- 必威体育下载

姓名
邮箱
手机号码
标题
留言内容
验证码

Abstract

Experimental techniques and theoretical calculations have made significant breakthroughs recently in realizing the ultrafast time resolution and the understanding of microscopic details on an atomic scale, which has brought new insights into the ultrafast microscopic dynamics of water system and aqueous system. Here we focus on the dynamic processes of ionization, dissociation, as well as plasmonization of water molecules, water clusters, and liquid water under different intensities of light excitation. The pump-probe technique allows one to extract the information about the orbital-dependent phase shift during photoionization, corresponding to delays on a time scale from tens to hundreds of attoseconds. Delay time in photoionization is found to be proportional to the delocalization of molecular/cluster orbitals. In addition, the information related to the Feshbach resonance is also of interest. By solving the scattering equations, the detailed information about the scattering cross section, the β-parameter, and the involved Rydberg orbitals during valence electron ionization of water is obtained. For liquid water undergoing irradiation by an optical field, the tunneling electrons are unable to move away and recombine with the parent molecule on a time scale of 100 fs if the external field is not strong enough (e.g. ~100 kV/cm). For terahertz fields as high as 250 kV/cm, electrons will move away from the parent molecule after tunnelling and undergo decoherence on a 10-fs time scale. At the beginning of tunneling the electrons will be more delocalized and will collapse to a certain position on a time scale of ~1 ps, and then slowly diffuse or recombine with holes on a longer time scale. For the strong excitation case, hot electrons may also be formed. When a hot electron is located on a particular water molecule, the O—H bond will be broken. When an electron ionizes away, a hole will be created. The hole will be located on a water molecule within 10 fs, and will trigger off subsequent processes such as proton transfer and coherent oscillations. In particular, after the hole is localized and before the proton is transferred, there is a brief appearance of the metastable $ {{{\mathrm{H}}}_{2}{\mathrm{O}}}^{+} $ ion, whose lifetime is experimentally captured and is predicted to be (46±10) fs. The nuclear quantum effect in this process plays a key role. Using the methods such as real time-time dependent density functional theory (rt-TDDFT), it is found that the water undergoes plasmonization under intense laser pulses corresponding to a field strength amplitude larger than 2.4 V/Å. The effective electron temperature in this period reaches over 20000 K. Strongly excited water in this state exhibits the behaviors of a liquid metal, and extremely strong nonthermal effect and nonadiabatic effect. In the process of plasmonization, a large fraction of chemical bonds in water molecules are broken and reorganize themselves, and many chemical species such as hydrogen molecules may appear, which also implies that laser-induced plasmonization can be used to synthesize new substances. Although the previous researches have brought about a very rich understanding, we have also found some details that still need to be explored: i) the influence of nuclear quantum effects has not been taken into account in most of theoretical calculations, which may result in the inadequate description and inaccurate prediction; ii) some of the microscopic details observed in simulations do not yet have a direct counterpart in experimental measurements; iii) the current simulation of water plasmonization is for the local behavior under the spatially uniform external field, while in the real situation there are spatial inhomogeneity and energy flow, which urgently need larger-scale excited state dynamics simulations. With the development of laser technology, the integration of water science and ultrafast technologies will be increasingly strong, so we believe that such a systematic understanding will play a key role in the future. It is expected that new research efforts will continue to contribute to a better understanding and the generation of new technologies in this exciting research field.

Keywords:

Authors and contacts

Corresponding author:Meng Sheng,smeng@iphy.ac.cn

Funds:Project supported by the National Key Research and Development Program of China (Grant Nos. 2021YFA1400201, 2021YFA1400503), the National Natural Science Foundation of China (Grant Nos. 11934003, 12025407, 11974400), and the Chinese Academy of Sciences (Grant Nos. YSBR-047, XDB330301).

