Design of a One-Dimensional Stacked Spin Peierls System with Room-Temperature Switching from Quantum Mechanical Predictions
Design of a One-Dimensional Stacked Spin Peierls System with Room-Temperature Switching from Quantum Mechanical Predictions
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根据量子力学预测设计具有室温切换的一维堆叠自旋 Peierls 系统
DOI：
10.1021/acs.jpclett.9b02219
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发表时间：
2019
期刊：
影响因子：
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通讯作者：
Xiao-Ming Ren
中科院分区：
文献类型：
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作者：
Hao Yang;Tao Cheng;William A. Goddard III;Xiao-Ming Ren
平面双-1,2-二硫代烯络合物阴离子的过渡金属（表示为[M(dithiolato)2] -和M = Ni， Pd或Pt离子）有利于在晶体中形成具有S = 1/2自旋链的阴离子柱状堆积，并且这种自旋链化合物经常经历自旋-佩尔斯型转变，使其成为导电和磁开关的有前途的材料。然而，目前的例子表明，对于大多数应用来说，转变温度太低了。我们利用量子力学预测，在自旋-佩尔斯型[Ni（二硫代酸）2]−配合物中，将阳离子排列从船型改变为椅型排列将大大稳定反铁磁耦合，显著提高转变温度。我们估计，带有椅子型阳离子填料的[Ni(mnt)2]基配合物（mnt =马来腈二硫酯）将分别导致S-、Se-和te -基mnt的临界温度分别为~ 170、~ 252和~ 310 K。我们还建议如何稳定这些系统的椅子型配置。
Planar bis-1,2-dithiolene complex anions of a transition metal (denoted as [M(dithiolato)2]−and M = Ni, Pd, or Pt ion) favor forming columnar stacks of anions in the crystal that feature S = 1/2 spin-chains, and such a spin-chain compound often undergoes a spin-Peierls-type transition, making this a promising material for conducting and magnetic switching. However, current examples show the transition temperatures are far too low for most applications. We use quantum mechanics to predict that changing the cation arrangement from the boat-type to the chair-type packing configuration in a spin-Peierls-type [Ni(dithiolato)2]−complex will substantially stabilize the antiferromagnetic coupling, dramatically increasing the transition temperature. We estimate that the [Ni(mnt)2]-based complexes (mnt = maleonitriledithiolate) with chair-type packing of cations will lead to critical temperatures of ∼170, ∼252, and ∼310 K for S-, Se-, and Te-based mnt, respectively. We also suggest how to stabilize the chair-type configurations of these systems.