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We present ultrafast quantitative interferometric pump-probe microscopy capable of tracking of photoexcitations in three dimensions with sub 5 nm spatial precision through retrieval of the full photoinduced transient complex refractive index with 15 fs temporal resolution. Using this we inves- tigate the quantum coherent photophysical process of ultrafast singlet exciton fission. Measurements on microcrystalline pentacene films grown on glass (SiO2) and boron nitride (hBN) reveal a 25 nm, 70 fs expansion of the joint-density-of-states along the crystal a,c-axes accompanied by a 6 nm, 115 fs contraction along the crystal b-axis. We propose that photogenerated singlet excitons un- dergo fission to correlated triplets pairs along the crystal a,c-axes within 70 fs and are subsequently decoupled into free-triplets along the crystal b-axes within 200 fs.

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• Creative Commons BY Attribution 4.0 International
  

Keyword: Ultrafast interferometric microscopy, singlet exciton fission, quantum coherent photophysical process

Date published: 2022-10-10

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Communications (ISSN: 20411723) vol. 13 issue. 1 5963

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Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1038/s41467-022-33647-5

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Updated at: 2025-02-27 16:30:54 +0900

Published on MDR: 2025-02-27 16:30:54 +0900