Soliton microdynamics of multiphase thermal conductivity of fuel materials of the uranium dioxide type with the generation of new-type surface vibrations

Abstract

The microdynamics of large-amplitude nonlinear atomic vibrations in crystals of the UO2, PuO2, and ThO2 types with the fluorite structure has been studied using the neutron spectrometry and computer simulation methods. Investigations performed on the DIN-2PI neutron spectrometer have revealed a fine structure of the multi-resonance spectral density of vibrations in UO2. The temperature dependence of the coefficient of thermal conductivity of UO2 with two maxima in the range from 500 to 3000 K and the multi-resonance density of vibrations has been interpreted according to the results of the computer simulation demonstrating the generation of single solitons and soliton beams at low and high temperatures. It has been shown that the maximum of the coefficient of thermal conductivity at a temperature of 500 K is determined by the energy transfer by solitons. A decrease in the coefficient of thermal conductivity in the range from 500 to 2000 K is determined by soliton-soliton scattering. An increase in the coefficient of thermal conductivity in the range from 2000 to 3000 K is determined by the generation of soliton beams with the formation of dynamic pores. It has been found that, in crystals of the UO2, PuO2, and ThO2 types, there are resonances of new-type surface vibrations between the dispersion branches of optical phonons. An additional resonance between the low-frequency optical branch and the acoustic branch has been revealed at finite temperatures. This resonance has been interpreted as a nonlinear local mode, in the framework of the quantum theory, possible, a biphonon. It has also been found that, with an increase in the excitation energy, there are soliton branches between this resonance and the acoustic branch in UO2, which in the phase plane cross the band of a nonlinear local mode with an increasing rate.