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Ultrafast energizing the parity-forbidden dark exciton in black phosphorus

Author

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  • Guangzhen Shen

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Xirui Tian

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Limin Cao

    (Wuhan University)

  • Hongli Guo

    (Zhejiang University)

  • Xintong Li

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Yishu Tian

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Xuefeng Cui

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Min Feng

    (Wuhan University)

  • Jin Zhao

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Bing Wang

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Hrvoje Petek

    (University of Pittsburgh)

  • Shijing Tan

    (University of Science and Technology of China
    University of Science and Technology of China)

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.

Suggested Citation

  • Guangzhen Shen & Xirui Tian & Limin Cao & Hongli Guo & Xintong Li & Yishu Tian & Xuefeng Cui & Min Feng & Jin Zhao & Bing Wang & Hrvoje Petek & Shijing Tan, 2025. "Ultrafast energizing the parity-forbidden dark exciton in black phosphorus," Nature Communications, Nature, vol. 16(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-58930-z
    DOI: 10.1038/s41467-025-58930-z
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    1. Xingxia Cui & Ding Han & Hongli Guo & Linwei Zhou & Jingsi Qiao & Qing Liu & Zhihao Cui & Yafei Li & Chungwei Lin & Limin Cao & Wei Ji & Hrvoje Petek & Min Feng, 2019. "Realizing nearly-free-electron like conduction band in a molecular film through mediating intermolecular van der Waals interactions," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    2. Kai-Qiang Lin & Jonas D. Ziegler & Marina A. Semina & Javid V. Mamedov & Kenji Watanabe & Takashi Taniguchi & Sebastian Bange & Alexey Chernikov & Mikhail M. Glazov & John M. Lupton, 2022. "High-lying valley-polarized trions in 2D semiconductors," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. T. Kazimierczuk & D. Fröhlich & S. Scheel & H. Stolz & M. Bayer, 2014. "Giant Rydberg excitons in the copper oxide Cu2O," Nature, Nature, vol. 514(7522), pages 343-347, October.
    4. Jingsi Qiao & Xianghua Kong & Zhi-Xin Hu & Feng Yang & Wei Ji, 2014. "High-mobility transport anisotropy and linear dichroism in few-layer black phosphorus," Nature Communications, Nature, vol. 5(1), pages 1-7, December.
    5. Shaohua Zhou & Changhua Bao & Benshu Fan & Hui Zhou & Qixuan Gao & Haoyuan Zhong & Tianyun Lin & Hang Liu & Pu Yu & Peizhe Tang & Sheng Meng & Wenhui Duan & Shuyun Zhou, 2023. "Pseudospin-selective Floquet band engineering in black phosphorus," Nature, Nature, vol. 614(7946), pages 75-80, February.
    6. Marcel Reutzel & Andi Li & Zehua Wang & Hrvoje Petek, 2020. "Coherent multidimensional photoelectron spectroscopy of ultrafast quasiparticle dressing by light," Nature Communications, Nature, vol. 11(1), pages 1-5, December.
    7. Tianju Zhang & Chaocheng Zhou & Xuezhen Feng & Ningning Dong & Hong Chen & Xianfeng Chen & Long Zhang & Jia Lin & Jun Wang, 2022. "Regulation of the luminescence mechanism of two-dimensional tin halide perovskites," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    8. David Schmitt & Jan Philipp Bange & Wiebke Bennecke & AbdulAziz AlMutairi & Giuseppe Meneghini & Kenji Watanabe & Takashi Taniguchi & Daniel Steil & D. Russell Luke & R. Thomas Weitz & Sabine Steil & , 2022. "Formation of moiré interlayer excitons in space and time," Nature, Nature, vol. 608(7923), pages 499-503, August.
    9. Ziliang Ye & Ting Cao & Kevin O’Brien & Hanyu Zhu & Xiaobo Yin & Yuan Wang & Steven G. Louie & Xiang Zhang, 2014. "Probing excitonic dark states in single-layer tungsten disulphide," Nature, Nature, vol. 513(7517), pages 214-218, September.
    10. Jianhui Fu & Qiang Xu & Guifang Han & Bo Wu & Cheng Hon Alfred Huan & Meng Lee Leek & Tze Chien Sum, 2017. "Hot carrier cooling mechanisms in halide perovskites," Nature Communications, Nature, vol. 8(1), pages 1-9, December.
    11. Hyungjin Kim & Shiekh Zia Uddin & Der-Hsien Lien & Matthew Yeh & Nima Sefidmooye Azar & Sivacarendran Balendhran & Taehun Kim & Niharika Gupta & Yoonsoo Rho & Costas P. Grigoropoulos & Kenneth B. Croz, 2021. "Actively variable-spectrum optoelectronics with black phosphorus," Nature, Nature, vol. 596(7871), pages 232-237, August.
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