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<p>Anharmonic lattice vibrations play a key role in many physical phenomena. The most direct evidence for anharmonicity is a measurement of the oscillation frequency as a function of the amplitude. For Raman-active lattice vibrations, this is not a trivial task, and anharmonicity is typically probed indirectly. Thus, direct measurement and control of the anharmonicity of a single Raman mode is still lacking. We show that ultrafast double pump-probe spectroscopy could be used to directly observe frequency shifts of Raman phonons as a function of the oscillation amplitude and disentangle the coherent contributions from quasi-harmonic sources such as temperature and changes to the carrier density in SnTe and SnSe. Moreover, we show that coherent displacive phononic excitation in tandem with electron-phonon coupling is a pathway to control phonon anharmonicity dynamically. Finally, our methodology could be used to isolate the basic mechanisms driving nonlinear optical phenomena based on their unique timestamps.</p>

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Coherent control through phonon anharmonicity

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月27日

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  • Gili Scharf,
  • Tomer Hasharoni,
  • Lara Donval,
  • Leah Ben Gur,
  • Alon Ron

摘要

Anharmonic lattice vibrations play a key role in many physical phenomena. The most direct evidence for anharmonicity is a measurement of the oscillation frequency as a function of the amplitude. For Raman-active lattice vibrations, this is not a trivial task, and anharmonicity is typically probed indirectly. Thus, direct measurement and control of the anharmonicity of a single Raman mode is still lacking. We show that ultrafast double pump-probe spectroscopy could be used to directly observe frequency shifts of Raman phonons as a function of the oscillation amplitude and disentangle the coherent contributions from quasi-harmonic sources such as temperature and changes to the carrier density in SnTe and SnSe. Moreover, we show that coherent displacive phononic excitation in tandem with electron-phonon coupling is a pathway to control phonon anharmonicity dynamically. Finally, our methodology could be used to isolate the basic mechanisms driving nonlinear optical phenomena based on their unique timestamps.