Quasiclassical trajectory calculations of the dissociation dynamics of CH3CHO at high energy yield many products

Journal of Physical Chemistry Letters

Volumn 2, Issue 14, 2011, Pages 1715-1719

  Han, Yong Chang ^a   Shepler, Benjamin C ^a,b   Bowman, Joel M ^a  

^a EMORY UNIVERSITY   (United States)

^b Georgia Gwinett College   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

BRANCHING RATIO; DISSOCIATION DYNAMICS; GLOBAL MINIMA; HIGH ENERGY; INTERNAL ENERGIES; PHOTOLYSIS WAVELENGTH; PRODUCT CHANNEL; QUASICLASSICAL TRAJECTORIES; QUASICLASSICAL TRAJECTORY CALCULATIONS; TOTAL ENERGY; VINYLALCOHOL;

ACETALDEHYDE; ACETYLENE; HIGH ENERGY PHYSICS; ISOMERS; LIGHTING; PHOTODISSOCIATION; PHOTOLYSIS; QUANTUM CHEMISTRY; TRAJECTORIES;

CALCULATIONS;

EID: 79960723281     PISSN: None     EISSN: 19487185     Source Type: Journal    
DOI: 10.1021/jz200719x     Document Type: Article

References (32)

1. Horowitz, A.; Calvert, J. G. Wavelength Dependence of the Primary Processes in Acetaldehyde Photolysis J. Phys. Chem. 1982, 86, 3105-3114
2. a) and Translational Distributions of the HCO Photoproduct J. Phys. Chem. 1994, 98, 10802-10808
3. 2A′) from Acetaldehyde: Distributions of Rotational States and Preferential Population of K Doublets of HCO J. Chem. Phys. 1996, 105, 4597/1-8
4. 3 + HCO J. Chem. Phys. 2000, 112, 1797/1-7
5. 4 + CO Channel J. Chem. Phys. 2001, 114, 6128/1-6
6. 1 Acetaldehyde: The Transition from Impulsive to Statistical Dynamics J. Chem. Phys. 2006, 124, 044302/1-15
7. Houston, P. L.; Kable, S. H. Photodissociation of Acetaldehyde as a Second Example of the Roaming Mechanism Proc. Natl. Acad. Sci. U.S.A. 2006, 103, 16079-16082 (Pubitemid 44715154)
8. Rubio-Lago, L.; Amaral, G. A.; Arregui, A.; Izquierdo, J. G.; Wang, F.; Zaouris, D.; Kitsopoulos, T. N.; Banares, L. Slice Imaging of the Photodissociation of Acetaldehyde at 248 nm. Evidence of a Roaming Mechanism Phys. Chem. Chem. Phys. 2007, 9, 6123-6127
9. 3CHO J. Chem. Phys. 2009, 130, 054310/1-8
10. Lee, S.-H. Dynamics of Multidissociation Paths of Acetaldehyde Photoexcited at 157 nm: Branching Ratios, Distributions of Kinetic Energy, and Angular Anisotropies of Products J. Chem. Phys. 2009, 131, 174312/1-10
11. Amaral, G. A.; Arregui, A.; Rubio-Lago, L.; Rodríguez, J. D.; Banares, L. Imaging the Radical Channel in Acetaldehyde Photodissociation: Competing Mechanisms at Energies Close to the Triplet Exit Barrier J. Chem. Phys. 2010, 133, 064303/1-8
12. 3CHO. J. Chem. Phys. 2011, in press.
13. 3CHO Photodissociation Nat. Chem. 2011, 3, 443-448
14. Yadav, J. S.; Goddard, J. D. Acetaldehyde Photochemistry: The Radical and Molecular Dissociations J. Chem. Phys. 1986, 84, 2682/1-9
15. King, R. A.; Allen, W. D.; Schaefer, H. F., III. On Apparent Quantized Transition-State Thresholds in the Photofragmentation of Acetaldehyde J. Chem. Phys. 2000, 112, 5585/1-8
