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反应动力学理论与计算研究组(1113组)
组群介绍
基元反应动力学研究组
团簇光谱与动力学研究组
反应动力学理论与计算研究组
表面反应动力学研究组
自由电子激光技术研究组
超快激光技术与动力学研究组
大连光源
反应动力学理论与计算研究组(1113组)

小组简介

       1113组组长是孙志刚研究员,组内共拥有2名研究员,3名副研究员,1名助理研究员,博士后4人,学生12人。研究内容主要是基于量子力学原理,研究气象分子反应和非弹性动力学以及激光场下气象分子动力学过程,和有关于量子反应动力学理论和数值计算方法的发展。


研究方向

1、分子反应动力学前沿动力学问题的研究 (负责人:孙志刚)

       化学反应是化学键形成和断裂的过程。在这一过程中,会伴随很多有趣的现象,特别是有关量子效应的现象,比如说,化学反应共振,几何相位效应以及分子反应散射过程中和众多光学现象类似的效应。研究这些问题,对于我们深入理解量子力学原理,理解微观层次上的化学反应过程,有重要的意义。


代表性文章:

(1) Daofu Yuan, Shengrui Yu, Wentao Chen, Jiwei Sang, Chang Luo, Tao Wang, Xin Xu, Piergiorgio Casavecchia, Xingan Wang,  Donghui Zhang, Zhigang Sun, Xueming Yang, Direct observation of forward-scattering oscillations in the H+HD→H2+D reaction, Nat. Chemistry (2018)
(2) Extremely short-lived reaction resonances in Cl + HD (v = 1)→ DCl + H due to chemical bond softening, Tiangang Yang, Jun Chen, Long Huang, Tao Wang, Chunlei Xiao, Zhigang Sun, Dongxu Dai, Xueming Yang, Donghui Zhang, Science, 347, 60 (2015)
(3) Bin Zhao, Zhigang Sun, Hua Guo, State-to-State Mode Specificity: Energy Sequestration and Flow Gated by Transition State, J. Am. Chem. Soc., 137, 15964 (2015)
(4) Dynamical Resonances Accessible Only by Reagent Vibrational Excitation in the F + HD→HF + D Reaction, Tao Wang, Jun Chen, Tiangang Yang, Chunlei Xiao, Zhigang Sun, Long Huang, Dongxu Dai, Xueming Yang, Donghui Zhang, Science, 342, 1499 (2013)
(5) State-to-state quantum dynamics of O + O2 isotope exchange reactions reveals nonstatistical behavior at atmospheric conditions, Zhigang Sun, Lan Liu, Shiying Lin, Reihhard Schinke, Hua Guo, Donghui Zhang, Proc. Natl. Acad. Sci. USA, 107, 555 (2010)
(6) The Extent of Non-Born-Oppenheimer Coupling in the Reaction of Cl(2P) with para-H2, Xignan Wang, Wenrui Dong, Chunlei Xiao, Li Che, Zefeng Ren, Dongxu Dai, Xiuyan Wang, Piergiorgio Casavecchia, Bin Jiang, Daiqian Xie, Zhigang Sun, Soo-Ying Lee, Donghui Zhang, Hans-Joachim Werner, Millard H. Alexande, Science, 322, 573 (2008)
(7) Probing the resonance potential in the F atom reaction with hydrogen deuteride with spectroscopic accuracy, Zefeng Ren, Li Che, Minghui Qiu, Xingan Wang, Wenrui Dong, Dongxu Dai, Xiuyan Wang, Xueming Yang, Zhigang Sun, Bina Fu, Soo-Ying Lee, Donghui Zhang, Proc. Natl. Acad. Sci. USA, 105, 12662 (2008)
(8) HF(v’= 3) forward scattering in the F+ H2 reaction: Shape resonance and slow-down mechanism, Xingan Wang, Wenrui Dong, Minghui Qiu, Zefeng Ren, Li Che, Dongxu Dai, Xiuyan Wang, Xueming Yang, Zhigang Sun, Bina Fu, Soo-Ying Lee, Xin Xu, Donghui Zhang, Proc. Natl. Acad. Sci. USA, 105, 6227 (2008)
(9) State-to-State Dynamics of H + O2 Reaction, Evidence for Nonstatistical Behavior, Zhigang Sun, Donghui Zhang, Chuanxiu Xu, Shulan Zhou, Daiqian Xie,  GyÖrgy Lendvay, Soo-Ying Lee, Shiying Lin, Hua Guo, J. Am. Chem. Soc., 130, 14962 (2008)
(10) Observation of Feshbach Resonances in the F+ H2 → HF +H Reaction, Minghui Qiu, Zefeng Ren, Li Che, Dongxu Dai, Steve A. Harich, Xiuyan Wang, Xueming Yang, Chuanxiu Xu, Daiqian Xie, Magnus Gustafsson, Rex T. Skodje, Zhigang Sun, Donghui Zhang, Science, 311, 1440 (2006)