FullText HTML: translate this paragraph

References

[1]
[2]
[3]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
[17]
[18]
[19]
[20]
[21]
[22]
[23]
[24]
[25]
[26]
[27]
[28]
[29]
[30]
[31]
[32]
[33]
[34]
[35]
[36]
[37]
[38]
[39]
[40]
[41]
[42]
[43]
[44]
[45]

Cited By

DownLoad: Full-Size Img PowerPoint

Resonance	Energy/eV	Widths/meV	Diercksen/eV	Xview	Yview	Zview
4sa₁ 5sa₁ 6sa₁	12.717 13.543 13.910	11.33 3.83 1.63	12.77 13.67 14.07
3db₂	12.886	2.81	13.13
3da₁	12.941	1.41	13.14
3db₁	13.020	2.60	13.25
4db₁ 5db₁	13.679 13.979	0.90 0.48	13.88 14.18
3da₁	13.030	2.71	13.23
4pb₂	13.208	3.07	13.35
4pb₁ 5pb₁ 6pb₁	13.297 13.796 14.039	3.29 1.36 0.74	13.45 13.97 13.97
4pa₁ 5pa₁ 6pa₁	13.317 13.804 14.044	13.72 6.15 3.24	13.51 13.99 14.30

DownLoad: CSV

Resonance	Energy/eV	Widths/meV	Diercksen/eV	Xview	Yview	Zview
3pb₂	15.888	219.45	15.77
3pb₂	15.888	219.45	15.77
3pa₁	16.212	3.14	15.97
4sa₁	16.885	7.63	16.47
3db₂	17.112	29.38	17.04
3da₂	17.180	2.12	17.03
4da₂ 5da₂	17.854 18.170	0.88 0.46	17.70 18.01

DownLoad: CSV

[1]
[2]
[3]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
[17]
[18]
[19]
[20]
[21]
[22]
[23]
[24]
[25]
[26]
[27]
[28]
[29]
[30]
[31]
[32]
[33]
[34]
[35]
[36]
[37]
[38]
[39]
[40]
[41]
[42]
[43]
[44]
[45]

