预测Fe Mössbauer核四极分裂与混合和双混合密度函数的57
Yihao Zhang1,2, Haonan Tang1,3, Wenli Zou1,3
1Institute of Modern Physics, Northwest University, Xi'an 710127, China.
International journal of molecular sciences
|March 27, 2025
概括
准确预测核四极分裂 (NQS) 是一个挑战. 双混合功能 PBE-0DH 和混合功能 rSCAN38 对含铁分子有前途,指导未来的密度功能发展.
科学领域:
- 计算化学的计算化学
- 量子化学 是一个量子化学.
- 频谱学是一种光谱学.
背景情况:
- 核四极分裂 (NQS) 在Mössbauer光谱学中至关重要.
- 准确的NQS理论预测是具有挑战性的,因为依赖于方法.
- 新兴的密度函数为改进NQS研究提供了潜力.
研究的目的:
- 评估11个混合和12个双混合密度函数用于NQS预测.
- 评估32个含铁分子的性能,包括相对论效应.
- 确定可靠的Mössbauer光谱的功能,并指导未来的发展.
主要方法:
- 计算了32个含铁分子 (约70个原子) 的NQS值.
- 采用精确的双组分 (X2C) 汉密尔顿式来实现嵌入的标量相对论效应.
- 评估了11个混合动力和12个双混合动力密度函数,包括新的函数.
主要成果:
- PBE-0DH (双混合动力) 实现了最佳性能 (MAE = 0.20 mm/s).
- rSCAN38 (混合动力) 是最佳的混合动力功能 (MAE = 0.25 mm/s) 具有更好的效率.
- 由于静态相关性,具有>10%精确交换的混合功能对铁素失败;双混合物表现更好.
结论:
- 对于Mössbauer NQS计算,建议使用 PBE-0DH 和 rSCAN38.
- 密度函数理论 (DFT) 与强大的静态相关性 (例如[Fe(H2O) 5NO]2+,FeO2− - 氨酸) 相斗争.
- 对于具有强烈静态相关性的系统,需要多配置方法.
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