2、精确势能面的构建 (负责人:傅碧娜,徐昕)

       拟合势能面是分子动力学,特别是量子分子动力学研究的基础。发展高效、普适的多项式函数拟合方法,比如说交换不变多项式神经网络方法等,采用尽可能少的从头算能量点,针对特定分子反应过程或光解动力学过程,特别是有非绝热效应和几何相位效应等的分子体系,构建多维高精度的分子全域势能面。期望能够提供足够精确的势能面,从而能够在在光谱精度上来研究分子动力学过程。


代表性文章:
(1) A neural network potential energy surface for F + CH4 reaction including multiple channels based on coupled cluster theory, Jun Chen, Xin Xu, Shu Liu, Dong H. Zhang, Phys. Chem. Chem. Phys., 20, 9090  (2018)
(2) Application of Clustering Algorithms to Partitioning Configuration Space in Fitting Reactive Potential Energy Surfaces, Yafu Guan, Shuo Yang, Dong H. Zhang, J. Phys. Chem. A, 122, 3140 (2018)
(3) Construction of reactive potential energy surfaces with Gaussian process regression: active data selection, Yafu Guan, Shuo Yang, Dong H. Zhang, Mol. Phys., 116, 823 (2018)
(4) Construction of diabatic energy surfaces for LiFH with artificial neural networks, Yafu Guan, Bina Fu, Dong H. Zhang, J. Chem. Phys., 147, 224307 (2017)
(5) Fitting potential energy surfaces with fundamental invariant neural network (Communication), Kejie Shao, Jun Chen, Zhiqiang Zhao and Dong H. Zhang, J. Chem. Phys., 145, 071101 (2016)
(6) A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(1D) + CH4 multichannel reaction, Kejie Shao, Bina Fu and Dong H. Zhang, Phys. Chem. Chem. Phys., 17, 24098 (2015)
(7) An accurate potential energy surface for the F + H2 → HF + H reaction by the coupled-cluster method, Jun Chen, Zhigang Sun, Dong H. Zhang, J. Chem. Phys., 142, 024303 (2015)
(8) A permutationally invariant full-dimensional ab initio potential energy surface for the abstraction and exchange channels of the H + CH4 system, Jun Li, Jun Chen, Zhiqiang Zhao, Daiqian Xie, Dong H. Zhang, Hua Guo, J. Chem. Phys., 142, 204302 (2015)
(9) 基于神经网络的分子体系势能面构造, 陈俊, 张东辉, 中国科学:化学, 45, 1241 (2015)
(10) Global Potential Energy Surface for the H+CH4 → H2+CH3 Reaction using Neural Networks, Xin Xu, Jun Chen, Dong H. Zhang, Chin. J. Chem. Phys., 27, 373 (2014)
(11) A global potential energy surface for the H2 + OH ↔ H2O + H reaction using neural networks, Jun Chen, Xin Xu, Xin Xu, Dong H. Zhang, J. Chem. Phys., 138, 154301 (2013)
(12) An accurate global potential energy surface for the OH + CO → H + CO2 reaction using neural networks (Communication), Jun Chen, Xin Xu, Xin Xu, Dong H. Zhang, J. Chem. Phys., 138, 221104 (2013)


