Spin density encodes intramolecular singlet exciton fission in pentacene dimers.

Abstract:

:The formation of two triplet excitons at the cost of one photon via singlet exciton fission in organic semiconductors can potentially enhance the photocurrent in photovoltaic devices. However, the role of spin density distribution in driving this photophysical process has been unclear until now. Here we present the significance of electronic spin density distribution in facilitating efficient intramolecular singlet exciton fission (iSEF) in π-bridged pentacene dimers. We synthetically modulate the spin density distribution in a series of pentacene dimers using phenyl-, thienyl- and selenyl- flanked diketopyrrolopyrrole (DPP) derivatives as π-bridges. Using femtosecond transient absorption spectroscopy, we find that efficient iSEF is only observed for the phenyl-derivative in ~2.4 ps while absent in the other two dimers. Electronic structure calculations reveal that phenyl-DPP bridge localizes α- and β-spin densities on distinct terminal pentacenes. Upon photoexcitation, a spin exchange mechanism enables iSEF from a singlet state which has an innate triplet pair character.

journal_name

Nat Commun

journal_title

Nature communications

authors

Krishnapriya KC,Roy P,Puttaraju B,Salzner U,Musser AJ,Jain M,Dasgupta J,Patil S

doi

10.1038/s41467-018-07736-3

subject

Has Abstract

pub_date

2019-01-03 00:00:00

pages

33

issue

1

issn

2041-1723

pii

10.1038/s41467-018-07736-3

journal_volume

10

pub_type

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