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光激发CeO₂中共存的大极化子与小极化子

Coexisting Large and Small Polarons in Photoexcited CeO$_2$

Valentina Mazzotti, Eleonora Spurio, Nicolas Delnour, Michael Hilke, Kirk H. Bevan, Alexander Shluger, Paola Luches, David G. Cooke

arXiv 2608.30164首次发表:更新:

发表机构

McGill University; Istituto Nanoscienze – CNR; University College London(麦吉尔大学; 意大利国家研究委员会纳米科学研究所; 伦敦大学学院)

机构由 AI 辅助整理,请以论文原文为准。

AI 中文总结

该研究利用时间分辨太赫兹光谱,揭示光激发CeO₂中同时存在Fröhlich型大空穴极化子与小电子极化子,明确其形成时间、特性及机制,为金属氧化物光催化剂的电荷转移动力学研究提供了基础。

AI 中文摘要

采用时间分辨太赫兹(THz)光谱探测CeO₂中的极化子形成过程。超快THz光导率主要由大空穴极化子和小电子极化子的贡献主导:离域的大空穴极化子以820±50 fs的时间尺度形成,属于Fröhlich型,其光导率可通过简单Drude模型很好地描述,瞬态空穴迁移率为100 cm²/Vs;小电子极化子通过与Ce晶格位点的局域耦合形成,该过程由晶格Born有效电荷的降低所揭示,伴随瞬态声子软化。这些结果确立了CeO₂的双极化子性质,为理解金属氧化物光催化剂中的电荷转移动力学提供了基础。

英文摘要

Time-resolved terahertz (THz) spectroscopy is used to probe polaron formation in CeO$_2$. The ultrafast THz photoconductivity is dominated by contributions from large hole and small electron polarons. Delocalized large hole polarons are formed on a $820 \pm 50$ fs time scale and are of Fröhlich type, with optical conductivity well described by a simple Drude model and a transient hole mobility of $100$ cm$^2$/Vs. Small electron polarons form via localized coupling to Ce lattice sites, revealed by reduction in the lattice Born effective charge causing a transient phonon softening. These results establish the dual polaron nature of CeO$_2$ and provide a basis for understanding charge transfer dynamics in metal oxide photocatalysts.

Comments11 pages, 6 figures (including Supplementary Information)

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