3、分子与表面作用的动力学研究(负责人:傅碧娜,张兆军)

       分子在金属表面解离吸附的动力学研究在多相催化等工业过程中占有重要的地位。由于表面的参与,分子在表面的解离吸附问题无论在电子结构计算还是在动力学研究方面都比孤立分子体系研究复杂和困难。我们通过构建目前最为精确的分子解离吸附势能面和发展高维量子动力学方法,对从简单双原子分子到多原子反应在表面的解离体系开展目前最为精确的理论研究,在气象分子与表面散射动力学研究领域取得突破。


代表性文章:
(1) Z. Zhang, T. Liu, B. Fu*, X. Yang, D. H. Zhang*, First-principles quantum dynamical theory for the dissociative chemisorption of H2O on rigid Cu(111), Nature Communications, 7, 11953 (2016).
(2) T. Liu, Z. Zhang, B. Fu*, X. Yang, D. H. Zhang*, A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle averaging, Chemical Science, 7, 1840 (2016).
(3) T. Liu, J. Chen, Z. Zhang, X. Shen, B. Fu*, D. H. Zhang*, Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface, J. Chem. Phys., 148, 144705 (2018).
(4) T. Liu, Z. Zhang, J. Chen, B. Fu*, D. H. Zhang*, An approximate full-dimensional quantum dynamics study of the mode specificity in the dissociative chemisorption of D2O on rigid Cu(111), Phys. Chem. Chem. Phys., 19, 11960 (2017).
(5) T. Liu, B. Fu*, D. H. Zhang*, HCl dissociating on a rigid Au(111) surface: A six-dimensional quantum mechanical study on a new potential energy surface based on the RPBE functional, J. Chem. Phys., 146, 164706 (2017).
(6) T. Liu, Z. Zhang, J. Chen, B. Fu*, D. H. Zhang*, Mode specificity of the dissociative chemisorption of HOD on rigid Cu(111): an approximate full-dimensional quantum dynamics study, Phys. Chem. Chem. Phys., 18, 26358 (2016). (Front cover paper)
(7) T. Liu, Z. Zhang, B. Fu*, X. Yang, D. H. Zhang*, Mode specificity for the dissociative chemisorption of H2O on Cu(111): a quantum dynamics study on an accurately fitted potential energy surface, Phys. Chem. Chem. Phys., 18, 8537 (2016) .
(8) T. Liu, B. Fu*, D. H. Zhang*, Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface, J. Chem. Phys., 141, 194302 (2014).
(9) T. Liu, B. Fu*, D. H. Zhang*, Six-dimensional quantum dynamics study for the dissociative adsorption of DCl on Au(111) surface, J. Chem. Phys., 140, 144701 (2014).


4、量子反应散射理论和计算方法的发展及其典型体系的动力学研究:(负责人:孙志刚、刘舒、张兆军)

       高精度、高效率的量子动力学计算方法,是采用有限的计算资源,开展更广泛分子动力学研究的基础。采用(伪)谱方法、谱有限差分方法以及谱有限元方法,选择/设计合适的分子坐标体系,发展普适、高效的态-态分辨的反应散射量子反应动力学方法,是推动量子分子反应散射理论领域的发展的源动力。


