PMID- 20707539 OWN - NLM STAT- MEDLINE DCOM- 20101122 LR - 20121115 IS - 1089-7690 (Electronic) IS - 0021-9606 (Linking) VI - 133 IP - 5 DP - 2010 Aug 7 TI - Mesoscale spatial distribution of electron spins studied by time-resolved small-angle and ultrasmall-angle neutron scattering with dynamic nuclear polarization: a case of 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) doped in high-density polyethylene. PG - 054504 LID - 10.1063/1.3460923 [doi] AB - We carried out time-resolved small-angle neutron scattering (SANS) and ultrasmall-angle neutron scattering (USANS) studies of dynamically polarized high-density polyethylene (HDPE) doped with 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) persistent free radicals. We observed a remarkable enhancement of the scattering intensity shortly after a switching of microwave frequency from positive (negative) to negative (positive) dynamic nuclear polarization (DNP). The enhancement was found to be due to spatially heterogeneous proton-spin polarization generated as a result of heterogeneously distributed TEMPO in the HDPE sample. The spatial fluctuation of the polarization ranged up to the length-scale of > or = 100 nm. This result strongly suggests that the TEMPO free radicals are localized more in nonfibrils but less in fibrils of HDPE. In this way, we propose that the time-resolved DNP-SANS and DNP-USANS be general techniques to determine mesoscale spatial distribution of electron spins in dielectric materials. FAU - Kumada, Takayuki AU - Kumada T AD - Quantum Beam Science Directorate, Kansai Photon Science Institute, Japan Atomic Energy Agency, Umemidai, Kizugawa, Kyoto 619-0215, Japan. kumada.takayuki@jaea.go.jp FAU - Noda, Yohei AU - Noda Y FAU - Koizumi, Satoshi AU - Koizumi S FAU - Hashimoto, Takeji AU - Hashimoto T LA - eng PT - Journal Article PT - Research Support, Non-U.S. Gov't PL - United States TA - J Chem Phys JT - The Journal of chemical physics JID - 0375360 RN - 0 (Cyclic N-Oxides) RN - 0 (Free Radicals) RN - 9002-88-4 (Polyethylene) RN - VQN7359ICQ (TEMPO) SB - IM MH - Cyclic N-Oxides/*chemistry MH - *Electrons MH - Free Radicals/chemistry MH - Polyethylene/*chemistry MH - Scattering, Small Angle MH - Time Factors MH - X-Ray Diffraction EDAT- 2010/08/17 06:00 MHDA- 2010/12/14 06:00 CRDT- 2010/08/17 06:00 PHST- 2010/08/17 06:00 [entrez] PHST- 2010/08/17 06:00 [pubmed] PHST- 2010/12/14 06:00 [medline] AID - 10.1063/1.3460923 [doi] PST - ppublish SO - J Chem Phys. 2010 Aug 7;133(5):054504. doi: 10.1063/1.3460923.