Université Paris-Saclay, Université Evry, CNRS, LAMBE UMR8587, 91025 Evry-Courcouronnes, France.
Department of Physics, College of Science, Princess Nourah bint Abdulrahman University, P.O. Box 84428, Riyadh 11671, Saudi Arabia.
J Chem Phys. 2023 Apr 14;158(14):144307. doi: 10.1063/5.0147313.
The spin-crossover Fe(bt)(NCS) complex is studied using spin-polarized density functional theory within the generalized gradient approximation, the Hubbard U and the weak van der Waals interactions in conjunction with the projector augmented wave method in its molecular and periodic arrangements. It is shown that the considered complex has three magnetic configurations [high spin state (HS)-HS, HS-low spin state (LS), and LS-LS] corresponding to those observed experimentally after two transition temperatures T of 163 K and T of 197 K. For the HS-HS magnetic state, we found that the two Fe centers are antiferromagnetically coupled for both molecular and periodic structures in good agreement with the experimental observations. Our results show that the computed total energy difference between the magnetic state configurations of the considered Fe complex is significantly smaller compared to those reported in the literature for other mono- or binuclear compounds.
采用自旋极化密度泛函理论（在广义梯度近似、Hubbard U 和弱范德华相互作用的基础上，结合投影缀加波方法），对自旋交叉Fe(bt)(NCS)配合物的分子和周期性结构进行了研究。结果表明，该配合物具有三种磁构象[高自旋态(HS)-HS、HS-低自旋态(LS)和 LS-LS]，与实验观测到的在 163 K 和 197 K 两个转变温度 T 1 和 T 2 之后的磁构象相对应。对于 HS-HS 磁态，我们发现两个 Fe 中心在分子和周期性结构中均呈反铁磁耦合，这与实验观测结果一致。我们的结果表明，与文献中报道的其他单核或双核化合物相比，所研究的 Fe 配合物的磁态构型之间的计算总能量差要小得多。
