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The photo-driven process of singlet fission generates coupled triplet pairs(TT) with fundamentally intriguing and potentially useful properties. Thequintet 5TT0 sublevel is particularly interesting for quantum informationbecause it is highly entangled, addressable with microwave pulses, and could bedetected using optical techniques. Previous theoretical work on a modelHamiltonian and nonadiabatic transition theory, called the JDE model, hasdetermined that this sublevel can be selectively populated if certainconditions are met. Among the most challenging, the molecules within the dimerundergoing singlet fission must have their principal magnetic axes parallel toone another and to an applied Zeeman field B0. Here, we present time-resolvedparamagnetic resonance (TR-EPR) spectroscopy of a single crystal sample of anovel tetracenethiophene compound featuring arrays of dimers aligned in thismanner, mounted so that the orientation of the field relative to the molecularaxes could be controlled. The observed spin sublevel populations in the pairedTT and unpaired (T+T) triplets are consistent with predictions from the JDEmodel, including preferential 5TT0 formation at z||B0, with one caveat - two5TT spin sublevels have little to no population. This may be due to crossingsbetween the 5TT and 3TT manifolds in the field range investigated by TR-EPR,consistent with the inter-triplet exchange energy determined by monitoringphotoluminescence at varying magnetic fields.

Triplet-Pair Spin Signatures from Macroscopically Aligned Heteroacenes in an Oriented Single Crystal