多重共振型BN分子的计算设计,用于反转单元和三元激发状态
Yong-Jin Pu1, Danillo Valverde2, Juan Carlos Sancho-García3
1RIKEN Center for Emergent Matter Science (CEMS), Wako, Saitama 351-0198, Japan.
The journal of physical chemistry. A
|November 27, 2023
概括
研究人员通过计算设计了和化物 (BN) 分子,用于有机电子产品的潜在用途. 这些分子表现出负单元-三元差距 (ΔEST),对于先进的应用至关重要.
科学领域:
- 计算化学计算化学
- 材料科学 材料科学 材料科学
- 有机电子 有机电子
背景情况:
- 设计具有特定电子性质的分子是先进材料的关键.
- 多重共振热激活延迟光 (MR-TADF) 材料需要精确控制单元-三元能量差距 (ΔEST).
研究的目的:
- 为了计算设计新的线性扩展多重共振 (MR) 型BN分子.
- 为了研究这些分子表现出负单元-三元差距 (ΔEST) 和大振荡器强度的潜力.
- 探索电子相关性在确定MR-TADF和反向单点三点间隙化合物的ΔEST中的作用.
主要方法:
- 在时间依赖密度函数理论 (TD-DFT) 框架内利用双混合函数.
- 采用基于波函数的方法,包括带有单元和双元的运动方程合集群 (EOM-CCSD) 和对称性调整的CC2 (SCS-CC2).
- 系统地研究了电子关联对单元和三元激发状态的影响.
主要成果:
- 随着 (B) 和 (N) 原子数量的增加,观察到 ΔEST 的逐渐减少.
- 一些设计的分子达到负的 ΔEST 值,表明反转的单元-三元能量水平.
- 计算的振荡器强度大于阿扎芬类分子的强度,具有反向单元-三元激发状态.
结论:
- 双混合函数提供了准确的 ΔEST 预测,与高级量子力学方法和实验数据保持一致.
- BN分子的尺寸和组成显著影响了它们的 ΔEST.
- 这项研究为设计具有负 ΔEST 的新型和添加剂的多芳香碳化合物为潜在的光电子应用提供了基础.
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