Low-power NIR-to-vis upconversion (UC) of incoherent excitation mediated by triplet-triplet annihilation (TTA) has a variety of promising applications, i.e. in photovoltaics, however these are strongly hampered by low UC efficiency...
Rubrene is the most widely used triplet-triplet annihilation (TTA) emitter for NIR-to-vis photon upconversion (UC), however, strong singlet fission (SF) in the solid films quenches its emission and hampers practical...
Solar energy harvesting is among the best solutions for a global transition toward carbon-neutral energy technologies. The existing solar energy harvesting technologies like photovoltaics (PV) and emerging molecular concepts such...
Singlet fission is detrimental to NIR-to-vis photon upconversion
in the solid rubrene (Rub) films, as it diminishes photoluminescence
efficiency. Previous studies have shown that thermally activated triplet
energy transport drives singlet fission with nearly 100% efficiency
in closely packed Rub crystals. Here, we examine triplet separation
and recombination as a function of intermolecular distance in the
crystalline films of Rub and the
t
-butyl substituted
rubrene (
t
BRub) derivative. The increased intermolecular
distance and altered molecular packing in
t
BRub films
cause suppressed singlet dissociation into free triplets due to slower
triplet energy transport. It was found that the formation of correlated
triplet pairs
1
(TT) and partial triplet separation
1
(T···T) occurs in both Rub and
t
BRub films despite differences in intermolecular coupling. Under
weak intermolecular coupling as in
t
BRub, geminate
triplet annihilation of
1
(T···T) outcompetes
dissociation into free triplets, resulting in emission from the
1
(TT) state. Essentially, increasing intermolecular distance
up to a certain point (a sweet spot) is a good strategy for suppressing
singlet fission and retaining triplet–triplet annihilation
properties.
Triplet-triplet annihilation (TTA) mediated NIR-to-vis photon upconversion (UC) operating under incoherent and low power excitation is increasingly attractive for various applications including photovoltaics. Unfortunately, efficient TTA emitters/annihilators for this spectral...
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