Benchmark Quantum Mechanical Calculations of Vibrationally Resolved Cross Sections and Rate Constants on ab Initio Potential Energy Surfaces for the F plus HD Reaction: Comparisons with Experiments

De Fazio Dario; Cavalli Simonetta; Aquilanti Vincenzo

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Benchmark Quantum Mechanical Calculations of Vibrationally Resolved Cross Sections and Rate Constants on ab Initio Potential Energy Surfaces for the F plus HD Reaction: Comparisons with Experiments

机译：F + HD反应从头计算势能面上振动解析截面和速率常数的基准量子力学计算：与实验的比较

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Quantum scattering calculations within the time-independent approach in an extended interval of energies were performed for the title reaction on four ab initio potential energy surfaces. The calculated integral cross sections, vibrational branching ratios, and rate constants are compared with scattering experiments as well as with chemical kinetics rate data available for this system for both the HF and DF channels. The calculations on the CSZ (J. Chem. Phys. 2015, 142, 024303) and LWAL (J. Chem. Phys. 2007, 127, 174302) surfaces are in close agreement between them and reproduce satisfactorily the experimental measurements. The agreement with the experiments is improved with respect to calculations on the earlier SW (J. Chem. Phys. 1996, 104, 6515) and FXZ (J. Chem. Phys. 2008, 129, 011103) surfaces. The results presented here witness the remarkable progress made by quantum chemistry calculations in describing the interatomic interactions governing the dynamics and kinetics of this reaction. They also suggest that comparison with translationally and rotationally averaged experimental observables is not sufficient to assess the relative accuracy of highly accurate potential energy surfaces. The dynamics and kinetics calculations show that temperatures lower than 50 K or molecular beam energy spread below 1 meV must be reached to discriminate the accuracy of the LWAL and the CSZ surfaces.

机译：在四个从头算势能面上进行标题反应的时间独立方法中，在扩展的能量间隔内进行了量子散射计算。将计算出的积分横截面，振动分支比和速率常数与散射实验以及该系统可用于HF和DF通道的化学动力学速率数据进行比较。 CSZ（J. Chem。Phys。2015，142，024303）和LWAL（J. Chem。Phys。2007，127，174302）表面之间的计算彼此之间非常吻合，并且可以令人满意地重现实验测量值。在较早的SW（J.Chem.Phys.1996，104，6515）和FXZ（J.Chem.Phys.2008，129，011103）表面上的计算方面，与实验的一致性得到改善。此处给出的结果见证了量子化学计算在描述控制该反应动力学和动力学的原子间相互作用方面取得的显着进展。他们还建议，与平移和旋转平均实验可观察值进行比较不足以评估高精度势能面的相对精度。动力学和动力学计算表明，必须达到低于50 K的温度或低于1 meV的分子束能量传播，才能区分LWAL和CSZ表面的精度。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2016年第27期|共12页
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De Fazio Dario; Cavalli Simonetta; Aquilanti Vincenzo;
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1. Benchmark Quantum Mechanical Calculations of Vibrationally Resolved Cross Sections and Rate Constants on ab Initio Potential Energy Surfaces for the F plus HD Reaction: Comparisons with Experiments [J] . De Fazio Dario, Cavalli Simonetta, Aquilanti Vincenzo The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2016,第27期

机译：F + HD反应从头计算势能面上振动解析截面和速率常数的基准量子力学计算：与实验的比较
2. Reaction Cross Sections and Rate Constants for the Cl + H_2 Reaction from Quasiclassical Trajectory Calculation on Two New ab Initio Potential Energy Surfaces [J] . Changsheng Shen, Tao Wu, Guanzhi Ju, The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2002,第1期

机译：从两个新的从头算起的势能面的拟经典轨迹计算，Cl + H_2反应的反应截面和速率常数
3. The dynamics of the prototype abstraction reaction Cl(~2P_(3/1,1/2)) + H_2:A comparison of crossed molecular beam experiments with exact quantum scattering calculations on coupled ab initio potential energy surfaces [J] . Nadia Balucani, Dimitris Skouteris, Giovanni Capozza Physical chemistry chemical physics: PCCP . 2004,第21期

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4. Ab Initio Evaluation of Reaction Rate Constants for Elementary Al Combustion Reactions - Part I: Potential Energy Surface Computation [C] . N. Butuk, R. Berry, T. Miller AIAA/ASME/SAE/ASEE Joint Propulsion Conference Exhibit . 2007

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7. Reaction cross section and rate constant calculations for the D + H2(v=0,1) → HD + H reaction on three ab initio potential energy surfaces. A quasiclassical trajectory study [O] . Aoiz F. Javier, Bañares Luis, Díez-Rojo T., 2013

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Benchmark Quantum Mechanical Calculations of Vibrationally Resolved Cross Sections and Rate Constants on ab Initio Potential Energy Surfaces for the F plus HD Reaction: Comparisons with Experiments

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