Six-Dimensional State-to-State Quantum Dynamics of H<sub>2</sub>/D<sub>2</sub> Scattering from Cu(100): Validity of Site-Averaging Model

Liang Zhang; Lingjun Zhu; Bin Jiang

doi:10.1063/1674-0068/cjcp2111248

Volume 35 Issue 1

Feb. 2022

Turn off MathJax

Article Contents

Article Navigation > Chinese Journal of Chemical Physics > 2022 > 35(1): 143-152

Liang Zhang, Lingjun Zhu, Bin Jiang. Six-Dimensional State-to-State Quantum Dynamics of H2/D2 Scattering from Cu(100): Validity of Site-Averaging Model[J]. Chinese Journal of Chemical Physics , 2022, 35(1): 143-152. doi: 10.1063/1674-0068/cjcp2111248

Citation:

Liang Zhang, Lingjun Zhu, Bin Jiang. Six-Dimensional State-to-State Quantum Dynamics of H₂/D₂ Scattering from Cu(100): Validity of Site-Averaging Model[J]. Chinese Journal of Chemical Physics , 2022, 35(1): 143-152. doi: 10.1063/1674-0068/cjcp2111248

Citation:

PDF( 6730 KB)

Six-Dimensional State-to-State Quantum Dynamics of H₂/D₂ Scattering from Cu(100): Validity of Site-Averaging Model

doi: 10.1063/1674-0068/cjcp2111248

Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, University of Science and Technology of China, Hefei 230026, China

More Information

Corresponding author: Liang Zhang, E-mail: lzhangch@mail.ustc.edu.cn; Bin Jiang, E-mail: bjiangch@ustc.edu.cn
Received Date: 2021-11-23
Accepted Date: 2021-12-16
Publish Date: 2022-02-27

Abstract

Abstract

Six-dimensional quantum dynamics calculations for the state-to-state scattering of H$ _2 $/D$ _2 $ on the rigid Cu(100) surface have been carried out using a time-dependent wave packet approach, based on an accurate neural network potential energy surface fit for thousands of density functional theory data computed with the optPBE-vdW density functional. The present results are compared with previous theoretical and experimental ones regarding to the rovibrationally (in)elastic scattering of H$ _2 $ and D$ _2 $ from Cu(100). In particular, we test the validity of the site-averaging approximation in this system by which the six-dimensional (in)elastic scattering probabilities are compared with the weighted average of four-dimensional results over fifteen fixed sites. Specifically, the site-averaging model reproduces vibrationally elastic scattering probabilities quite well, though less well for vibrationally inelastic results at high energies. These results support the use of the site-averaging model to reduce computational costs in future investigations on the state-to-state scattering dynamics of heavy diatomic or polyatomic molecules from metal surfaces, where full-dimensional calculations are too expensive.
- State-to-state scattering,
- Quantum dynamics,
- Surface,
- Site-averaging

^†Part of Special Issue "In Memory of Prof. Nanquan Lou on the occasion of his 100th anniversary".

FullText(HTML)

References(47)

