-
The C(3P) + H2 → CH+H reaction in a collision energy range of 1.0–2.0 eV with the initial state
$\nu = 0{\rm{ }},j = 0$ is investigated based on the new potential energy surface (PES) by using the Chebyshev wave packet method. All partial wave contributions up to J = 60 are calculated explicitly by the coupled state (CS) approximation method and the Coriolis coupling (CC) effect. Dynamic properties such as reaction probabilities, integral cross sections, and state specific rate constants are calculated. The calculated probabilities and integral reaction cross sections display an increasing trend with the increase of the collision energy and an oscillatory structure due to the CH2 well on the reaction path. The thermal rate constants of the endoergic reaction with a temperature ranging from 1000 K to 2000 K are obtained also. The calculated rate constants increase in the entire temperature range, showing a sharp T dependence in a range of 1400–2000 K. The rate constants are sensitive to the temperature due to the high threshold of the title reaction. In addition, the results of the exact calculations including CC effect are compared with those from the CS approximation. For smaller J, the CS probabilities are larger than the CC results, while for larger J, they are smaller than the CC ones. For reaction cross sections and rate constants, the CS results and the CC ones are in good agreement with each other at lower energy. However, they turn different at higher energy. The comparison between the CC and CS results indicates that neglecting the Coriolis coupling leads the cross sections and the rate constants to be underestimated due to the formation of a CH2 complex supported by stationary point of CH2(${\tilde{\rm X}}{}^3 \rm A''$ ) PES. It is suggested that the CH2 complex plays an important role in the process of the title reaction. However, it seems to overestimate the CS and CC rate constants because the barrier recrossing is neglected. Unfortunately, the results obtained in the present work have no corresponding theoretical or experimental data to be compared with, therefore these results provide simply a certain reference significance to the follow-up study of the title reaction.-
Keywords:
- CH2 system /
- potential energy surface /
- reaction probability /
- integral cross section
[1] Bockhorn H, Galdo N, Herbertz H A, Fetting F 1971 Combust. Sci. Technol. 2 329
Google Scholar
[2] Flower D R, Pineau des Foreêts G 1998 Mon. Not. R. Astron. Soc. 297 1182
Google Scholar
[3] Bucher M E, Glinski R J 1999 Mon. Not. R. Astron. Soc. 308 29
Google Scholar
[4] Bearda R A, vanHemert M C, vanDishoeck E F 1992 J. Chem. Phys. 97 8240
Google Scholar
[5] Scott D C, De Juan, J, Robie D C, Schwartz-Lavi D, Reisler H 1992 J. Phys. Chem. 96 2509
Google Scholar
[6] Jursich G M, Wiesenfeld J R 1985 J. Chem. Phys. 83 910
Google Scholar
[7] Mikulecky K, Gericke K H 1993 J. Chem. Phys. 98 1244
Google Scholar
[8] Bussery-Honvault B, Honvault P, Launay J M 2001 J. Chem. Phys. 115 10701
Google Scholar
[9] Bussery-Honvault B, Julien J, Honvault P, Launay J M 2005 Phys. Chem. Chem. Phys. 7 1476
Google Scholar
[10] Joseph S, Varandas A J C 2009 J. Phys. Chem. A 113 4175
Google Scholar
[11] Zhang C F, Fu M K, Shen Z T, Ma H T, Bian W S 2014 J. Chem. Phys. 140 234301
Google Scholar
[12] Lin S Y, Guo H 2004 J. Phys. Chem. A 108 2141
Google Scholar
