Evolution of Ferromagnetic and Antiferromagnetic States in Iron Nitride Clusters FenN and FenN2 (n = 1–10),The Journal of Physical Chemistry A

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Evolution of Ferromagnetic and Antiferromagnetic States in Iron Nitride Clusters FenN and FenN2 (n = 1–10)
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2021-08-31 , DOI: 10.1021/acs.jpca.1c05769
Gennady L Gutsev ₁ , Sergey M Aldoshin ₂ , Lavrenty G Gutsev _{2,

3} , Bala R Ramachandran ₃

Affiliation

First-principles density functional theory calculations on neutral and singly negatively and positively charged iron clusters Fe_n and iron nitride clusters Fe_nN and Fe_nN₂ (n = 1–10) in the range of 1 ≤ n ≤ 10 revealed that there is a strong competition between ferromagnetic and antiferromagnetic states especially in the Fe_nN₂^0,±1 cluster series. This phenomenon was related to superexchange via a bridging N atom between two iron atoms in the Fe_nN₂^0,±1 cluster series and to a double superexchange effect via a Fe atom shared by two N atoms in the Fe_nN₂^0,±1 series. A thorough examination of the structure–energy–spin state relationships in these clusters is conducted, leading to new insights and confirmation of available experimental results on structural parameters and dissociation energetics. The bond energies of both nitrogen atoms in the Fe_nN₂ series are approximately the same. They weakly depend on the charge of the host cluster and fluctuate around 5.5 eV when moving along the series. The energy of N₂ desorption is relatively small; it varies by about 1.0 eV and depends on the charge of the cluster. The experimental finding that N₂ dissociates on the Fe_n⁺ clusters beginning with n = 4 was supported by the results of our computations. Our computed values of the Fe_n⁺–N bonding energies agree with the experimental data within the experimental uncertainty bars. It was found that the attachment of one or two N atoms does not seriously affect the polarizability, electron affinity, or ionization energy of the host iron clusters independent of the charge.

中文翻译：

氮化铁团簇 FenN 和 FenN2 中铁磁和反铁磁态的演变（n = 1-10）

第一性原理密度泛函理论计算在1 ≤ n ≤ 10范围内的中性和带单个负电荷和正电荷的铁簇 Fe _n和氮化铁簇 Fe _n N 和 Fe _n N ₂ ( n = 1-10)表明有是铁磁态和反铁磁态之间的强烈竞争，尤其是在 Fe _n N ₂^0,±1簇系列中。这种现象与通过 Fe _n N ₂^0,±1簇系列中两个铁原子之间桥接 N 原子的超交换以及通过 Fe 中两个 N 原子共享的 Fe 原子产生的双重超交换效应有关_n N₂^0,±1系列。对这些簇中的结构-能量-自旋状态关系进行了彻底检查，从而获得了新的见解并确认了有关结构参数和解离能量学的可用实验结果。Fe_n N₂系列中两个氮原子的键能大致相同。它们微弱地依赖于主机簇的电荷，并在沿串联移动时在 5.5 eV 左右波动。N₂解吸能量较小；它变化约 1.0 eV，并取决于簇的电荷。N₂在 Fe_n⁺簇上解离的实验发现我们的计算结果支持n = 4。我们计算的 Fe _n⁺ –N 键能值与实验不确定条内的实验数据一致。发现一个或两个 N 原子的附着不会严重影响与电荷无关的主体铁簇的极化率、电子亲和力或电离能。

更新日期：2021-09-16

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