代表性文章:
(1) Quantum real wave packet method by using spectral difference for a triatomic reactive scattering, Xueming Li, Zhigang Sun, Chem. Phys., (2018)
(2) Time-Dependent Wave Packet Dynamics Calculations of Cross Sections for Ultracold Scattering of Molecules, Jiayi Hou, Shu Liu, Donghui Zhang, Krems, Roman V., Phys. Rev. Lett. 120, 143401 (2018)
(3) Dynamical barrier and isotope effects in the simplest substitution reaction via Walden inversion mechanism, Zhiqiang Zhao, Zhaojun Zhang, Shu Liu, Donghui Zhang, Nat. Comm., 8, 14506 (2017)
(4) A local mode picture for H atom reaction with vibrationally excited H2O: a full dimensional state-to-state quantum dynamics investigation, Shu Liu, Donghui Zhang, Chem. Sci. 7, 261 (2016)
(5) A reactant-coordinate-based wave packet method for full-dimensional state-to-state quantum dynamics of tetra-atomic reactions: Application to both the abstraction and exchange channels in the H+ H2O reaction, Bin Zhao, Hua Guo, Zhigang Sun, J. Chem. Phys., 144, 064104 (2016) 
(6) A reactant-coordinate-based approach to state-to-state differential cross sections for tetratomic reactions, Bin Zhao, Hua Guo, Zhigang Sun,  J. Chem. Phys., 145, 184106 (2016)
(7) Calculation of state-to-state differential and integral cross sections for atom-diatom reactions with transition-state wave packets, Bin Zhao, Hua Guo, Zhigang Sun, J. Chem. Phys.,  140, 234110 (2014) 
(8) Calculation of state-to-state cross sections for triatomic reaction by the multi-configuration time-dependent Hartree method, Bin Zhao, Dong H. Zhang, Soo-Y Lee, Zhigang Sun, J. Chem. Phys., 140, 164108 (2014)
(9) An exact short-time solver for the time-dependent Schrodinger equation (Communication), Zhigang Sun, Weitao Yang,  J. Chem. Phys., 134, 041101(2011)
(10)  Experimental and Theoretical Differential Cross Sections for a Four-Atom Reaction: HD+OH→H2O+D, Chunlei Xiao, Xin Xu, Shu Liu, Tao Wang, Wenrui Dong, Tiangang Yang, Zhigang Sun, Dongxu Dai, Xin Xu, Donghui Zhang, Xueming Yang,Science, 333, 440 (2011)


5、复杂多原子体系的准经典动力学和RPMD计算:(负责人:傅碧娜)

       基于目前的计算机水平,精确的量子动力学对于研究复杂的多原子分子反应体系是非常困难的,但是燃烧过程中重要的反应往往是复杂的多原子分子体系。基于基本不变量-神经网络(FI-NN)和置换不变多项式(PIP)拟合方法,构建这些体系的高精度势能面,并且采用QCT和发展RPMD方法研究反应的微观动力学机理以及反应的速率常数,是目前理解这些燃烧反应机理的一个有效途径。


代表性文章:
(1) Trapped abstraction in the O(1D)+CHD3→OH+CD3 reaction reaction, Jiayue Yang, Kejie Shao, Dong Zhang, Quan Shuai, Bina Fu*, Dong H. Zhang*, Xueming Yang*, J. Phys. Chem. Lett. 5, 3106, (2014).
(2) Intersystem crossing and dynamics in O(3P)+C2H4 multichannel reaction: Experiment validates theory, Bina Fu, Yong-chang Han, Joel M. Bowman, Luca Angelucci, Nadia Balucani, Francesca Leonori, Piergiorgio Casavecchia, PNAS, 109, 9733, (2012).
(3) Three-state trajectory surface hopping studies of the photodissociation dynamics of formaldehyde on ab initio potential energy surfaces, Bina Fu, Benjamin C. Shepler, Joel M. Bowman, J. Am. Chem. Soc., 133, 7957, (2011).
(4) A global full-dimensional potential energy surface and quasiclassical trajectory study of the O(1D) + CH4 multichannel reaction, K. Shao, Bina Fu*, D. H. Zhang*, Phys. Chem. Chem. Phys., 17, 24098 (2015).
(5) Crossed Molecular Beams and Quasiclassical Trajectory Surface Hopping Studies of the Multichannel Nonadiabatic O(3P) + Ethylene Reaction at High Collision Energy, N. Balucani, F. Leonori, P. Casavecchia*, Bina Fu*, J. M. Bowman, J. Phys. Chem. A, 119, 12498 (2015).
(6) Quasiclassical Trajectory Study of the Reaction of CD4 with O(1D), K. Shao, Bina. Fu*, D. H. Zhang*,  Chin. J. Chem. Phys., 28, 403 (2015).
(7) Quasiclassical trajectory studies of 18O(3P)+NO2 isotope exchange and reaction to O2 +NO on D0 and D1 potentials, Bina Fu*, D. H. Zhang, J. M. Bowman, J. Chem. Phys., 139, 024303 (2013).