[13] Sun Z P, Zhang C F, Lin S Y, Zheng Y J, Meng Q T, Bian W S 2013 J. Chem. Phys. 139 014306
Google Scholar
[14] Lu R F, Wang Y H, Deng K M 2013 J. Comput. Chem. 34 1735
Google Scholar
[15] Joseph S, Caridade P J S B, Varandas A J C 2011 J. Phys. Chem. A 115 7882
Google Scholar
[16] Wu Y, Zhang C F, Cao J W, Bian W S 2014 J. Phys. Chem. A 118 4235
Google Scholar
[17] Shen Z T, Cao J W, Bian W S 2015 J. Chem. Phys. 142 164309
Google Scholar
[18] Hickson K M, Suleimanov Y V 2017 Phys. Chem. Chem. Phys. 19 480
Google Scholar
[19] González-Lezana T, Larrégaray P, Bonnet L, Wu Y N, Bian W S 2018 J. Chem. Phys. 148 234305
Google Scholar
[20] Knowles P, Handy N C, Carter S 1983 Mol. Phys. 49 681
Google Scholar
[21] Murrell J, Dunne L 1983 Chem. Phys. Lett. 102 155
Google Scholar
[22] Harding L B, Guadagnini R, Schatz G C 1993 J. Phys. Chem. 97 5472
Google Scholar
[23] Werner H J, Knowles P J 1988 J. Chem. Phys. 89 5803
Google Scholar
[24] Knowles P J, Werner H J 1988 Chem. Phys. Lett. 145 514
Google Scholar
[25] van Harrevelt R, Van Hemert M C, Schatz G C 2002 J. Chem. Phys. 116 6002
Google Scholar
[26] Gamallo P, Defazio P, Akpinar S, Petrongolo C 2012 J. Phys. Chem. A 116 8291
Google Scholar
[27] Guadagnini R, Schatz G C 1996 J. Phys. Chem. 100 18944
Google Scholar
[28] Scholefield M R, Choi J H, Goyal S, Reisler H 1998 Chem. Phys. Lett. 288 487
Google Scholar
[29] Ehbrecht A, Kowalski A, Ottinger Ch 1998 Chem. Phys. Lett. 284 205
Google Scholar
[30] Zhang L L, Liu D, Yue D G, Song Y Z, Meng Q T 2020 J. Phys. B: At. Mol. Opt. Phys. 53 095202
Google Scholar
[31] Zhang J Z H 1999 Theory and Application of Quantum Molecular Dynamics (Singapore: World Scientific) pp201–218
[32] Gao F, Wang X L, Zhao W L, Song Y Z, Meng Q T 2018 Eur. Phys. J. D 72 224
Google Scholar
[33] Gao F, Zhang L L, Zhao W L, Meng Q T, Song Y Z 2019 J. Chem. Phys. 150 224304
Google Scholar
[34] Mandelshtam V A, Taylor H S 1995 J. Chem. Phys. 102 7390
Google Scholar
[35] Mandelshtam V A, Taylor H S 1995 J. Chem. Phys. 103 2903
Google Scholar
[36] Tal-Ezer H, Kosloff R 1984 J. Chem. Phys. 81 3967
Google Scholar
[37] Zhang D H, Zhang J Z H 1994 J. Chem. Phys. 101 1146
Google Scholar
[38] Meijer A J H M, Goldfield E M, Gray S K, Balint-Kurti G G 1998 Chem. Phys. Lett. 293 270
Google Scholar
[39] Althorpe S C 2001 J. Chem. Phys. 114 1601
Google Scholar
[40] Lin S Y, Guo H 2006 J. Chem. Phys. 124 031101
Google Scholar
[41] Blint R, Newton M 1975 Chem. Phys. Lett. 32 178
Google Scholar
[42] Zhai H C, Lin S Y 2015 Chem. Phys. 455 57
Google Scholar
[43] Carroll T E, Goldfield E M 2001 J. Phys. Chem. A 105 2251
Google Scholar
[44] Meijer A J H M, Goldeld E M 1999 J. Chem. Phys. 110 870
Google Scholar
[45] Chu T S, Han K L 2008 Phys. Chem. Chem. Phys. 10 2431
Google Scholar
[46] Peng Y, Jiang Z A, Chen J S 2017 J. Phys. Chem. A 121 2209
Google Scholar
-
图 1 CH2等势线, 图中等势线间隔为0.1 eV (a) C沿着共线构型靠近H2分子; (b) C 沿着T构型插入H2
Figure 1. Equipotential contour plot for CH2, the contour increments are 0.1 eV: (a) For bond stretching in C-H-H linear geometry; (b) for T-shaped insertion of C into H2 diatoms.
图 2 90°和180°的最小能量路径
Figure 2. The minimum energy paths as a function of RCH-RHH at 90° and 180°.
图 3 不同分波的反应几率随着碰撞能量的变化
Figure 3. The reaction probabilities vs. collision energy at different J.
图 4 CC与CS反应几率比较
Figure 4. Comparisons between the CC and CS probability.
图 5 C+H2反应的积分散射截面
Figure 5. The integral cross section of the C+H2 reaction.
