Fan Benshu, De Giovannini Umberto, Hübener Hannes, Zhou Shuyun, Duan Wenhui, Rubio Angel, Tang Peizhe
State Key Laboratory of Low-Dimensional Quantum Physics and Department of Physics, Tsinghua University, Beijing 100084, People's Republic of China.
Max Planck Institute for the Structure and Dynamics of Matter, Center for Free Electron Laser Science, 22761 Hamburg, Germany.
Sci Adv. 2025 Aug 22;11(34):eadw2744. doi: 10.1126/sciadv.adw2744. Epub 2025 Aug 20.
Optical selection rules endorsed by symmetry are crucial for understanding the optical properties of quantum materials and the associated ultrafast spectral phenomena. Here, we introduce momentum-resolved Floquet optical selection rules using group theory to elucidate the pump-probe photoemission spectral distributions of monolayer black phosphorus (BP), which are governed by the symmetries of both the material and the lasers. Using time-dependent density functional theory (TDDFT), we further investigate the dynamical evolution of Floquet(-Volkov) states in the photoemission spectra of monolayer BP, revealing their spectral weights at specific momenta for each sideband. These observations are comprehensively explained by the proposed Floquet optical selection rules. Our framework not only clarifies experimental photoemission spectra but also uncovers unexplored characteristics under different pump-probe configurations. Our results are expected to deepen the understanding of light-induced ultrafast spectra in BP and can be extended to other Floquet systems.
由对称性支持的光学选择规则对于理解量子材料的光学性质以及相关的超快光谱现象至关重要。在此,我们引入基于群论的动量分辨弗洛凯光学选择规则,以阐明单层黑磷(BP)的泵浦 - 探测光电子能谱分布,这些分布由材料和激光的对称性共同决定。使用含时密度泛函理论(TDDFT),我们进一步研究了单层BP光电子能谱中弗洛凯( - 沃尔科夫)态的动力学演化,揭示了每个边带在特定动量下的光谱权重。所提出的弗洛凯光学选择规则全面解释了这些观测结果。我们的框架不仅阐明了实验光电子能谱,还揭示了不同泵浦 - 探测配置下未被探索的特性。我们的结果有望加深对BP中光诱导超快光谱的理解,并可扩展到其他弗洛凯系统。