# Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials

Welsch R, Manthe U (2012)

The Journal Of Chemical Physics 137(24).

Download

**No fulltext has been uploaded. References only!**

*Journal Article*|

*Published*|

*English*

No fulltext has been uploaded

Author

Department

Abstract

The multi-layer extension of the multi-configurational time-dependent Hartree (MCTDH) approach is applied to the investigation of elementary bimolecular chemical reactions. Cumulative reaction probabilities and thermal rate constants of the H + CH4 -> H-2 + CH3 reaction are calculated using flux correlation functions and the quantum transition state concept. Different coordinate systems and potential energy surfaces (PESs) are studied. The convergence properties of different layerings are investigated and the efficiency of multi-layer MCTDH approach is compared to the standard MCTDH approach. It is found that the multi-layer approach can decrease the numerical effort by more than an order of magnitude. The increased efficiency resulting from the multi-layer MCTDH approach is crucial for quantum dynamical calculations on recent global H + CH4 -> H-2 + CH3 PESs, e. g., the ZBB3-PES [Z. Xie, J. M. Bowman, and X. Zhang, J. Chem. Phys. 125, 133120 (2006)] based on permutational invariant polynomials, which are numerically more demanding than earlier PESs. The results indicate that an accurate description of all transition state frequencies is important to obtain accurate thermal rate constants. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4772585]

Publishing Year

ISSN

PUB-ID

### Cite this

Welsch R, Manthe U. Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials.

*The Journal Of Chemical Physics*. 2012;137(24).Welsch, R., & Manthe, U. (2012). Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials.

*The Journal Of Chemical Physics*,*137*(24), 244106. doi:10.1063/1.4772585Welsch, R., and Manthe, U. (2012). Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials.

*The Journal Of Chemical Physics*137.Welsch, R., & Manthe, U., 2012. Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials.

*The Journal Of Chemical Physics*, 137(24).R. Welsch and U. Manthe, “Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials”,

*The Journal Of Chemical Physics*, vol. 137, 2012.Welsch, R., Manthe, U.: Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials. The Journal Of Chemical Physics. 137, (2012).

Welsch, Ralph, and Manthe, Uwe. “Reaction dynamics with the multi-layer multi-configurational time-dependent Hartree approach: H + CH4 -> H-2 + CH3 rate constants for different potentials”.

*The Journal Of Chemical Physics*137.24 (2012).
This data publication is cited in the following publications:

This publication cites the following data publications:

### 13 Citations in Europe PMC

Data provided by Europe PubMed Central.

An investigation of one- versus two-dimensional semiclassical transition state theory for H atom abstraction and exchange reactions.

Greene SM, Shan X, Clary DC.,

PMID: 26931687

Greene SM, Shan X, Clary DC.,

*J Chem Phys*144(8), 2016PMID: 26931687

Oscillatory reaction cross sections caused by normal mode sampling in quasiclassical trajectory calculations.

Nagy T, Vikar A, Lendvay G.,

PMID: 26747798

Nagy T, Vikar A, Lendvay G.,

*J Chem Phys*144(1), 2016PMID: 26747798

Mode specific dynamics of the H2 + CH3 → H + CH4 reaction studied using quasi-classical trajectory and eight-dimensional quantum dynamics methods.

Wang Y, Li J, Chen L, Lu Y, Yang M, Guo H.,

PMID: 26493907

Wang Y, Li J, Chen L, Lu Y, Yang M, Guo H.,

*J Chem Phys*143(15), 2015PMID: 26493907

A permutationally invariant full-dimensional ab initio potential energy surface for the abstraction and exchange channels of the H + CH4 system.

Li J, Chen J, Zhao Z, Xie D, Zhang DH, Guo H.,

PMID: 26026442

Li J, Chen J, Zhao Z, Xie D, Zhang DH, Guo H.,

*J Chem Phys*142(20), 2015PMID: 26026442

Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 → H2 + CH3 reaction on a neural network PES.

Welsch R, Manthe U.,

PMID: 25681908

Welsch R, Manthe U.,

*J Chem Phys*142(6), 2015PMID: 25681908

The role of the transition state in polyatomic reactions: initial state-selected reaction probabilities of the H + CH₄ → H₂ + CH₃ reaction.

Welsch R, Manthe U.,

PMID: 25381520

Welsch R, Manthe U.,

*J Chem Phys*141(17), 2014PMID: 25381520

Correlation functions for fully or partially state-resolved reactive scattering calculations.

Manthe U, Welsch R.,

PMID: 24985624

Manthe U, Welsch R.,

*J Chem Phys*140(24), 2014PMID: 24985624

Accuracy of the centrifugal sudden approximation in the H + CHD₃ → H₂ + CD₃ reaction.

Zhang Z, Chen J, Liu S, Zhang DH.,

PMID: 24929385

Zhang Z, Chen J, Liu S, Zhang DH.,

*J Chem Phys*140(22), 2014PMID: 24929385

Calculation of state-to-state cross sections for triatomic reaction by the multi-configuration time-dependent Hartree method.

Zhao B, Zhang DH, Lee SY, Sun Z.,

PMID: 24784254

Zhao B, Zhang DH, Lee SY, Sun Z.,

*J Chem Phys*140(16), 2014PMID: 24784254

Multi-layer Potfit: an accurate potential representation for efficient high-dimensional quantum dynamics.

Otto F.,

PMID: 24410220

Otto F.,

*J Chem Phys*140(1), 2014PMID: 24410220

Coupled potential energy surface for the F(2P)+CH4→HF+CH3 entrance channel and quantum dynamics of the CH4·F- photodetachment.

Westermann T, Eisfeld W, Manthe U.,

PMID: 23822305

Westermann T, Eisfeld W, Manthe U.,

*J Chem Phys*139(1), 2013PMID: 23822305

Fast Shepard interpolation on graphics processing units: potential energy surfaces and dynamics for H + CH4 → H2 + CH3.

Welsch R, Manthe U.,

PMID: 23635122

Welsch R, Manthe U.,

*J Chem Phys*138(16), 2013PMID: 23635122

Rate coefficients and kinetic isotope effects of the X + CH4 → CH3 + HX (X = H, D, Mu) reactions from ring polymer molecular dynamics.

Li Y, Suleimanov YV, Li J, Green WH, Guo H.,

PMID: 23485294

Li Y, Suleimanov YV, Li J, Green WH, Guo H.,

*J Chem Phys*138(9), 2013PMID: 23485294

### 109 References

Data provided by Europe PubMed Central.

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

AUTHOR UNKNOWN, 0

Calculating initial-state-selected reaction probabilities from thermal flux eigenstates: a transition-state-based approach.

Huarte-Larranaga F, Manthe U.,

PMID: 16351247

Huarte-Larranaga F, Manthe U.,

*J Chem Phys*123(20), 2005PMID: 16351247

State-to-state reaction probabilities within the quantum transition state framework.

Welsch R, Huarte-Larranaga F, Manthe U.,

PMID: 22360179

Welsch R, Huarte-Larranaga F, Manthe U.,

*J Chem Phys*136(6), 2012PMID: 22360179

AUTHOR UNKNOWN, 0

### Export

0 Marked Publications### Web of Science

View record in Web of Science®### Sources

PMID: 23277927

PubMed | Europe PMC