16. 4 + CO: Direct Ab Initio Dynamics Study J. Phys. Chem. A 2002, 106, 11415-11421 (Pubitemid 35433822)
17. 3 + HCO: Direct Ab Initio Molecular Dynamics Study Chem. Phys. Lett. 2003, 371, 568-575 (Pubitemid 36379712)
18. 4 + CO: II. Direct Ab Initio Molecular Dynamics Study Chem. Phys. Lett. 2006, 421, 549-553
19. Kurosaki, Y. Hydrogen-Atom Production Channels of Acetaldehyde Photodissociation: Direct DFT Molecular Dynamics Study J. Mol. Struct. (THEOCHEM) 2008, 850, 9-16
20. Chen, S.; Fang, W.-H. Insights into Photodissociation Dynamics of Acetaldehyde from Ab Initio Calculations and Molecular Dynamics Simulations J. Chem. Phys. 2009, 131, 054306/1-6
21. Shepler, B. C.; Braams, B. J.; Bowman, J. M. Quasiclassical Trajectory Calculations of Acetaldehyde Dissociation on a Global Potential Energy Surface Indicate Significant Non-transition State Dynamics J. Phys. Chem. A 2007, 111, 8282-8285 (Pubitemid 47387978)
22. 3CHO Photodissociation Revealed on a Global Potential Energy Surface J. Phys. Chem. A 2008, 112, 9344-9351
23. Townsend, D.; Lahankar, S. A.; Lee, S. K.; Chambreau, S. D.; Suits, A. G.; Zhang, X.; Rheinecker, J.; Harding, L. B.; Bowman, J. M. The Roaming Atom: Straying from the Reaction Path in Formaldehyde Decomposition Science 2004, 306, 1158-1161 (Pubitemid 39488989)
24. Suits, A. G. Roaming Atoms and Radicals: A New Mechanism in Molecular Dissociation Acc. Chem. Res. 2008, 41, 873-881
25. Bowman, J. M.; Shepler, B. C. Roaming Radicals Annu. Rev. Phys. Chem. 2011, 62, 531-553
26. Heazlewood, B. R.; Jordan, M. J. T.; Kable, S. H.; Selby, T. M.; Osborn, D. L.; Shepler, B. C.; Braams, B. J.; Bowman, J. M. Roaming is the Dominant Mechanism for Molecular Products in Acetaldehyde Photodissociation Proc. Natl. Acad. Sci. U.S.A. 2008, 105, 12719-12724
27. Chen, C.; Braams, B.; Lee, D. Y.; Bowman, J. M.; Houston, P. L.; Stranges, D. Evidence for Vinylidene Production in the Photodissociation of the Allyl Radical J. Phys. Chem. Lett. 2010, 1, 1875-1880
28. Chen, C; Braams, B. J.; Lee, D. Y.; Bowman, J. M.; Houston, P. L.; Stranges, D. The Dynamics of Allyl Radical Dissociation J. Phys. Chem. A 2011, 115, 6797-6804
29. Werner, H.-J.; Knowles, P. J.; Lindh, R.; Manby, F. R.; Schuetz, M.; Celani, P.; Korona, T.; Rauhut, G.; Amos, R. D.; Bernhardsson, A. MOLPRO, version 2006.1, a package of ab initio programs. See http://www.molpro.net.
30. Braams, B. J.; Bowman, J. M. Permutationally Invariant Potential Energy Surfaces in High Dimensionality Int. Rev. Phys. Chem. 2009, 28, 577-606
31. 4, O] System from Ab Initio Calculations by the Scaled Hypersphere Search Method J. Phys. Chem. A 2007, 111, 5099-5110 (Pubitemid 47012624)
32. Zou, S.; Bowman, J. M. A New Ab Initio Potential Energy Surface Describing Acetylene/Vinylidene Isomerization Chem. Phys. Lett. 2003, 368, 421-424 (Pubitemid 36027820)