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<p>Spin-crossover complexes are promising candidates for molecular bits owing to their magnetic bistability. However, it’s a formidable challenge to turn densely packed spin-crossover molecules into high-density bits due to cooperative switching dynamics inherent in spin-crossover aggregates. Herein, coordination-field engineering is demonstrated by scanning tunneling microscopy/spectroscopy and density functional theory as an efficient strategy to modulate the cooperative dynamics of surface-confined spin-crossover chains. Within these chains, Ni centers exhibit collective spin transitions upon local stimuli. This spin-crossover cooperativity can be disrupted by coordination-field modification via hetero-metal/ligand doping, which converts partial switchable coordination centers into non-switchable nodes. These nodes divide the single-bit-like spin-crossover chain into multiple independently-switchable segments and thereby augment the bit density. One-by-one erasable write-in of these spin-crossover bits is achieved by scanning tunneling microscope tip manipulation. These results highlight how to precisely tweak the cooperative dynamics of the spin-crossover aggregates to advance their potential applications for high-density memory.</p>

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Atomically tweaking spin-crossover cooperativity to augment molecular memory density

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月23日

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  • Jing Liu,
  • Yuchen Bai,
  • Zhen Xu,
  • Qiwei Chen,
  • Jinliang Pan,
  • Yuxuan Lin,
  • Ting Hu,
  • Haoyang Deng,
  • Yifan Gao,
  • Li Huang,
  • Yongfeng Wang,
  • Kai Wu

摘要

Spin-crossover complexes are promising candidates for molecular bits owing to their magnetic bistability. However, it’s a formidable challenge to turn densely packed spin-crossover molecules into high-density bits due to cooperative switching dynamics inherent in spin-crossover aggregates. Herein, coordination-field engineering is demonstrated by scanning tunneling microscopy/spectroscopy and density functional theory as an efficient strategy to modulate the cooperative dynamics of surface-confined spin-crossover chains. Within these chains, Ni centers exhibit collective spin transitions upon local stimuli. This spin-crossover cooperativity can be disrupted by coordination-field modification via hetero-metal/ligand doping, which converts partial switchable coordination centers into non-switchable nodes. These nodes divide the single-bit-like spin-crossover chain into multiple independently-switchable segments and thereby augment the bit density. One-by-one erasable write-in of these spin-crossover bits is achieved by scanning tunneling microscope tip manipulation. These results highlight how to precisely tweak the cooperative dynamics of the spin-crossover aggregates to advance their potential applications for high-density memory.