References

[1]	G. B. Park, B. C. Krüger, D. Borodin, T. N. Kitsopoulos, and A. M. Wodtke, Rep. Prog. Phys. 82, 096401 (2019). doi: 10.1088/1361-6633/ab320e
[2]	B. Jiang, R. Liu, J. Li, D. Xie, M. Yang, and H. Guo, Chem. Sci. 4, 3249 (2013). doi: 10.1039/c3sc51040a
[3]	B. Jiang, M. Yang, D. Xie, and H. Guo, Chem. Soc. Rev. 45, 3621 (2016). doi: 10.1039/C5CS00360A
[4]	S. Nave, A. K. Tiwari, and B. Jackson, J. Phys. Chem. A 118, 9615 (2014). doi: 10.1021/jp5063644
[5]	J. Werdecker, M. E. van Reijzen, B. J. Chen, and R. D. Beck, Phys. Rev. Lett. 120, 053402 (2018). doi: 10.1103/PhysRevLett.120.053402
[6]	L. Zhang and B. Jiang, Phys. Rev. Lett. 123, 106001 (2019). doi: 10.1103/PhysRevLett.123.106001
[7]	L. Zhang and B. Jiang, J. Chem. Phys. 153, 214702 (2020). doi: 10.1063/5.0030490
[8]	J. Werdecker, B. J. Chen, M. E. Van Reijzen, A. Farjamnia, B. Jackson, and R. D. Beck, Phys. Rev. Res. 2, 043251 (2020). doi: 10.1103/PhysRevResearch.2.043251
[9]	G. J. Kroes, Phys. Chem. Chem. Phys. 14, 14966 (2012). doi: 10.1039/c2cp42471a
[10]	G. J. Kroes, Prog. Surf. Sci. 60, 1 (1999). doi: 10.1016/S0079-6816(99)00006-4
[11]	B. Jiang and H. Guo, Phys. Chem. Chem. Phys. 16, 24704 (2014). doi: 10.1039/C4CP03761H
[12]	T. Liu, B. Fu, and D. H. Zhang, J. Chem. Phys. 139, 184705 (2013). doi: 10.1063/1.4829508
[13]	Z. Zhang, T. Liu, B. Fu, X. Yang, and D. H. Zhang, Nat. Comm. 7, 11953 (2016). doi: 10.1038/ncomms11953
[14]	T. Liu, J. Chen, Z. Zhang, X. Shen, B. Fu, and D. H. Zhang, J. Chem. Phys. 148, 144705 (2018). doi: 10.1063/1.5023069
[15]	X. Hu, B. Jiang, D. Xie, and H. Guo, J. Chem. Phys. 143, 114706 (2015). doi: 10.1063/1.4931040
[16]	T. Liu, B. Fu, and D. H. Zhang, J. Chem. Phys. 146, 164706 (2017). doi: 10.1063/1.4982051
[17]	T. Liu, B. Fu, and D. H. Zhang, J. Chem. Phys. 149, 054702 (2018). doi: 10.1063/1.5036805
[18]	T. Liu, B. Fu, and D. H. Zhang, J. Chem. Phys. 141, 194302 (2014). doi: 10.1063/1.4901894
[19]	J. Dai and J. C. Light, J. Chem. Phys. 107, 1676 (1997). doi: 10.1063/1.474520
[20]	H. Shi, T. Liu, Y. Fu, X. Lu, B. Fu, and D. H. Zhang, J. Phys. Chem. C 125, 23105 (2021). doi: 10.1021/acs.jpcc.1c05334
[21]	B. Jiang and H. Guo, J. Chem. Phys. 143, 164705 (2015). doi: 10.1063/1.4934357
[22]	B. Jiang, H. Song, M. Yang, and H. Guo, J. Chem. Phys. 144, 164706 (2016). doi: 10.1063/1.4947492
[23]	E. Watts and G. O. Sitz, J. Chem. Phys. 114, 4171 (2001). doi: 10.1063/1.1344233
[24]	L. C. Shackman and G. O. Sitz, J. Chem. Phys. 123, 064712 (2005). doi: 10.1063/1.1993555
[25]	L. Sementa, M. Wijzenbroek, B. J. v. Kolck, M. F. Somers, A. Al-Halabi, H. F. Busnengo, R. A. Olsen, G. J. Kroes, M. Rutkowski, C. Thewes, N. F. Kleimeier, and H. Zacharias, J. Chem. Phys. 138, 044708 (2013). doi: 10.1063/1.4776224
[26]	C. Díaz, E. Pijper, R. A. Olsen, H. F. Busnengo, D. J. Auerbach, and G. J. Kroes, Science 326, 832 (2009). doi: 10.1126/science.1178722
[27]	L. Zhu, Y. Zhang, L. Zhang, X. Zhou, and B. Jiang, Phys. Chem. Chem. Phys. 22, 13958 (2020). doi: 10.1039/D0CP02291H
[28]	J. Klimeš, D. R. Bowler, and A. Michaelides, J. Phys. : Condens. Matter 22, 022201 (2010). doi: 10.1088/0953-8984/22/2/022201
[29]	Y. Zhang, C. Hu, and B. Jiang, J. Phys. Chem. Lett. 10, 4962 (2019). doi: 10.1021/acs.jpclett.9b02037
[30]	G. Kresse and J. Furthmuller, Comp. Mater. Sci. 6, 15 (1996). doi: 10.1016/0927-0256(96)00008-0
[31]	G. Kresse and J. Furthmuller, Phys. Rev. B 54, 11169 (1996). doi: 10.1103/PhysRevB.54.11169
[32]	P. E. Blöchl, Phys. Rev. B 50, 17953 (1994). doi: 10.1103/PhysRevB.50.17953
[33]	J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996). doi: 10.1103/PhysRevLett.77.3865
[34]	R. Yin, Y. Zhang, and B. Jiang, J. Phys. Chem. Lett. 10, 5969 (2019). doi: 10.1021/acs.jpclett.9b01806
[35]	M. Huang, X. Zhou, Y. Zhang, L. Zhou, M. Alducin, B. Jiang, and H. Guo, Phys. Rev. B 100, 201407(R) (2019).
[36]	Y. Zhang, R. J. Maurer, and B. Jiang, J. Phys. Chem. C 124, 186 (2020). doi: 10.1021/acs.jpcc.9b09965
[37]	C. Hu, Y. Zhang, and B. Jiang, J. Phys. Chem. C 124, 23190 (2020). doi: 10.1021/acs.jpcc.0c07182
[38]	R. Yin and B. Jiang, Phys. Rev. Lett. 126, 156101 (2021). doi: 10.1103/PhysRevLett.126.156101
[39]	Q. Lin, L. Zhang, Y. Zhang, and B. Jiang, J. Chem. Theory Comput. 17, 2691 (2021). doi: 10.1021/acs.jctc.1c00166
[40]	D. T. Colbert and W. H. Miller, J. Chem. Phys. 96, 1982 (1992). doi: 10.1063/1.462100
[41]	D. H. Zhang and J. Z. H. Zhang, J. Chem. Phys. 99, 5615 (1993). doi: 10.1063/1.465954
[42]	J. Dai and J. C. Light, J. Chem. Phys. 107, 8432 (1997). doi: 10.1063/1.475043
[43]	J. A. Flect Jr., J. R. Morris, and M. D. Feit, Appl. Phys. 10, 129 (1976).
[44]	S. Y. Lin and H. Guo, J. Chem. Phys. 119, 11602 (2003). doi: 10.1063/1.1624060
[45]	S. Y. Lin and H. Guo, J. Chem. Phys. 117, 5183 (2002). doi: 10.1063/1.1500731
[46]	J. Dai and J. Z. H. Zhang, J. Phys. Chem. 100, 6898 (1996). doi: 10.1021/jp9536662
[47]	F. Nattino, C. Díaz, B. Jackson, and G. J. Kroes, Phys. Rev. Lett. 108, 236104 (2012). doi: 10.1103/PhysRevLett.108.236104