大学化学 >> 2025, Vol. 40 >> Issue (3): 178-185.doi: 10.12461/PKU.DXHX202406024

所属专题: 理论与计算化学在化学及其交叉学科教学中的应用

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应用量化计算理解水分子的振动斯塔克效应

赵素品, 谢静   

  1. 北京理工大学化学与化工学院, 北京 102488
  • 收稿日期:2024-06-11 录用日期:2024-08-15 发布日期:2025-03-19
  • 通讯作者: 谢静 E-mail:jingxie@bit.edu.cn
  • 基金资助:
    国家自然科学基金(21903004,22273004)

Understanding the Vibrational Stark Effect of Water Molecules Using Quantum Chemistry Calculations

Supin Zhao, Jing Xie   

  1. School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
  • Received:2024-06-11 Accepted:2024-08-15 Published:2025-03-19
  • Contact: Jing Xie E-mail:jingxie@bit.edu.cn

摘要: 振动斯塔克效应(vibrational Stark effect)是指振动光谱在外加电场作用下发生移动的现象,该效应在现代化学中有广泛的应用。为了增进对振动斯达克效应的理解,本文选择了水的单分子H2O和二聚体分子(H2O)2,通过密度泛函理论计算展示了外加定向电场对这两个分子的振动频率的影响。计算显示,外加定向电场直接影响分子的几何结构、电荷密度、偶极矩、能量,以及振动频率。随着电场强度的增大,H2O和(H2O)2分子的红外振动光谱都出现了收缩现象,即高频的O―H伸缩振动红移,而低频的H―O―H弯曲振动蓝移,这与文献中模拟结果一致。本文为理解振动斯塔克效应提供了一个简单清晰的理论计算案例。

关键词: 斯塔克效应, 定向外电场, 量子化学计算, 红外光谱

Abstract: The vibrational Stark effect refers to the infrared spectral lines shifting when exposed to an external electric field. This effect has broad applications in modern chemistry. To facilitate the understanding of the vibrational Stark effect, we selected two water molecules for study, i.e., the monomer H2O and the dimer (H2O)2. Using density functional theory calculations, we investigated the influence of an applied electric field directly affects the targeted molecules' geometry, electron density, dipole moment, energy, and vibrational frequencies. As the field strength increases, both H2O and (H2O)2 exhibits spectral shrink, with a redshift of the high-frequency O―H stretching vibrations and a blueshift of the lower-frequency H―O―H bending vibrations. These findings are consistent with previous simulation results reported in the literature. This work provides a straightforward and clear computational case for understanding the vibrational Stark effect.

Key words: Stark effect, Oriented external electric fields, Quantum chemical calculation, Infrared vibration spectrum