双钼钒酸中超快光致形成一种 metastable hidden state
材料科学
2025-12-10 v1
摘要
双钼钒酸（BiVO）是太阳燃料应用中的关键光催化剂，但关于光生极性态及其支配光化学路径的晶格动力学的根本问题仍存疑问。本文利用 femtosecond 光泵-X射线探针技术追踪BiVO在多个长度和时间尺度上的光致电子和结构动力学。瞬态X射线吸收光谱捕捉到VO四面体内亚皮秒电子局域化，符合小极性态形成；而时间分辨X射线衍射揭示了更慢的多皮秒晶格重组形成一种与单斜母质态和高温四方相都结构不同的隐藏光激发态。结合密度泛函理论，我们表明空穴-晶格相互作用动态降低了母质态单斜畸变，从而稳定了隐藏态。我们的结果表明，电子和空穴-晶格耦合共同塑造了激发态景观，对载流子传输、界面能态以及光化学能转换路径具有深远意义。
引用
@article{arxiv.2512.08287,
title = {Ultrafast light-induced formation of a metastable hidden state in bismuth vanadate},
author = {Viktoria F. Kunzelmann and Verena Streibel and Philip Schwinghammer and Philipp Kollenz and Burak Guzelturk and Franziska S. Hegner and Lissa Eyre and Frederico P. Delgado and Tsedenia A. Zewdie and Markus W. Heindl and Danyellen D. Monteiro Galindo and Daniel Sandner and Guanda Zhou and Elise Sirotti and Stanislav Bodnar and Yifeng Jiang and Yohei Uemura and Tobias Eklund and Frederico Lima and Xinchao Huang and Doriana Vinci and Fernando Ardana Lamas and Peter Zalden and Hristo Iglev and David A. Egger and Felix Deschler and Ian D. Sharp},
journal= {arXiv preprint arXiv:2512.08287},
year = {2025}
}