NDLI: Structures and electronic states of photoexcited states in a system of two nitroxide radicals linked to fullerene studied by two-dimensional pulsed nutation and time-resolved electron paramagnetic resonance spectroscopy

Content Provider	Springer Nature Link
Author	Ohba, Y. Nishimura, M. Mizuochi, N. Yamauchi, S.
Copyright Year	2004
Abstract	Magnetic properties of fulleropyrrolidine adducts with two stable nitroxide radicals (2,2,6,6-tetramethylpiperidine-1-oxyl, TEMPO) were studied in toluene solution by continuous-wave time-resolved (TR) and pulsed electron paramagnetic resonance (EPR) spectroscopy in the ground and photoexcited states. Four isomers of the bisadduct,trans-1,trans-2,trans-3, and equatorial forms, having the second pyrrolidine ring at different [6-6] bonds were synthesized. In the ground states, the exchange interaction between two TEMPOs is so small that the spin state of the bisadduct is a doublet in nature. By means of spectral simulations of the EPR spectra in frozen solution at 70 K, the upper limit of the exchange interaction was estimated to be 5 MHz for thetrans-1 andtrans-2 and 10 MHz for thetrans-3 and equatorial isomers. The simulation was also made to determine relative positions of the two TEMPO groups with respect to the pyrrolidine ring. Photoexcited states of the bisadducts with excitation of the 532 nm laser pulse were studied in frozen toluene solution at 5–100 K by using two-dimensional (2-D) pulsed nutation EPR and TREPR. The spin multiplicity of the excited state was determined by the nutation frequency. All of the four bisadducts showed strong exchange couplings between two TEMPOs and fullerene triplet3C 60 * , resulting in the generation of the excited quintet and triplet states. The excited triplet states have been observed and assigned for the first time in strongly coupled triplet-radical systems. The zero-field splittings of the quintet state determined from the 2-D nutation EPR spectra were analyzed as the sum of the spinspin interactions among the three paramagnetic centers, two TEMPOs and3C 60 * . On the basis of these analyses, the spin distribution on the3C 60 * part and the geometry of two TEMPOs are discussed.
Starting Page	117
Ending Page	134
Page Count	18
File Format	PDF
ISSN	09379347
Journal	Applied Magnetic Resonance
Volume Number	26
Issue Number	1-2
e-ISSN	16137507
Language	English
Publisher	Springer-Verlag
Publisher Date	2004-01-01
Publisher Place	Vienna
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	Solid State Physics Spectroscopy/Spectrometry Physical Chemistry Organic Chemistry
Content Type	Text
Resource Type	Article
Subject	Atomic and Molecular Physics, and Optics

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