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The methods and approaches for investigation of orientation distribution and rotational mobility of molecules by numerical analysis of EPR spectra were considered. It was shown that for adequate estimation of mechanism and determination of rotational parameters of small probe molecules in structured matrixes such as liquid crystals it is necessary to analyze jointly a series of spectra recorded at different positions of aligned sample in magnetic field. The novel method was proposed for simulation of angular dependence of EPR spectra with considering rotational mobility of radicals. Perspectives of using of this method for investigation of bimodal orientation distribution were demonstrated.