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It has been claimed that longitudinal field muon spin relaxation (LF-μSR) experiments on the organic semiconductor (OSC) tris-(8-hydroxyquinoline)aluminum(III) (Alq3) have measured electron hopping rates of ∼ 1 0 12 s − 1 , while density functional theory (DFT) calculations suggest that electron hopping between a muoniated radical and a neighboring molecule is energetically unfavorable and that the LF-μSR experiments were probing muoniated radicals with localized spin density. We have performed avoided level crossing muon spin resonance (ALC-μSR) and transverse field muon spin rotation (TF-μSR) measurements on Alq3 and 8-hydroxyquinoline (8hq), which is meant to model the muoniated radicals present in Alq3 when they are not in an OSC. These are supplemented by benchmarked DFT calculations. The ALC-μSR and TF-μSR spectra of 8hq and Alq3 are best explained by Mu adding to all six secondary carbons of the quinolate rings with roughly equal yields and localized spin density. There is no evidence in the TF-μSR spectrum of Alq3 for the formation of radicals with muon hyperfine coupling constants of 23 or 91 MHz as reported earlier by others. Our measurements support the view that there is localized spin density on the molecule to which Mu is covalently bound and the muon is not a passive probe in organic systems as it can be incorporated into radicals that have different electronic structures to the parent compounds. The muoniated radicals in Alq3 are more short-lived than in 8hq, which could be due to interactions with mobile electrons in the OSC, but with electron spin flip rates on the order of ∼ 1 0 7 s − 1 . [ABSTRACT FROM AUTHOR]

Avoided level crossing muon spin resonance (ALC-μSR) has been used to study the reorientational dynamics of muon-spin-labelled 2,4,6-trimethylbenzoate (246TMB−) counterions and their interaction with DODMAC (dioctadecyldimethylammonium chloride) bilayers in the Lα and Lβ liquid crystalline states. The muoniated radical anion formed by the addition of muonium to the secondary carbons of the aromatic ring of 246TMB− is used as a local spin probe. The muon and methylene proton hyperfine parameters and the electron spin relaxation rate (λe) of the muoniated spin probe were determined as a function of temperature by modelling the ALC-μSR spectra with Monte Carlo numerical simulations. The observation of a Δ1 resonance indicates that 246TMB− is undergoing anisotropic motion and doesn't reside in the aqueous layer in either the Lα and Lβ phases. The lack of an abrupt change in the hyperfine parameters or λe when the system goes from the Lβ to the Lα lamellar liquid crystalline phases suggests that 246TMB− is located at the oil–water interface rather than within the bilayer. The hyperfine parameters indicate that 246TMB− is undergoing large amplitude reorientational motion about a preferred orientation resulting from the bilayer's electric field. The interaction between 246TMB− and the bilayer decreases and the amplitude of the wobbling-in-a-cone motion increases with increasing temperature. The temperature dependence of the electron spin relaxation rate indicates the barrier to reorientation is 41.7 kJ mol−1. [ABSTRACT FROM AUTHOR]

It has been claimed that longitudinal field muon spin relaxation (LF-μSR) experiments on the organic semiconductor (OSC) tris-(8-hydroxyquinoline)aluminum(III) (Alq 3 ) have measured electron hopping rates of ∼10 12 s -1 , while density functional theory (DFT) calculations suggest that electron hopping between a muoniated radical and a neighboring molecule is energetically unfavorable and that the LF-μSR experiments were probing muoniated radicals with localized spin density. We have performed avoided level crossing muon spin resonance (ALC-μSR) and transverse field muon spin rotation (TF-μSR) measurements on Alq 3 and 8-hydroxyquinoline (8hq), which is meant to model the muoniated radicals present in Alq 3 when they are not in an OSC. These are supplemented by benchmarked DFT calculations. The ALC-μSR and TF-μSR spectra of 8hq and Alq 3 are best explained by Mu adding to all six secondary carbons of the quinolate rings with roughly equal yields and localized spin density. There is no evidence in the TF-μSR spectrum of Alq 3 for the formation of radicals with muon hyperfine coupling constants of 23 or 91 MHz as reported earlier by others. Our measurements support the view that there is localized spin density on the molecule to which Mu is covalently bound and the muon is not a passive probe in organic systems as it can be incorporated into radicals that have different electronic structures to the parent compounds. The muoniated radicals in Alq 3 are more short-lived than in 8hq, which could be due to interactions with mobile electrons in the OSC, but with electron spin flip rates on the order of ∼10 7 s -1 .