Relationship between hydrogen bond network dynamics of water and its terahertz spectrum

Duan Tong-Chuan; Yan Shao-Jian; Zhao Yan; Sun Ting-Yu; Li Yang-Mei; Zhu Zhi

doi:10.7498/aps.70.20211731

Abstract

Water is the source of all life. The understanding of the terahertz absorption spectrum of water is the prerequisite for the application of terahertz technology to biomedicine. The choice of terahertz frequency is essential for achieving the biological effects of terahertz with high efficiency and low energy consumption. The complex hydrogen bond network of water possesses a broad terahertz absorption peak. Therefore, it is necessary to study the relation between the dynamics of the hydrogen bond network of water and its terahertz absorption spectrum. However, the research in this field is still lacking. Using molecular dynamics simulation methods, the terahertz absorption spectra of different water models at room temperature and pressure are studied in this work. Furthermore, taking the temperature as a variable, the dependence of the terahertz absorption spectrum of water on the strength of the hydrogen bond network is explored. It is found that rising temperature makes the terahertz absorption spectrum of the hydrogen bond network red-shift, indicating that the center frequency of the spectrum is strongly correlated with the strength of the hydrogen bond. Further studies show that there is a linear relationship between the hydrogen bond lifetime of water and the center frequency of vibration absorption peak of the hydrogen bond network. The underlying mechanism can be disclosed by imitating the hydrogen bonds in the hydrogen bond network as springs then using the spring oscillator model. These findings are conducive to understanding in depth the complex hydrogen bond network dynamics in water and promoting the study of terahertz biological effects.

Keywords:

terahertz /
water /
hydrogen bond

Authors and contacts

1.
Key Laboratory of Optical Technology and Instrument for Medicine, Ministry of Education, College of Optical-Electrical and Computer Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China
2.
Innovation Laboratory of Terahertz Biophysics, National Innovation Institute of Defense Technology, Beijing 100071, China

Corresponding author: Li Yang-Mei, sunberry1211@hotmail.com ; Zhu Zhi, zhuzhi@usst.edu.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2021YFA1200404), the National Natural Science Foundation of China (Grant No. 11904231), the Sailing Program of Shanghai, China (Grant No. 19YF1434100), and the National Defense Technology Innovation Special Zone, China.

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References

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Cited By

图 1 太赫兹与生物分子的密切关系以及太赫兹调控细胞动力学　(a) 生物大分子的转/振动的频率在THz频段; (b) 水的太赫兹吸收谱, 绿色区域是有望非热地调控生物分子的广义太赫兹频率的4个窗口; (c) 水的太赫兹吸收谱的振动模式^[36]; (d) 太赫兹波非热调控细胞动力学, 涉及发挥细胞生物功能的水通道蛋白、DNA、钾离子通道、钙离子通道

Figure 1. Close relationship between terahertz and biomolecules and the regulation of cell dynamics by terahertz: (a) Frequency of rotation/vibration of biological macromolecules is in the THz frequency band; (b) terahertz absorption spectrum of water, the green region is the four frequency windows in which electromagnetic wave is expected to non-thermally regulate biomolecules; (c) vibration modes of water corresponding to its terahertz absorption spectrum^[36]; (d) terahertz waves non-thermally regulate the dynamics of a cell, involving aquaporins, DNA, potassium and calcium channels that perform biological functions of the cell.

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图 2 不同水模型建模的体相水的太赫兹吸收谱和温度对其太赫兹吸收谱的影响　(a) 不同水模型建模的体相水的太赫兹吸收光谱以及实验测量所得体相水的太赫兹吸收谱之间的对比; (b) 对于不同水模型构成的体相水, 其氢键网络的太赫兹吸收谱; (c) 不同温度下, SPC/E水模型建模的体相水的太赫兹吸收谱; (d) 不同温度下, 对于SPC/E水模型构成的体相水, 其氢键网络的太赫兹吸收谱

Figure 2. THz absorption spectra of bulk water modeled by different water models and effects of temperature on its spectra: (a) Comparison of THz absorption spectra of bulk water under different water models and its spectra from experimental measurement; (b) THz absorption spectra of hydrogen bond network of bulk water under different water models; (c) THz absorption spectra of bulk water modeled by SPC/E water model at different temperatures; (d) THz absorption spectra of hydrogen bond network of bulk water modeled by SPC/E water model at different temperatures.

DownLoad: Full-Size Img PowerPoint

图 3 不同水模型构成的体相水的结构和动力学性质的分析　(a) 不同水模型构成的体相水的径向分布函数; (b) 不同水模型构成的体相水的扩散系数; (c) 特定的水模型(SPC/E)下, 温度对体相水的径向分布函数的影响; (d) 不同温度下SPC/E的扩散系数

Figure 3. Analyses of structure and dynamic behavior of bulk water modeled by different water models: (a) Radial distribution function of bulk water under different water models; (b) diffusion coefficient of bulk water under different water models; (c) under specific water model (SPC/E), the effect of temperature on the radial distribution function of bulk water; (d) diffusion coefficient of bulk water at different temperatures.

