液态甲胺中双稳态溶剂化双电子:神秘的自旋交叉动力学及双电子交换

doi:10.6040/j.issn.1671-9352.9.2021.013

摘要/Abstract

摘要： 本文利用从头算分子动力学模拟研究了一类普适液体介质(液态甲胺)中溶剂化双电子的结构及动力学行为,揭示了其独特的结构特征及时间演化动力学, 特别是发现了溶剂化双电子具有迷人的自旋交叉动力学特征,是一类双稳态的双极化子。模拟结果表明,液态甲胺中2个电子优先定域于2个独立的溶剂笼,且进行非协同时间演化。单态时具有稳态动力学演化特征,而三态时则表现为电子交换动力学。非常有趣的是单态及三态轨迹均表明此类动态双极化子展现了双稳态,在时间演化上呈现铁磁态与反铁磁态之间频繁的自旋转换。本工作首次详细报道了一类广泛应用液态介质中双稳态溶剂化双电子的动态自旋交叉现象及动力学规律,为探索此类磁性液体的实际应用提供了新的见解。

关键词: 溶剂化双电子, 双稳态双极化子, 自旋交叉动力学, 电子迁移, 从头算分子动力学模拟自我评价

Abstract: We present a detailed ab initio molecular dynamics simulation study on solvated dielectron in a type of commonly used liquid medium(liquid methylamine)and reveal unique structures and time evolution dynamics of two excess electrons. We particularly unravel intriguing spin crossover dynamics character of a solvated dielectron which features a bistable bipolaron. Our simulation results indicate that a dielectron in liquid methylamine prefers to accommodate into two independent cavities and evolves non-synchronously with steady dynamics in the singlet state or electron exchange dynamics in the triplet state. More interestingly, both trajectories reveal that the dynamic bipolaron exhibits bistability with frequent spin crossovers between the ferromagnetic and antiferromagnetic states in time evolution. This work presents the first detailed study on the dynamic spin crossover phenomenon of a bistable solvated dielectron in a commonly used liquid medium and provides novel insights into the magnetic liquids for promising applications.

Key words: solvated dielectron, bistable bipolaron, spin crossover dynamics, electron migration, ab initio molecular dynamics simulation

中图分类号:

O641.12+1

步宇翔, 罗奇. 液态甲胺中双稳态溶剂化双电子:神秘的自旋交叉动力学及双电子交换[J]. 《山东大学学报(理学版)》, 2021, 56(10): 113-126.

BU Yuxiang, LUO Qi. Bistable solvated dielectron in liquid methylamine: intriguing spin crossover dynamics and dielectron exchanges[J]. JOURNAL OF SHANDONG UNIVERSITY(NATURAL SCIENCE), 2021, 56(10): 113-126.

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