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

Kazuki Nakamura, Laurent Guérin, Gaël Privault, Koji Nakabayashi (), Marius Hervé, Eric Collet () and Shin-ichi Ohkoshi ()
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Kazuki Nakamura: The University of Tokyo
Laurent Guérin: Department of Chemistry
Gaël Privault: Department of Chemistry
Koji Nakabayashi: The University of Tokyo
Marius Hervé: Department of Chemistry
Eric Collet: Department of Chemistry
Shin-ichi Ohkoshi: The University of Tokyo

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-60401-4

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