The entangled triplet pair state in acene and heteroacene materials
Journal
Nature communications
Journal Volume
8
Journal Issue
1
Date Issued
2017-07-12
Author(s)
Musser, Andrew J
Bayliss, Sam L
Lukman, Steven
Tamura, Hiroyuki
Bubnova, Olga
Hallani, Rawad K
Meneau, Aurélie
Resel, Roland
Maruyama, Munetaka
Hotta, Shu
Herz, Laura M
Beljonne, David
Anthony, John E
Clark, Jenny
Sirringhaus, Henning
Abstract
Entanglement of states is one of the most surprising and counter-intuitive consequences of quantum mechanics, with potent applications in cryptography and computing. In organic materials, one particularly significant manifestation is the spin-entangled triplet-pair state, which mediates the spin-conserving fission of one spin-0 singlet exciton into two spin-1 triplet excitons. Despite long theoretical and experimental exploration, the nature of the triplet-pair state and inter-triplet interactions have proved elusive. Here we use a range of organic semiconductors that undergo singlet exciton fission to reveal the photophysical properties of entangled triplet-pair states. We find that the triplet pair is bound with respect to free triplets with an energy that is largely material independent (∼30 meV). During its lifetime, the component triplets behave cooperatively as a singlet and emit light through a Herzberg-Teller-type mechanism, resulting in vibronically structured photoluminescence. In photovoltaic blends, charge transfer can occur from the bound triplet pairs with >100% photon-to-charge conversion efficiency.
Subjects
SINGLET-EXCITON-FISSION; ELECTRONIC-STRUCTURE; TETRACENE CRYSTALS; CHARGE-TRANSFER; QUANTUM EFFICIENCY; THIN-FILMS; PENTACENE; ANNIHILATION; FLUORESCENCE; DYNAMICS
SDGs
Publisher
NATURE PUBLISHING GROUP
Type
journal article