6、表面反应微观动力学模拟:(负责人:苏海燕)

       催化反应主要是吸附质在催化剂表面的成、断键过程,从原子尺度识别控制吸附质-表面化学键及催化活性的关键因素,进而指导材料合成与优化设计,是理论研究面临的巨大挑战。基于第一性原理计算和微观反应动力学的多相催化理论研究,侧重于吸附质-表面成键新理论的发展以及能源和环境催化相关过程,如 CO/CO2加氢、电催化氧还原/析氧的机理研究具有重要的意义。


代表性文章:
1. Establishing and Understanding Adsorption−Energy Scaling Relations with Negative Slopes, H. Y. Su+, K. J. Sun+, W. Q. Wang, Z. H. Zeng, F. Calle-Vallejo*, W. X. Li*, J. Phys. Chem. Lett.  7, 5302 (2016)
2. Crystallographic Dependence of CO Activation on Cobalt Catalysts: HCP versus FCC, J. X. Liu+, H. Y. Su+, D. P. Sun, W. X. Li, J. Am. Chem. Soc. 135 ,16284 (2013)  (引用92次)
3. Theoretical insights and the corresponding construction of supported metal catalysts for highly selective CO2-to-CO conversion, X. D. Chen, X. Su, H. Y. Su*, X. Y. Liu, S. Miao, Y. H. Zhao, K. J. Sun, Y. Q. Huang*, T. Zhang, ACS Catal., 7, 4613 (2017)
4. First-Principles Study of Structure Sensitivity of Chain Growth and Selectivity in Fischer-Tropsch Synthesis on HCP Cobalt Catalysts, H. Y. Su, Y. H. Zhao, J. X. Liu, K. J. Sun*, W. X. Li*, Catal. Sci. Technol.  7, 2967 (2017) (期刊热点论文)
5. Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces, I. C. Man, H. Y. Su, F. Calle-Vallejo, J. I. Martinez, N. G. Inoglu, J. Kitchin, T. F. Jaramillo, J. Norskov, J. Rossmeisl*, ChemCatChem, 3, 1159 (2011) (ESI高被引论文/封面,引用718次)
6. Interface-Confined Ferrous Centers for Catalytic Oxidation, Q. Fu+, W. X. Li+, Y. X. Yao, H. Y. Liu, H. Y. Su, D. Ma, X. K. Gu, L. M. Chen, Z. Wang, H. Zhang, B. Wang, X. H. Bao*, Science 328, 1141 (2010) (ESI高被引论文,引用441次)

合作伙伴
(1) Prof. Hua Guo (New Mexico University)
(2) Prof. Millard Alexander (University of Maryland)
(3) Prof. Francois Lique (Université du Havre)
(4) Prof. Daiqian Xie (Najing University) 
(4) Prof. Xu Xin (Fudan University) 
(4) Prof. Fabien Gatti (Université Paris-Saclay) 
(5) Prof. Shanxi Tian (University of Science and Technology of China) 
(6) Prof. Daniel M. Neumark (University of California, Berkeley, USA)


研究人员

     
孙志刚 研究员 傅碧娜 研究员      


 
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