combination of time-resolved photoluminescence (TRPL), spatially resolved TRPL, and exciton–exciton annihilation measurements, we examine how structural order influences exciton diffusion in both the columnar- nematic and crystalline phases. We show that crystallization leads to a twofold increase in exciton diffusion length, reaching values comparable to those observed in state-of-the-art non-fullerene acceptors. Although the molecules exhibit a typical Stokes shift that is not particularly favorable for Förster energy transfer (FRET), ecffiient exciton transport is nonetheless achieved—enabled by long exciton lifetimes and anisotropic energy transfer within its distinctive bridged-columnar architecture. These results, supported by FRET analysis, highlight the effectiveness of the molecule's tailored dumbbell-shaped design and its ability to self-assemble into ordered structures that support both long-range exciton diffusion and efficient charge mobility.
