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FT-EPR Spectrum taken at a delay of 200 ns after laser excitation showing two sets of narrow lines of ground state N@C 60 and N@C 70 molecules as well as a single line of 3 C 60
Source publication
The release of atomic nitrogen from fullerene cages under irradiation with ultraviolet laserlight has been studied. The experiments show that there is a more favorable decay pathway for NatC60 than for NatC70, indicating that the lifetime of the metastable triplet state is not controlling the escape.
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Citations
N@C60, a nitrogen atom encapsulated in a fullerene shell, has an electron-nuclear spin system with outstanding coherence properties attractive for quantum computation. The stability of this molecule is known to be limited due to thermal escape of the nitrogen atom from the C60 cage but little is known about the stability towards optical excitation, which is one possible tool for an indirect scheme to manipulate and read out quantum information. Here, we report the results of a systematic study regarding thermal and optical effects on the stability of N@C60. The central result is that stability under intense laser irradiation can be obtained when the sample remains cooled below a certain temperature. Furthermore, the effect of molecules from the atmosphere or matrix (e.g. oxygen, toluene etc.) on N@C60 is discussed with respect to spin read-out experiments and the decomposition of N@C60. As a result, appropriate experimental conditions for optical quantum state read-out of this material are identified.
Using CW-ESR spectroscopy, the photo induced decomposition of N@C60 in five solvents under irradiation with 254 nm and 365 nm ultra violet light was measured. The results indicate that the decomposition rate of N@C60 is highly dependent on the solvent chosen. The finding shows that carbon disulphide and cis/trans-decalin are the most suitable solvents for future photoexitation experiments of N@C60. In addition a comparison between decay rate of N@C60 in ambient and degassed solvents suggests that decomposition is not principally via an interaction of the 3C60 excited state and the nitrogen atom.
