Pressure-Selective Magnetic Switching via Spatially Separated Soft Interlayer and Rigid Charge-Transfer Intralayer
Abstract
We report a pressure-responsive molecule-based magnet featuring a layered cyanido-bridged Co–W assembly, [{CoII(4-phenoxypyridine)4}3{WV(CN)8}2], exhibiting a distinct pressure-selective magnetic behavior. The compound forms two-dimensional charge-transfer layers with large interlayer separation induced by bulky ligands, enabling a dimensional crossover of magnetization from two-dimensional to three-dimensional behavior at low temperatures. Applying moderate pressure up to 0.27 GPa selectively compresses the layers, eliminating the dimensional crossover and enhancing ferromagnetic interactions, increasing both the Curie temperature and coercive field. Upon further compression, the interlayer distance reaches a limit, triggering a pressure-induced charge-transfer phase transition from the high-spin CoII–WV to the low-spin CoIII–WIV state, which weakens ferromagnetism and eventually leads to complete paramagnetic behavior at higher pressures. The difference in the compressibility between the soft interlayer regions and the rigid charge-transfer intralayer enables two-step magnetic control solely by pressure, a rare feature in molecule-based magnets. High-pressure X-ray diffraction and microscopic imaging confirm the structural sensitivity of the interlayer regions and correlate the pressure-induced phase transitions with the sequential pressure-induced color changes. These findings demonstrate that the interlayer distance and its rigid layer are key parameters for designing pressure-responsive magnetic materials, offering a new strategy for controllable molecular magnetism via external stimuli.
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BibTeX
@article{ota2026pressureselective,
title = {{Pressure-Selective Magnetic Switching via Spatially Separated Soft Interlayer and Rigid Charge-Transfer Intralayer}},
author = {Wakano Ota and Kazuki Nakamura and Gaël Privault and Haruki Taira and Riyo Nagao and Koji Nakabayashi and Eric Collet and Hirokazu Kadobayashi and Naohisa Hirao and Laurent Guérin and Shin-Ichi Ohkoshi},
journal = {Journal of the American Chemical Society},
year = {2026},
month = aug,
doi = {10.1021/jacs.6c10267},
url = {https://hal.science/hal-05743579v1},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Pressure-Selective Magnetic Switching via Spatially Separated Soft Interlayer and Rigid Charge-Transfer Intralayer
AU - Wakano Ota
AU - Kazuki Nakamura
AU - Gaël Privault
AU - Haruki Taira
AU - Riyo Nagao
AU - Koji Nakabayashi
AU - Eric Collet
AU - Hirokazu Kadobayashi
AU - Naohisa Hirao
AU - Laurent Guérin
AU - Shin-Ichi Ohkoshi
PY - 2026
DA - 2026/08/06
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c10267
UR - https://hal.science/hal-05743579v1
AB - We report a pressure-responsive molecule-based magnet featuring a layered cyanido-bridged Co–W assembly, [{CoII(4-phenoxypyridine)4}3{WV(CN)8}2], exhibiting a distinct pressure-selective magnetic behavior. The compound forms two-dimensional charge-transfer layers with large interlayer separation induced by bulky ligands, enabling a dimensional crossover of magnetization from two-dimensional to three-dimensional behavior at low temperatures. Applying moderate pressure up to 0.27 GPa selectively compresses the layers, eliminating the dimensional crossover and enhancing ferromagnetic interactions, increasing both the Curie temperature and coercive field. Upon further compression, the interlayer distance reaches a limit, triggering a pressure-induced charge-transfer phase transition from the high-spin CoII–WV to the low-spin CoIII–WIV state, which weakens ferromagnetism and eventually leads to complete paramagnetic behavior at higher pressures. The difference in the compressibility between the soft interlayer regions and the rigid charge-transfer intralayer enables two-step magnetic control solely by pressure, a rare feature in molecule-based magnets. High-pressure X-ray diffraction and microscopic imaging confirm the structural sensitivity of the interlayer regions and correlate the pressure-induced phase transitions with the sequential pressure-induced color changes. These findings demonstrate that the interlayer distance and its rigid layer are key parameters for designing pressure-responsive magnetic materials, offering a new strategy for controllable molecular magnetism via external stimuli.
SN - 0002-7863
SN - 1520-5126
ER -