图 6 C+H2反应的速率常数
Figure 6. The rate constant of the C+H2 reaction.
表 1 波包计算中的数值参量(除特殊说明, 均采用原子单位a.u.)
Table 1. Parameters used in wave packet calculation (The atomic unit is used in the calculation unless otherwise stated).
坐标取值范围
和基组数$R \in ({10^{{\rm{ - }}16}}, \, 16)$, $({N_R} = 203)$ $r \in (0.5, \, 12)$, $({N_r} = 99)$ $\gamma \in ({90^ \circ }, \, {180^ \circ })$, $({N_\gamma } = 50)$ 吸收势 ${R_{\rm{d}}} = 11.0$, ${d_R} = 0.0006$ ${r_{\rm{d}}} = 7.5$, ${d_r} = 0.001$ 初始波包 ${R_0} = 8.0$, ${E_0} = 1.55\;{\rm{ eV}}$, $\delta = 0.3$ 光谱控制 0.5 流计算的位置 ${r_{\rm{f}}} = 7.4$ 传播步数 100000 
DownLoad: CSV
-
[1] Bockhorn H, Galdo N, Herbertz H A, Fetting F 1971 Combust. Sci. Technol. 2 329
Google Scholar
[2] Flower D R, Pineau des Foreêts G 1998 Mon. Not. R. Astron. Soc. 297 1182
Google Scholar
[3] Bucher M E, Glinski R J 1999 Mon. Not. R. Astron. Soc. 308 29
Google Scholar
[4] Bearda R A, vanHemert M C, vanDishoeck E F 1992 J. Chem. Phys. 97 8240
Google Scholar
[5] Scott D C, De Juan, J, Robie D C, Schwartz-Lavi D, Reisler H 1992 J. Phys. Chem. 96 2509
Google Scholar
[6] Jursich G M, Wiesenfeld J R 1985 J. Chem. Phys. 83 910
Google Scholar
[7] Mikulecky K, Gericke K H 1993 J. Chem. Phys. 98 1244
Google Scholar
[8] Bussery-Honvault B, Honvault P, Launay J M 2001 J. Chem. Phys. 115 10701
Google Scholar
[9] Bussery-Honvault B, Julien J, Honvault P, Launay J M 2005 Phys. Chem. Chem. Phys. 7 1476
Google Scholar
[10] Joseph S, Varandas A J C 2009 J. Phys. Chem. A 113 4175
Google Scholar
[11] Zhang C F, Fu M K, Shen Z T, Ma H T, Bian W S 2014 J. Chem. Phys. 140 234301
Google Scholar
[12] Lin S Y, Guo H 2004 J. Phys. Chem. A 108 2141
Google Scholar
[13] Sun Z P, Zhang C F, Lin S Y, Zheng Y J, Meng Q T, Bian W S 2013 J. Chem. Phys. 139 014306
Google Scholar
[14] Lu R F, Wang Y H, Deng K M 2013 J. Comput. Chem. 34 1735
Google Scholar
[15] Joseph S, Caridade P J S B, Varandas A J C 2011 J. Phys. Chem. A 115 7882
Google Scholar
[16] Wu Y, Zhang C F, Cao J W, Bian W S 2014 J. Phys. Chem. A 118 4235
Google Scholar
[17] Shen Z T, Cao J W, Bian W S 2015 J. Chem. Phys. 142 164309
Google Scholar
[18] Hickson K M, Suleimanov Y V 2017 Phys. Chem. Chem. Phys. 19 480
Google Scholar
[19] González-Lezana T, Larrégaray P, Bonnet L, Wu Y N, Bian W S 2018 J. Chem. Phys. 148 234305
Google Scholar
[20] Knowles P, Handy N C, Carter S 1983 Mol. Phys. 49 681
Google Scholar
[21] Murrell J, Dunne L 1983 Chem. Phys. Lett. 102 155
Google Scholar
[22] Harding L B, Guadagnini R, Schatz G C 1993 J. Phys. Chem. 97 5472
Google Scholar
[23] Werner H J, Knowles P J 1988 J. Chem. Phys. 89 5803
Google Scholar
[24] Knowles P J, Werner H J 1988 Chem. Phys. Lett. 145 514
Google Scholar
[25] van Harrevelt R, Van Hemert M C, Schatz G C 2002 J. Chem. Phys. 116 6002
Google Scholar
[26] Gamallo P, Defazio P, Akpinar S, Petrongolo C 2012 J. Phys. Chem. A 116 8291
Google Scholar
[27] Guadagnini R, Schatz G C 1996 J. Phys. Chem. 100 18944
Google Scholar
