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Effective Negative Diffusion of Singlet Excitons in Organic Semiconductors.


ABSTRACT: Using diffraction-limited ultrafast imaging techniques, we investigate the propagation of singlet and triplet excitons in single-crystal tetracene. Instead of an expected broadening, the distribution of singlet excitons narrows on a nanosecond time scale after photoexcitation. This narrowing results in an effective negative diffusion in which singlet excitons migrate toward the high-density region, eventually leading to a singlet exciton distribution that is smaller than the laser excitation spot. Modeling the excited-state dynamics demonstrates that the origin of the anomalous diffusion is rooted in nonlinear triplet-triplet annihilation (TTA). We anticipate that this is a general phenomenon that can be used to study exciton diffusion and nonlinear TTA rates in semiconductors relevant for organic optoelectronics.

SUBMITTER: Berghuis AM 

PROVIDER: S-EPMC7869104 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Effective Negative Diffusion of Singlet Excitons in Organic Semiconductors.

Berghuis Anton Matthijs AM   Raziman T V TV   Halpin Alexei A   Wang Shaojun S   Curto Alberto G AG   Rivas Jaime Gómez JG  

The journal of physical chemistry letters 20210128 4


Using diffraction-limited ultrafast imaging techniques, we investigate the propagation of singlet and triplet excitons in single-crystal tetracene. Instead of an expected broadening, the distribution of singlet excitons narrows on a nanosecond time scale after photoexcitation. This narrowing results in an effective negative diffusion in which singlet excitons migrate toward the high-density region, eventually leading to a singlet exciton distribution that is smaller than the laser excitation spo  ...[more]

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