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Ionic to neutral conversion induced by resonant excitation of molecular vibrations coupled to intermolecular charge transfer

T. Morimoto1, H. Suzuki1, T. Otaki1, N. Sono1, N. Kida1,2, T. Miyamoto1,2,*, and H. Okamoto1,2,†

  • 1Department of Advanced Materials Science, University of Tokyo, Kashiwa 5-1-5, Chiba 277-8561, Japan
  • 2AIST-UTokyo Advanced Operando-Measurement Technology Open Innovation Laboratory, National Institute of Advanced Industrial Science and Technology, Chiba 277-8568, Japan

  • *miyamoto@k.u-tokyo.ac.jp
  • †okamotoh@k.u-tokyo.ac.jp
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Phys. Rev. Research 3, L042028 – Published 18 November, 2021

DOI: https://doi.org/10.1103/PhysRevResearch.3.L042028

Abstract

In organic molecular compounds, intramolecular vibration is sometimes coupled with intermolecular charge transfer (CT). In such materials, vibrational excitation by a midinfrared (MIR) pulse causes collective intermolecular CTs that can be a route to an electronic-state conversion. Here, we report that an ionic-to-neutral (IN) conversion in tetrathiafulvalene-p-chloranil (TTF-CA) can be driven by a strong vibrational excitation induced by an MIR pulse. Using MIR-pump subcycle-reflectivity-probe and second-harmonic-generation-probe measurements, we discuss the coherent electron and lattice dynamics during and after the IN conversion, which are distinct from the dynamics of the photoinduced transition by electronic excitation alone.

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Information

Phys. Rev. Research 3, L042028– Published 18 November, 2021
  • Received 23 March 2020
  • Revised 16 August 2021
  • Accepted 22 October 2021
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