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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
Source PublicationJOURNAL OF CHEMICAL PHYSICS
2014-09-28
DOI10.1063/1.4896201
Volume141Issue:12
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectPhysics, Atomic, Molecular & Chemical
WOS Research AreaPhysics
WOS KeywordCRIEGEE 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
AbstractEmploying 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.
Language英语
WOS IDWOS:000342844100039
Citation statistics
Cited Times:20[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/145675
Collection中国科学院大连化学物理研究所
Affiliation1.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
Recommended Citation
GB/T 7714
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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