TY - JOUR
T1 - The entangled triplet pair state in acene and heteroacene materials
AU - Yong, Chaw Keong
AU - Musser, Andrew J.
AU - Bayliss, Sam L.
AU - Lukman, Steven
AU - Tamura, Hiroyuki
AU - Bubnova, Olga
AU - Hallani, Rawad K.
AU - Meneau, Aurelie
AU - Resel, Roland
AU - Maruyama, Munetaka
AU - Hotta, Shu
AU - Herz, Laura M.
AU - Beljonne, David
AU - Anthony, John E.
AU - Clark, Jenny
AU - Sirringhaus, Henning
N1 - Publisher Copyright:
© The Author(s) 2017.
PY - 2017/7/12
Y1 - 2017/7/12
N2 - 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.
AB - 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.
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U2 - 10.1038/ncomms15953
DO - 10.1038/ncomms15953
M3 - Article
C2 - 28699637
AN - SCOPUS:85024132897
SN - 2041-1723
VL - 8
JO - Nature Communications
JF - Nature Communications
M1 - 15953
ER -