Bandlike Transport and Charge-Carrier Dynamics in BiOI Films.
Bandlike Transport and Charge-Carrier Dynamics in BiOI Films.
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DOI：
10.1021/acs.jpclett.3c01520
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发表时间：
2023-07-27
影响因子：
5.7
通讯作者：
Herz, Laura M.
中科院分区：
文献类型：
--
作者：
Lal, Snigdha;Righetto, Marcello;Ulatowski, Aleksander M.;Motti, Silvia G.;Sun, Zhuotong;MacManus-Driscoll, Judith L.;Hoye, Robert L. Z.;Herz, Laura M.
随着卤化铅钙钛矿（LHP）作为高效太阳能电池材料的出现，研究已经取得进展，以探索稳定，丰富和无毒的替代品。然而，这种无铅钙钛矿材料（PIM）的性能仍然明显落后于其LHP对应物。对于铋基PIM，一个重要的原因是经常观察到的超快电荷载流子局域化（或自陷），这对长程迁移率施加了根本限制。在这里，我们报告的太赫兹（THz）的光电导动力学薄膜的BiOI和证明缺乏这样的自陷，具有良好的电荷载流子迁移率，在295 K达到103 cm 2 V-1 s-1，并逐渐增加到1013 cm 2 V-1 s-1在5 K，表示占主导地位的带状运输。使用瞬态光致发光和太赫兹和微波电导率光谱的组合，我们进一步研究电荷载流子复合过程，揭示了在纳秒和低双分子带-带复合的BiOI中的缺陷的电子的电荷特定的捕获。根据钝化协议的发展，BiOI因此成为铋基半导体家族中的上级光捕获半导体。
Following the emergence of lead halide perovskites (LHPs) as materials for efficient solar cells, research has progressed to explore stable, abundant, and nontoxic alternatives. However, the performance of such lead-free perovskite-inspired materials (PIMs) still lags significantly behind that of their LHP counterparts. For bismuth-based PIMs, one significant reason is a frequently observed ultrafast charge-carrier localization (or self-trapping), which imposes a fundamental limit on long-range mobility. Here we report the terahertz (THz) photoconductivity dynamics in thin films of BiOI and demonstrate a lack of such self-trapping, with good charge-carrier mobility, reaching ∼3 cm2 V–1 s–1 at 295 K and increasing gradually to ∼13 cm2 V–1 s–1 at 5 K, indicative of prevailing bandlike transport. Using a combination of transient photoluminescence and THz- and microwave-conductivity spectroscopy, we further investigate charge-carrier recombination processes, revealing charge-specific trapping of electrons at defects in BiOI over nanoseconds and low bimolecular band-to-band recombination. Subject to the development of passivation protocols, BiOI thus emerges as a superior light-harvesting semiconductor among the family of bismuth-based semiconductors.
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