DownLoad: Full-Size Img PowerPoint

图 4 氢键动力学与氢键网络振动的太赫兹吸收峰的中心频率之间的关系　(a) 由不同水模型构成的体相水的氢键的自相关函数; (b) 由不同水模型构成的体相水的氢键寿命; (c) 不同水模型下, 氢键网络振动的太赫兹吸收谱的中心频率与氢键寿命的对应关系; (d) 不同温度下, 体相水的氢键寿命; (e) 不同温度下, 水的氢键网络振动的太赫兹吸收峰的中心频率与氢键寿命的关系; (f) 氢键网络示意图

Figure 4. Relationship between hydrogen bond dynamics and the center frequency of THz absorption spectra for the vibration of hydrogen bond network: (a) Hydrogen bond autocorrelation functions of bulk water under different water models; (b) lifetime of hydrogen bond of bulk water under different water models; (c) for bulk water under different water models, the relationship between the center frequency of THz absorption spectra for the vibration of hydrogen bond network and the lifetime of hydrogen bond; (d) lifetime of hydrogen bond for bulk water at different temperatures; (e) at different temperatures, the relationship between the center frequency of THz absorption spectra for the vibration of the hydrogen bond network and the lifetime of the hydrogen bond; (f) schematic diagram of the hydrogen bond network.

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表 1 所用水模型的力场参数的比较

Table 1. Comparison of the force field parameters of different water models employed.

Water model	σ_O—O/Å	ε_OO/(kJ·mol^–1)	q_H/e	q_O or q_vir/e	θ/(°)	r_H—O/Å
SPC	3.166	0.650	0.410	–0.820	109.470	1.000
SPC/E	3.166	0.650	0.424	–0.848	109.470	1.000
TIP3P	3.151	0.636	0.417	–0.834	104.520	0.957
TIP4P	3.154	0.649	0.520	–1.040	104.520	0.957
TIP4P-Ew	3.164	0.681	0.524	–1.048	104.520	0.957

DownLoad: CSV

[1]	Ball P 2017 Proc. Natl. Acad. Sci. U.S.A. 114 13327 Google Scholar
[2]	Ball P 2008 Chem. Rev. 108 74 Google Scholar
[3]	Xie Z, Li Z, Lou G, Liang Q, Chen J X, Kou J L, Wei G N 2021 Commun. Theor. Phys. 73 055602 Google Scholar
[4]	Xie Z, Li Z, Li J Y, Kou J L, Yao J, Fan J T 2021 J. Chem. Phys. 154 024705 Google Scholar
[5]	王强, 曹则贤 2019 物理学报 68 015101 Google Scholar Wang Q, Cao Z X 2019 Acta Phys. Sin. 68 015101 Google Scholar
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[7]	叶树集, 李传召, 张佳慧, 谈军军, 罗毅 2019 物理学报 68 013101 Google Scholar Ye S J, Li C Z, Zhang J H, Tan J J, Luo Y 2019 Acta Phys. Sin. 68 013101 Google Scholar
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[9]	Zhang Q L, Wu Y X, Yang R Y, Zhang J L, Wang R F 2021 Chem. Phys. Lett. 762 138139 Google Scholar
[10]	Zhou G B, Li L, Peng K L, Wang X P, Yang Z 2021 J. Phys. Chem. C 125 7971 Google Scholar
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[12]	Zhou G B, Huang L L 2021 Mol. Simul. 47 925 Google Scholar
[13]	Rahman A, Stillinger F H 1971 J. Chem. Phys. 55 3336 Google Scholar
[14]	Berendsen H J, Postma J P, van Gunsteren W F, Hermans J 1981 Interaction Models for Water in Relation to Protein Hydration//Pullman B 1981 Intermolecular Forces (Dordrecht: Springer) pp331–342
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[20]	Akyildiz I F, Jornet J M, Han C 2014 Phys. Commun. 12 16 Google Scholar
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[37]	Guillot B, Guissani Y 1997 Phys. Rev. Lett. 78 2401 Google Scholar
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[41]	Einstein A 1905 Ann. Phys. 17 549 Google Scholar
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[43]	Guo Y W, Qin J Y, Hu J H, Cao J H, Zhu Z, Wang C L 2020 Nucl. Sci. Tech. 31 1 Google Scholar
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[45]	Zhu Z, Sheng N, Wan R Z, Fang H P 2014 J. Phys. Chem. A 118 8936 Google Scholar
[46]	Heyden M, Sun J, Funkner S, Mathias G, Forbert H, Havenith M, Marx D 2010 Proc. Natl. Acad. Sci. U.S.A. 107 12068 Google Scholar
[47]	Glättli A, Daura X, Van Gunsteren W F 2003 J. Comput. Chem. 24 1087 Google Scholar
[48]	Soper A 2000 Chem. Phys. 258 121 Google Scholar
[49]	Kubo R 1966 Rep. Prog. Phys. 29 255 Google Scholar

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