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Temperature dependence of reflectivity of amorphous silicon dioxide: Evidence of delocalized excitons weakly scattered by phonons

机译:非晶二氧化硅反射率的温度依赖性:   离子激子的声子在声子中微弱地散射

摘要

We studied the reflectivity spectra of amorphous silicon dioxide detectedunder vacuum UV synchrotron radiation as a function of temperature between 10and 300 K. Kramers-Kronig dispersion analysis of reflectivity spectra allowedus to determine the absorption coefficient in the range from 8 to 17.5 eV.Spectra show four main peaks, the spectral positions of which are consistentwith literature data. An appreciable dependence of the line-shape ontemperature is observed for the first two peaks only. We demonstrate theexciton peak at 10.4 eV to have a very good Lorentzian band-shape at all theexamined temperatures. Based on existing theoretical models, this allows toargue excitons in SiO2 to be weakly scattered by phonons, thus retaining theirmobility properties notwithstanding the effects of exciton-phonon coupling andof intrinsic structural disorder of amorphous SiO2. Moreover, the observedtemperature dependence of the peak position together with the features of theUrbach absorption tail and of self-trapped exciton emission allow us toestimate the main parameters ruling exciton dynamics in SiO2. The features ofthe intrinsic Urbach absorption tail can be satisfactorily explained as aconsequence of those of the first excitonic peak, supporting the interpretationof the Urbach tail in SiO2 as a consequence of the momentary self-trapping ofthe 10.4 eV exciton. Finally, the characteristics of the other energy peaks arediscussed and an excitonic origin also for the 11.6 eV peak is put forward. Onthe whole, our results show that exciton dynamics accounts for all opticalproperties of pure silicon dioxide from 8 up to 11 eV.
机译:我们研究了在真空紫外同步加速器辐射下检测到的无定形二氧化硅的反射光谱与温度之间的函数关系,该反射光谱是温度介于10和300 K之间的。主峰,其光谱位置与文献数据一致。仅对于前两个峰观察到线形对温度的明显依赖。我们证明了在所有检查温度下10.4 eV处的激子峰都具有很好的洛伦兹带形。根据现有的理论模型,这允许SiO2中的激激激子被声子弱散射,从而尽管存在激子-声子耦合和无定形SiO2的固有结构无序的影响,但仍保持了其迁移性。此外,观察到的峰位置的温度依赖性以及乌尔巴赫吸收尾和自陷激子发射的特征使我们能够估计决定SiO2中激子动力学的主要参数。固有的Urbach吸收尾巴的特征可以令人满意地解释为第一个激子峰的特征,支持SiO2中Urbach尾巴的解释是由于10.4 eV激子的瞬时自陷所致。最后,讨论了其他能量峰的特征,并提出了11.6 eV峰的激子起源。总体而言,我们的结果表明,激子动力学解释了纯二氧化硅从8到11 eV的所有光学性质。

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