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Ultrafast charge-transfer-induced spin transition in cobalt-tungstate molecular photomagnets

Author

Listed:
  • Kazuki Nakamura

    (The University of Tokyo
    Department of Chemistry)

  • Laurent Guérin

    (Department of Chemistry
    IPR (Institut de Physique) - UMR 6251)

  • Gaël Privault

    (Department of Chemistry
    IPR (Institut de Physique) - UMR 6251)

  • Koji Nakabayashi

    (The University of Tokyo
    Department of Chemistry)

  • Marius Hervé

    (Department of Chemistry
    IPR (Institut de Physique) - UMR 6251)

  • Eric Collet

    (Department of Chemistry
    IPR (Institut de Physique) - UMR 6251
    Institut Universitaire de France (IUF))

  • Shin-ichi Ohkoshi

    (The University of Tokyo
    Department of Chemistry)

Abstract

In materials exhibiting photoinduced phase transitions, and in which both charge transfer and spin transitions occur, there has long been a debate about which process drives the phase transition. Herein, we present experimental evidence supporting an optically charge-transfer-induced spin transition (CTIST) process, as demonstrated through femtosecond optical spectroscopy in two-dimensional cyanido-bridged cobalt-tungstate photomagnets. Optical and magnetic studies revealed that the photoexcitation of the ground low-temperature (LT) CoIIILS-WIV state leads to a photoinduced phase transition towards the CoIIHS-WV state, which is similar to the high temperature (HT) state. Ultrafast spectroscopy further indicates that this optical excitation of the intermetallic W-to-Co charge-transfer band produces a transient photoexcited (PE) CoIILS-WV state, which decays within 130 fs through a spin transition towards the CoIIHS-WV state. Here we show that the CTIST dynamics corresponds to the CoIIILS-WIV (LT) → CoIILS-WV (PE) → CoIIHS-WV (HT) sequence. The present work sheds a new light on understanding optical dynamics underlying the photoinduced phase transitions.

Suggested Citation

  • Kazuki Nakamura & Laurent Guérin & Gaël Privault & Koji Nakabayashi & Marius Hervé & Eric Collet & Shin-ichi Ohkoshi, 2025. "Ultrafast charge-transfer-induced spin transition in cobalt-tungstate molecular photomagnets," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-60401-4
    DOI: 10.1038/s41467-025-60401-4
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    1. Wenkai Zhang & Roberto Alonso-Mori & Uwe Bergmann & Christian Bressler & Matthieu Chollet & Andreas Galler & Wojciech Gawelda & Ryan G. Hadt & Robert W. Hartsock & Thomas Kroll & Kasper S. Kjær & Kath, 2014. "Tracking excited-state charge and spin dynamics in iron coordination complexes," Nature, Nature, vol. 509(7500), pages 345-348, May.
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