Terahertz Sum-Frequency Excitation of a Raman-Active Phonon

Sebastian Maehrlein, Alexander Paarmann, Martin Wolf, and Tobias Kampfrath
Phys. Rev. Lett. 119, 127402 – Published 22 September 2017
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Abstract

In stimulated Raman scattering, two incident optical waves induce a force oscillating at the difference of the two light frequencies. This process has enabled important applications such as the excitation and coherent control of phonons and magnons by femtosecond laser pulses. Here, we experimentally and theoretically demonstrate the so far neglected up-conversion counterpart of this process: THz sum-frequency excitation of a Raman-active phonon mode, which is tantamount to two-photon absorption by an optical transition between two adjacent vibrational levels. Coherent control of an optical lattice vibration of diamond is achieved by an intense terahertz pulse whose spectrum is centered at half the phonon frequency of 40 THz. Remarkably, the carrier-envelope phase of the THz pulse is directly transferred into the phase of the lattice vibration. New prospects in general infrared spectroscopy, action spectroscopy, and lattice trajectory control in the electronic ground state emerge.

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  • Received 9 March 2017

DOI:https://doi.org/10.1103/PhysRevLett.119.127402

© 2017 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & OpticalCondensed Matter, Materials & Applied Physics

Authors & Affiliations

Sebastian Maehrlein1,*, Alexander Paarmann1, Martin Wolf1, and Tobias Kampfrath1,2

  • 1Department of Physical Chemistry, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195 Berlin, Germany
  • 2Department of Physics, Freie Universität Berlin, Arnimallee 14, 14195 Berlin, Germany

  • *maehrlein@fhi-berlin.mpg.de

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Issue

Vol. 119, Iss. 12 — 22 September 2017

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