自旋电子学
堆积
化学物理
化学
凝聚态物理
极化子
自旋(空气动力学)
金属有机骨架
纳米技术
铁磁性
材料科学
物理
物理化学
电子
量子力学
热力学
吸附
有机化学
作者
Lijun Yang,Ziqi Hu,Petko St. Petkov,Shuai Fu,Haoyuan Qi,Chuanhui Huang,Yannan Liu,Xing Huang,Mingchao Wang,Peng Zhang,Ute Kaiser,Mischa Bonn,Hai I. Wang,Paolo Samorı́,Eugenio Coronado,Renhao Dong,Xinliang Feng
摘要
Two-dimensional conjugated metal–organic frameworks (2D c-MOFs) have attracted increasing interest in electronics due to their (semi)conducting properties. Charge-neutral 2D c-MOFs also possess persistent organic radicals that can be viewed as spin-concentrated arrays, affording new opportunities for spintronics. However, the strong π-interaction between neighboring layers of layer-stacked 2D c-MOFs annihilates active spin centers and significantly accelerates spin relaxation, severely limiting their potential as spin qubits. Herein, we report the precise tuning of the charge transport and spin dynamics in 2D c-MOFs via the control of interlayer stacking. The introduction of bulky side groups on the conjugated ligands enables a significant dislocation of the 2D c-MOFs layers from serrated stacking to staggered stacking, thereby spatially weakening the interlayer interactions. As a consequence, the electrical conductivity of 2D c-MOFs decreases by 6 orders of magnitude, while the spin density achieves more than a 30-fold increase and the spin–lattice relaxation time (T1) is increased up to ∼60 μs, hence being superior to the reference 2D c-MOFs with compact stackings whose spin relaxation is too fast to be detected. Spin dynamics results also reveal that spinless polaron pairs or bipolarons play critical roles in the charge transport of these 2D c-MOFs. Our strategy provides a bottom-up approach for enlarging spin dynamics in 2D c-MOFs, opening up pathways for developing MOF-based spintronics.
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