[1]	Zhu Yu-Hao, Li Rui.Study of electronic structure and optical transition properties of low-lying excited states of AuB molecules based on configuration interaction method. Acta Physica Sinica, 2024, 73(5): 053101.doi:10.7498/aps.73.20231347
[2]	Li Duo-Duo, Zhang Song.Molecular structures in the non-adiabatic relaxaiton processes of excited states of pentafluoropyridine. Acta Physica Sinica, 2024, 73(4): 043101.doi:10.7498/aps.73.20231570
[3]	Xing Feng-Zhu, Cui Jian-Po, Wang Yan-Zhao, Gu Jian-Zhong.Two-proton emission from excited states of proton-rich nuclei. Acta Physica Sinica, 2022, 71(6): 062301.doi:10.7498/aps.71.20211839
[4]	Duan Tong-Chuan, Yan Shao-Jian, Zhao Yan, Sun Ting-Yu, Li Yang-Mei, Zhu Zhi.Relationship between hydrogen bond network dynamics of water and its terahertz spectrum. Acta Physica Sinica, 2021, 70(24): 248702.doi:10.7498/aps.70.20211731
[5]	Li Ya-Sha, Sun Lin-Xiang, Zhou Xiao, Chen Kai, Wang Hui-Yao.Structure and excitation characteristics of C₅F₁₀O under external electric field based on density functional theory. Acta Physica Sinica, 2020, 69(1): 013101.doi:10.7498/aps.69.20191455
[6]	Ye Shu-Ji, Li Chuan-Zhao, Zhang Jia-Hui, Tan Jun-Jun, Luo Yi.Research progress of molecular structure and dynamics of biological water. Acta Physica Sinica, 2019, 68(1): 013101.doi:10.7498/aps.68.20181273
[7]	Zhang Jin-Fang, Ren Ya-Na, Wang Jun-Min, Yang Bao-Dong.Investigation of the two-color polarization spectroscopy between the excited states based on cesium atoms. Acta Physica Sinica, 2019, 68(11): 113201.doi:10.7498/aps.68.20181872
[8]	Luo Jin-Long, Ling Feng-Zi, Li Shuai, Wang Yan-Mei, Zhang Bing.Ultrafast photodissociation dynamics of butanone in 3s Rydberg state. Acta Physica Sinica, 2017, 66(2): 023301.doi:10.7498/aps.66.023301
[9]	Liu Xiao-Jun, Miao Feng-Juan, Li Rui, Zhang Cun-Hua, Li Qi-Nan, Yan Bing.Configuration interaction study on electronic structures and transitional properties of excited states of GeO molecule. Acta Physica Sinica, 2015, 64(12): 123101.doi:10.7498/aps.64.123101
[10]	Zhao Cui-Lan, Wang Li-Li, Zhao Li-Li.Properties of excited state of polaron in quantum disk in finite depth parabolic potential well. Acta Physica Sinica, 2015, 64(18): 186301.doi:10.7498/aps.64.186301
[11]	Qi Xiao-Qiu, Wang Feng, Dai Chang-Jian.Photoexcitation and photoionization of alkali atoms. Acta Physica Sinica, 2015, 64(13): 133201.doi:10.7498/aps.64.133201
[12]	Cao Xin-Wei, Ren Yang, Liu Hui, Li Shu-Li.Molecular structure and excited states for BN under strong electric field. Acta Physica Sinica, 2014, 63(4): 043101.doi:10.7498/aps.63.043101
[13]	Tian Yuan-Ye, Guo Fu-Ming, Zeng Si-Liang, Yang Yu-Jun.Investigation of photoionization of excited atom irradiated by the high-frequency intense laser. Acta Physica Sinica, 2013, 62(11): 113201.doi:10.7498/aps.62.113201
[14]	Zhang Yun-An, Tao Jun-Yong, Chen Xun, Liu Bin.Influence of water on the tensile properties of amorphous silica：a reactive molecular dynamics simulation. Acta Physica Sinica, 2013, 62(24): 246801.doi:10.7498/aps.62.246801
[15]	Gao Shuang-Hong, Ren Zhao-Yu, Guo Ping, Zheng Ji-Ming, Du Gong-He, Wan Li-Juan, Zheng Lin-Lin.Magnetic properties and excited states of thegraphene quantum dots. Acta Physica Sinica, 2011, 60(4): 047105.doi:10.7498/aps.60.047105
[16]	Xu Guo-Liang, Xia Yao-Zheng, Liu Xue-Feng, Zhang Xian-Zhou, Liu Yu-Fang.Effect of external electric field excitation on titanium monoxide. Acta Physica Sinica, 2010, 59(11): 7762-7768.doi:10.7498/aps.59.7762
[17]	Cai Shao-Hong, Zhou Ye-Hong.The excited states structure for chloroethylene under the external electric field. Acta Physica Sinica, 2010, 59(11): 7749-7755.doi:10.7498/aps.59.7749
[18]	Wei Qun, Yang Zi-Yuan, Wang Can-Jun, Xu Qi-Ming.Effects of excited states for d3 ions on spin-Hamiltonian parameters of the ground state 4A2 in axial-symmetrical crystal field. Acta Physica Sinica, 2007, 56(1): 507-511.doi:10.7498/aps.56.507
[19]	Xu Guo-Liang, Zhu Zheng-He, Ma Mei-Zhong, Xie An-Dong.Study on the effect of external electric field excitation on methane. Acta Physica Sinica, 2005, 54(7): 3087-3093.doi:10.7498/aps.54.3087
[20]	Tang Nai-Yun, Chen Xiao-Shuang, Lu Wei.The effect of size distribution on photoluminescence of excited states from InAs/GaAs quantum dots. Acta Physica Sinica, 2005, 54(12): 5855-5860.doi:10.7498/aps.54.5855

Catalog

Vol. 73, Issue 8 - 2024-04-20

Metrics

Abstract views:1927
PDF Downloads:130
Cited By:0

Search

Article