Coherent manipulation of second-harmonic generation via terahertz-field mediated phonon-polariton in zinc oxide

Yifei Fang, Jiajing Hao, Jianhua Sang, Jixing Gao, Liwei Song (), Ye Tian () and Ruxin Li ()
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Yifei Fang: Chinese Academy of Sciences
Jiajing Hao: Chinese Academy of Sciences
Jianhua Sang: Chinese Academy of Sciences
Jixing Gao: Chinese Academy of Sciences
Liwei Song: Chinese Academy of Sciences
Ye Tian: Chinese Academy of Sciences
Ruxin Li: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract The coherent control of phonon polaritons (PhPs) in holds transformative potential for nonlinear photonics. We demonstrate terahertz-driven excitation of low-frequency PhPs in zinc oxide (ZnO) crystals, with their nonlinear dynamics resolved via time-resolved second harmonic generation (SHG) spectroscopy. By achieving phase matching via nine sequential reflections within a millimeter-scale crystal, we observe sustained SHG oscillations with 3-4 THz modulation frequencies, achieving optimal extinction ratios of ~18 dB that persist for 90 picoseconds—a temporal span directly governed by polariton propagation dynamics. This work establishes a dual-functionality platform enabling spectral-temporal resolved mapping of quasiparticle interaction dynamics while simultaneously advancing polariton-engineered nonlinear optical modulators through symmetry-broken frequency conversion architectures.

Date: 2025
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DOI: 10.1038/s41467-025-60851-w

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