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中国物理学会期刊

纳米晶锐钛矿相TiO2的非简谐效应和声子局域

CSTR: 32037.14.aps.57.3077

Anharmonic phonon coupling and phonon confinement in nanocrystalline anatase TiO2

CSTR: 32037.14.aps.57.3077
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  • 对晶粒尺寸为194,86和56nm的纳米晶锐钛矿相TiO2,进行了从83到723K的变温拉曼散射测量,并对Eg(1)模式进行了详细研究.根据非简谐效应和声子局域模型,对Eg(1)拉曼峰进行了拟合与计算.结果表明,以上三种纳米晶粒的晶格振动机理,在本质上是相同的.三声子过程对频率蓝移起主要作用.为了得到很好的拟合,需要同时考虑三声子和四声子过程.随着温度的升高,四声子过程增强,并对三声子过程起抵消作用.与非简谐衰减相关的声子寿命随着晶粒

     

    A temperature-dependent Raman scattering study of the Eg(1) mode was carried out at 83 to 723K for nanocrystalline anatase TiO2 with different sizes of 194,86 and 56nm. By means of a combined model of anharmonic coupling and phonon confinement,the Eg(1) Raman spectra were fitted and calculated. The results show that,the temperature-dependent lattice vibration fundamentals are essentially the same for the three samples. The blue shift of Raman frequencies mainly comes from the contribution of three-phonon processes. In order to get good fittings,both the three- and four-phonon processes need to be considered. With increasing temperature,the four-phonon process becomes more important and counteracts the effect of the three-phonon process. The anharmonic-decay-related phonon lifetime increases as nanocrystalline size decreases,and the smaller nanoparticles have slower anharmonic decay. At low temperatures,the phonon confinement is responsible for a much shorter phonon lifetime for the 56-nm nanocrystals. The phonon confinement induces a blue shift of the Eg(1) mode and an asymmetrical broadening at high frequencies. It has a relatively larger effect on the linewidth broadening than on the peak shift.

     

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