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Producing Conventional and Transient Amino(mercapto)methyl Radicals by Addition of Muonium to a Crystalline Thioformamide (Mes*NHCH=S).
Chemphyschem
June 2024
Department of Applied Chemistry, School of Materials and Chemical Technology, Tokyo Institute of Technology, 2-12-1-H113 Ookayama, Meguro-ku, Tokyo, 152-8552, Japan.
Muonium (Mu=μe) is composed of a muon of light isotope of proton (μ) and electron (e) and can be used as a light surrogate for a hydrogen atom. In this paper, we investigated addition of muonium to a newly synthesized Mes*-substituted thioformamide (Mes*NHCH=S, Mes*=2,4,6-tBuCH). Transverse-field muon spin rotation (TF-μSR) of a solution sample of the thioformamide confirmed addition of muonium to the sulfur atom leading to the corresponding C-centered radical [Mes*NHC(H)⋅-SMu].
View Article and Find Full Text PDFDifluoromethylborates and Muonium for the Study of Isonitrile Insertion Affording Phenanthridines via Imidoyl Radicals.
J Org Chem
July 2023
Department of Applied Chemistry, School of Materials and Chemical Technology, Tokyo Institute of Technology, 2-12-1-H-113 Ookayama, Meguro-ku, Tokyo 152-8552, Japan.
The 6-(difluoromethyl)phenanthridine unit is a highly attractive fluoroalkyl-substituted planar nitrogen heterocycle in pharmaceutical and agrochemical research. In this paper, we report that difluoromethylborates can be used as a source of difluoromethyl radicals for isonitrile insertion, leading to 6-(difluoromethyl)phenanthridines. Tuning the aryl substituents in the difluoromethylborates and oxidizing reagents enabled the synthesis of 6-(difluoromethyl)phenanthridines through the generation of difluoromethyl radical and spontaneous intramolecular cyclization of the CFH-imidoyl radical intermediates.
View Article and Find Full Text PDFMuon-Nitrogen Quadrupolar Level Crossing Resonance in a Charge Transfer Salt.
J Phys Chem C Nanomater Interfaces
May 2022
ISIS Neutron and Muon Source, STFC Rutherford Appleton Laboratory, Chilton, Oxfordshire OX11 0QX, United Kingdom.
Although muons are primarily regarded as a local spin probe, they can also access the charge state of an atom or molecule via quadrupolar level crossing resonance (QLCR) spectroscopy. We use LiTCNQ (TCNQ = 7,7,8,8-tetracyanoquinodimethane), a simple charge transfer salt, to test the potential of this technique in molecular systems by studying the interaction of a positive muon with the TCNQ nitrogen atoms. We show that both a positive muon and muonium are able to add to the nitrogen, leading to a singlet spin state for the addition molecule.
View Article and Find Full Text PDFDynamics and local environment of an aromatic counterion bound to di-chain cationic surfactant bilayers studied by avoided level crossing muon spin resonance: evidence for counterion condensation.
Phys Chem Chem Phys
November 2021
Centre for Molecular and Materials Science, TRIUMF, Vancouver, Canada.
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 L and L 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 () of the muoniated spin probe were determined as a function of temperature by modelling the ALC-μSR spectra with Monte Carlo numerical simulations.
View Article and Find Full Text PDFLocal Electronic Structure and Dynamics of Muon-Polaron Complexes in Fe_{2}O_{3}.
Phys Rev Lett
January 2021
Department of Physics and Astronomy, University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada.
We perform detailed muon spin rotation (μSR) measurements in the classic antiferromagnet Fe_{2}O_{3} and explain the spectra by considering dynamic population and dissociation of charge-neutral muon-polaron complexes. We show that charge-neutral muon states in Fe_{2}O_{3}, despite lacking the signatures typical of charge-neutral muonium centers in nonmagnetic materials, have a significant impact on the measured μSR frequencies and relaxation rates. Our identification of such polaronic muon centers in Fe_{2}O_{3} suggests that isolated hydrogen (H) impurities form analogous complexes, and that H interstitials may be a source of charge carrier density in Fe_{2}O_{3}.
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