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A full-dimensional multilayer multiconfiguration time-dependent Hartree study on the ultraviolet absorption spectrum of formaldehyde oxide
Meng, Qingyong1; Meyer, Hans-Dieter2
刊名JOURNAL OF CHEMICAL PHYSICS
2014-09-28
DOI10.1063/1.4896201
141期:12
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Physics, Atomic, Molecular & Chemical
研究领域[WOS]Physics
关键词[WOS]CRIEGEE INTERMEDIATE CH2OO ; CONFIGURATION-INTERACTION CALCULATIONS ; CORRELATED MOLECULAR CALCULATIONS ; GAUSSIAN-BASIS SETS ; SULFURIC-ACID CONCENTRATIONS ; CONSISTENT BASIS-SETS ; WAVE-FUNCTIONS ; PROPAGATING WAVEPACKETS ; BENCHMARK CALCULATIONS ; MCTDH METHOD
英文摘要Employing the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method in conjunction with the multistate multimode vibronic coupling Hamiltonian (MMVCH) model, we perform a full dimensional (9D) quantum dynamical study on the simplest Criegee intermediate, formaldehyde oxide, in five lower-lying singlet electronic states. The ultraviolet (UV) spectrum is then simulated by a Fourier transform of the auto-correlation function. The MMVCH model is built based on extensive MRCI(8e, 8o)/aug-cc-pVTZ calculations. To ensure a fast convergence of the final calculations, a large number of ML-MCTDH test calculations is performed to find an appropriate multilayer separations (ML-trees) of the ML-MCTDH nuclear wave functions, and the dynamical calculations are carefully checked to ensure that the calculations are well converged. To compare the computational efficiency, standard MCTDH simulations using the same Hamiltonian are also performed. A comparison of the MCTDH and ML-MCTDH calculations shows that even for the present not-too-large system (9D here) the ML-MCTDH calculations can save a considerable amount of computational resources while producing identical spectra as the MCTDH calculations. Furthermore, the present theoretical (B) over tilde (1) A ' <- (X) over tilde (1) A ' UV spectral band and the corresponding experimental measurements [J. M. Beames, F. Liu, L. Lu, and M. I. Lester, J. Am. Chem. Soc. 134, 20045-20048 (2012); L. Sheps, J. Phys. Chem. Lett. 4, 4201-4205 (2013); W.-L. Ting, Y.-H. Chen, W. Chao, M. C. Smith, and J. J.-M. Lin, Phys. Chem. Chem. Phys. 16, 10438-10443 (2014)] are discussed. To the best of our knowledge, this is the first theoretical UV spectrum simulated for this molecule including nuclear motion beyond an adiabatic harmonic approximation. (C) 2014 AIP Publishing LLC.
语种英语
WOS记录号WOS:000342844100039
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/145675
专题中国科学院大连化学物理研究所
作者单位1.Chinese Acad Sci, State Key Lab Mol React Dynam, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
2.Heidelberg Univ, Inst Phys Chem, D-69120 Heidelberg, Germany
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Meng, Qingyong,Meyer, Hans-Dieter. A full-dimensional multilayer multiconfiguration time-dependent Hartree study on the ultraviolet absorption spectrum of formaldehyde oxide[J]. JOURNAL OF CHEMICAL PHYSICS,2014,141(12).
APA Meng, Qingyong,&Meyer, Hans-Dieter.(2014).A full-dimensional multilayer multiconfiguration time-dependent Hartree study on the ultraviolet absorption spectrum of formaldehyde oxide.JOURNAL OF CHEMICAL PHYSICS,141(12).
MLA Meng, Qingyong,et al."A full-dimensional multilayer multiconfiguration time-dependent Hartree study on the ultraviolet absorption spectrum of formaldehyde oxide".JOURNAL OF CHEMICAL PHYSICS 141.12(2014).
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