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Transient birefringence of liquids induced by terahertz electric-field torque on permanent molecular dipoles

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  • Mohsen Sajadi

    (Fritz Haber Institute of the Max Planck Society)

  • Martin Wolf

    (Fritz Haber Institute of the Max Planck Society)

  • Tobias Kampfrath

    (Fritz Haber Institute of the Max Planck Society)

Abstract

Collective low-frequency molecular motions have large impact on chemical reactions and structural relaxation in liquids. So far, these modes have mostly been accessed indirectly by off-resonant optical pulses. Here, we provide evidence that intense terahertz (THz) pulses can resonantly excite reorientational-librational modes of aprotic and strongly polar liquids through coupling to the permanent molecular dipole moments. We observe a significantly enhanced response because the transient optical birefringence is up to an order of magnitude higher than obtained with optical excitation. Frequency-dependent measurements and a simple analytical model indicate that the enhancement arises from resonantly driven librations and their coupling to reorientational motion, assisted by the pump field and/or a cage translational mode. Our results open up the path to applications such as efficient molecular alignment, enhanced transient Kerr signals and systematic resonant nonlinear THz spectroscopy of the coupling between intermolecular modes in liquids.

Suggested Citation

  • Mohsen Sajadi & Martin Wolf & Tobias Kampfrath, 2017. "Transient birefringence of liquids induced by terahertz electric-field torque on permanent molecular dipoles," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms14963
    DOI: 10.1038/ncomms14963
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