[28] Scholefield M R, Choi J H, Goyal S, Reisler H 1998 Chem. Phys. Lett. 288 487
Google Scholar
[29] Ehbrecht A, Kowalski A, Ottinger Ch 1998 Chem. Phys. Lett. 284 205
Google Scholar
[30] Zhang L L, Liu D, Yue D G, Song Y Z, Meng Q T 2020 J. Phys. B: At. Mol. Opt. Phys. 53 095202
Google Scholar
[31] Zhang J Z H 1999 Theory and Application of Quantum Molecular Dynamics (Singapore: World Scientific) pp201–218
[32] Gao F, Wang X L, Zhao W L, Song Y Z, Meng Q T 2018 Eur. Phys. J. D 72 224
Google Scholar
[33] Gao F, Zhang L L, Zhao W L, Meng Q T, Song Y Z 2019 J. Chem. Phys. 150 224304
Google Scholar
[34] Mandelshtam V A, Taylor H S 1995 J. Chem. Phys. 102 7390
Google Scholar
[35] Mandelshtam V A, Taylor H S 1995 J. Chem. Phys. 103 2903
Google Scholar
[36] Tal-Ezer H, Kosloff R 1984 J. Chem. Phys. 81 3967
Google Scholar
[37] Zhang D H, Zhang J Z H 1994 J. Chem. Phys. 101 1146
Google Scholar
[38] Meijer A J H M, Goldfield E M, Gray S K, Balint-Kurti G G 1998 Chem. Phys. Lett. 293 270
Google Scholar
[39] Althorpe S C 2001 J. Chem. Phys. 114 1601
Google Scholar
[40] Lin S Y, Guo H 2006 J. Chem. Phys. 124 031101
Google Scholar
[41] Blint R, Newton M 1975 Chem. Phys. Lett. 32 178
Google Scholar
[42] Zhai H C, Lin S Y 2015 Chem. Phys. 455 57
Google Scholar
[43] Carroll T E, Goldfield E M 2001 J. Phys. Chem. A 105 2251
Google Scholar
[44] Meijer A J H M, Goldeld E M 1999 J. Chem. Phys. 110 870
Google Scholar
[45] Chu T S, Han K L 2008 Phys. Chem. Chem. Phys. 10 2431
Google Scholar
[46] Peng Y, Jiang Z A, Chen J S 2017 J. Phys. Chem. A 121 2209
Google Scholar
-
[1] Zhao Wen-Li, Song Yu-Zhi, Ma Chao, Gao Feng, Meng Qing-Tian. Quantum dynamics study of reaction H+SiH using a new potential energy surface of SiH2(11A′). Acta Physica Sinica, 2024, 73(20): 203401. doi: 10.7498/aps.73.20240859 [2] Cui Zi-Chun, Yang Mo-Han, Ruan Xiao-Peng, Fan Xiao-Li, Zhou Feng, Liu Wei-Min. High-throughput calculation of interfacial friction of two-dimensional material. Acta Physica Sinica, 2023, 72(2): 026801. doi: 10.7498/aps.72.20221676 [3] Qiu Zi-Heng, Ahmed Yousif Ghazal, Long Jin-You, Zhang Song. Theoretical studies on molecular conformers and infrared spectra of triethylamine. Acta Physica Sinica, 2022, 71(10): 103601. doi: 10.7498/aps.71.20220123 [4] Zhao Wen-Li, Sun Feng-Wei, Zhang Hong, Wang Yong-Gang, Gao Feng, Meng Qing-Tian. Quantum dynamics studies of the $\rm D+SiD^+ \to D_2+Si^ +$ reaction. Acta Physica Sinica, 2022, 71(22): 228201. doi: 10.7498/aps.71.20221155[5] Li Wen-Tao, Yuan Mei-Ling, Wang Jie-Min. Dynamics of C+ + H2 reaction based on a new potential energy surface. Acta Physica Sinica, 2022, 71(9): 093402. doi: 10.7498/aps.71.20212241 [6] Qiao Zheng1\2, Wang Ya-Li, Wu Ming-Wei, Feng Er-Yin, Huang Wu-Ying. Potential energy surface and cold collision dynamics of Xe-NH(X3∑-) system. Acta Physica Sinica, 2018, 67(21): 213401. doi: 10.7498/aps.67.20181321 [7] Wei Qiang. Exploring the stereodynamics of C(3P)+NO(X2)CO(X1+)+N(4S) reaction