Ultrafast energizing the parity-forbidden dark exciton in black phosphorus

Guangzhen Shen, Xirui Tian, Limin Cao, Hongli Guo, Xintong Li, Yishu Tian, Xuefeng Cui, Min Feng, Jin Zhao (), Bing Wang (), Hrvoje Petek () and Shijing Tan ()
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Guangzhen Shen: University of Science and Technology of China
Xirui Tian: University of Science and Technology of China
Limin Cao: Wuhan University
Hongli Guo: Zhejiang University
Xintong Li: University of Science and Technology of China
Yishu Tian: University of Science and Technology of China
Xuefeng Cui: University of Science and Technology of China
Min Feng: Wuhan University
Jin Zhao: University of Science and Technology of China
Bing Wang: University of Science and Technology of China
Hrvoje Petek: University of Pittsburgh
Shijing Tan: University of Science and Technology of China

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract As conventional electronic materials approach their physical limits, the application of ultrafast optical fields to access transient states of matter captures imagination. The inversion symmetry governs the optical parity selection rule, differentiating between accessible and inaccessible states of matter. To circumvent parity-forbidden transitions, the common practice is to break the inversion symmetry by material design or external fields. Here we report how the application of femtosecond ultraviolet pulses can energize a parity-forbidden dark exciton state in black phosphorus while maintaining its intrinsic material symmetry. Unlike its conventional bandgap absorption in visible-to-infrared, femtosecond ultraviolet excitation turns on efficient Coulomb scattering, promoting carrier multiplication and electronic heating to ~3000 K, and consequently populating its parity-forbidden states. Interferometric time- and angle-resolved two-photon photoemission spectroscopy reveals dark exciton dynamics of black phosphorus on ~100 fs time scale and its anisotropic wavefunctions in energy-momentum space, illuminating its potential applications in optoelectronics and photochemistry under ultraviolet optical excitation.

Date: 2025
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DOI: 10.1038/s41467-025-58930-z

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