Strong Local-Field Enhancement of the Nonlinear Soft-Mode Response in a Molecular Crystal

Giulia Folpini, Klaus Reimann, Michael Woerner, Thomas Elsaesser, Johannes Hoja, and Alexandre Tkatchenko
Phys. Rev. Lett. 119, 097404 – Published 1 September 2017
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Abstract

The nonlinear response of soft-mode excitations in polycrystalline acetylsalicylic acid (aspirin) is studied with two-dimensional terahertz spectroscopy. We demonstrate that the correlation of CH3 rotational modes with collective oscillations of π electrons drives the system into the nonperturbative regime of light-matter interaction, even for a moderate strength of the THz driving field on the order of 50kV/cm. Nonlinear absorption around 1.1 THz leads to a blueshifted coherent emission at 1.7 THz, revealing the dynamic breakup of the strong electron-phonon correlations. The observed behavior is reproduced by theoretical calculations including dynamic local-field correlations.

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  • Received 21 December 2016

DOI:https://doi.org/10.1103/PhysRevLett.119.097404

© 2017 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Giulia Folpini, Klaus Reimann, Michael Woerner*, and Thomas Elsaesser

  • Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie, 12489 Berlin, Germany

Johannes Hoja and Alexandre Tkatchenko

  • Physics and Materials Science Research Unit, University of Luxembourg, L-1511 Luxembourg, Luxembourg and Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany

  • *woerner@mbi-berlin.de
  • alexandre.tkatchenko@uni.lu

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Issue

Vol. 119, Iss. 9 — 1 September 2017

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