on 4A potential energy surface. Acta Physica Sinica, 2015, 64(17): 173401. doi: 10.7498/aps.64.173401 [8] Yang Xue, Yan Bing, Lian Ke-Yan, Ding Da-Jun. Theoretical study on the photodissociation reaction of α-cyclohexanedione in ground state. Acta Physica Sinica, 2015, 64(21): 213101. doi: 10.7498/aps.64.213101 [9] Han Yu-Long, Li Zhen, Wang Jiang-Hong, Feng Er-Yin, Huang Wu-Ying. Potential energy surface and spectra prediction for the Mg-CO complex. Acta Physica Sinica, 2013, 62(9): 093101. doi: 10.7498/aps.62.093101 [10] Shen Guang-Xian, Wang Rong-Kai, Linghu Rong-Feng, Zhou Xun, Yang Xiang-Dong. Theoretical calculation of the vib-rotational interaction potential and the differential coefficient cross sections for He-HD (HT, DT) system. Acta Physica Sinica, 2012, 61(21): 213101. doi: 10.7498/aps.61.213101 [11] . Influence of isotope substitution of sodium molecule on the integral cross sections of rotational excitation in low-temperature collisions of He-Na2. Acta Physica Sinica, 2011, 60(2): 020304. doi: 10.7498/aps.60.020304 [12] Li Wen-Feng, Linghu Rong-Feng, Cheng Xin-Lu, Yang Xiang-Dong. Theoretical calculation of integral cross sections of rotational excitation for collisions in isotopes of He atom with Na2 molecule. Acta Physica Sinica, 2010, 59(7): 4591-4597. doi: 10.7498/aps.59.4591 [13] Yu Chun-Ri, Wang Rong-Kai, Cheng Xin-Lu, Yang Xiang-Dong. Theoretical study of the effect of potential models on scattering cross sections for He-HF system. Acta Physica Sinica, 2007, 56(5): 2577-2584. doi: 10.7498/aps.56.2577 [14] Yu Chun-Ri, Feng Er-Yin, Cheng Xin-Lu, Yang Xiang-Dong. Theoretical study of the potential energy surface and differential scattering cross sections of He-HI complex. Acta Physica Sinica, 2007, 56(8): 4441-4447. doi: 10.7498/aps.56.4441 [15] Jiang Zhen-Yi, Li Sheng-Tao. First principles study of potential energy curves of NiTi alloy. Acta Physica Sinica, 2006, 55(11): 6032-6035. doi: 10.7498/aps.55.6032 [16] Han Hui-Xian, Peng Qian, Wen Zhen-Yi, Wang Yu-Bin. Local potential energy surface and vibration analysis for the S2O molecule. Acta Physica Sinica, 2005, 54(1): 78-84. doi: 10.7498/aps.54.78 [17] Wang Xiao-Yan, Ding Shi-Liang. Constructing potential energy surface of tetratomic molecules using Lie algebra. Acta Physica Sinica, 2004, 53(2): 423-426. doi: 10.7498/aps.53.423 [18] Zhang Cheng-Hua, Qiu Wei, Xin Jun-Li, Nu Ying-Yu, Wang X iao-Wei, Wang Jing-Yang. The calculation of triple-differential cross sections of hydrogen atom single-io nization by electrons. Acta Physica Sinica, 2003, 52(10): 2449-2452. doi: 10.7498/aps.52.2449 [19] Sun Gui-Hua, Yang Xiang-Dong. . Acta Physica Sinica, 2002, 51(3): 506-511. doi: 10.7498/aps.51.506 [20] JIN SHI-QI, XU ZHI-ZHAN. ELECTRON IMPACT WITH ARGON EXCITATION OUT OF THE e-Ar(3p54s,J=2). Acta Physica Sinica, 1998, 47(10): 1621-1624. doi: 10.7498/aps.47.1621
DownLoad:
Catalog
Metrics
- Abstract views: 6041
- PDF Downloads: 70
- Cited By: 0
