Theoretical Chemistry Accounts

, Volume 128, Issue 4–6, pp 727–734 | Cite as

On the anomaly of the quasiclassical product distributions of the \(\hbox{OH} +\hbox{CO} \rightarrow\hbox{H} +\hbox{CO}_2\) reaction

Regular Article
First Online:
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Abstract

A grid empowered molecular simulator (GEMS) embodying in a single workflow the ab initio treatment of elementary chemical processes has been extended to four atom reactions. GEMS has been used to carry out a massive quasiclassical investigation for the \(\hbox{OH} +\hbox{CO} \rightarrow\hbox{H} +\hbox{CO}_2\) reaction on the most recently proposed potential energy surface. The type of potential energy surface used and the possibility of running the simulations on the grid have allowed us to keep the error of the order of a few percent at all values of the collision energy and to estimate accurately the dependence of the reaction cross section on the collision energy. The accuracy of the calculations has allowed to unequivocally single out the fact that the calculated center-of-mass angular distribution is clearly isotropic and radically differs from the asymmetric forward–backward structure obtained from the experiment. However, when the laboratory frame analogues are compared, the difference almost vanishes.

Keywords

Reactive scattering OH + CO reaction Quasiclassical trajectories Product distributions Molecular simulator Chemistry on grid 
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Notes

Acknowledgments

The Leiden ab initio results were kindly supplied to us by R. Valero and G.J. Kroes. The LAB_AD program was kindly supplied to us by F.J. Aoiz. Partial financial support from Spanish MICINN (CTQ-2008-02578/BQU), Italian MIUR, EGEE-III and ARPA Umbria is acknowledged. This work has been carried out also as part of the activities of the cooperation scheme of the QDYN working group of the COST CMST European Cooperative Project CHEMGRID (Action D37). Computational assistance and resources were provided by the IZO-SGI SGIker (UPV/EHU, MICINN, GV/EJ, ESF), Spanish Supercomputing Network (BSC-RES) and CINECA.

References

  1. 1.
    Warnatz J, Maas U, Dibble RW (2006) Combustion: physical and chemical fundamentals, modeling and simulation, experiments, pollutant formation, 4th edn. Springer, BerlinGoogle Scholar
  2. 2.
    Miller JA, Kee RJ, Westbrook CK (1990) Annu Rev Phys Chem 41:345CrossRefGoogle Scholar
  3. 3.
    Wayne RP (2000) Chemistry of atmospheres. Oxford University Press, OxfordGoogle Scholar
  4. 4.
    Finlayson-Pitts BJ, Pitts JN (2000) Chemistry of the upper and lower atmosphere theory. Academic Press, LondonGoogle Scholar
  5. 5.
    Westenberg AA, deHaas NJ (1973) J Chem Phys 58:4061CrossRefGoogle Scholar
  6. 6.
    Vandooren J, Peters J, Van Tiggelen PJ (1975) Proc Combust Inst 15:745Google Scholar
  7. 7.
    Ravishankara AR, Thompson RL (1983) Chem Phys Lett 99:377CrossRefGoogle Scholar
  8. 8.
    Wooldridge MS, Hanson RK, Bowman CT (1994) Proc Combust Inst 25:741Google Scholar
  9. 9.
    Lissianski V, Yang H, Qin Z, Mueller MR, Shin KS, Gardiner WC Jr (1995) Chem Phys Lett 240:57CrossRefGoogle Scholar
  10. 10.
    Wooldridge MS, Hanson RK, Bowman CT (1996) Int J Chem Kinet 28:361CrossRefGoogle Scholar
  11. 11.
    Feilberg KL, Sellevåg SR, Nielsen CJ, Griffith WDT, Johnson MS (2002) Phys Chem Chem Phys 4:4687CrossRefGoogle Scholar
  12. 12.
    Fulle D, Hamann HF, Hippler H, Troe J (1996) J Chem Phys 105:983CrossRefGoogle Scholar
  13. 13.
    Golden DM, Smith GP, McEwen AB, Yu CL, Eiteneer B, Frenklach M, Vaghjiani GL, Ravishankara AR, Tully FP (1998) J Phys Chem A 102:8598CrossRefGoogle Scholar
  14. 14.
    Senosiain JP, Musgrave CB, Golden DM (2003) Int J Chem Kinet 35:464CrossRefGoogle Scholar
  15. 15.
    Senosiain JP, Klipenstein SJ, Miller JA (2005) Proc Combust Inst 30:945CrossRefGoogle Scholar
  16. 16.
    Li J, Zhao Z, Kazakov A, Chaos M, Dryer FL, Scire JJ Jr (2007) Int J Chem Kinet 39:109CrossRefGoogle Scholar
  17. 17.
    Wolfrum J (1987) Faraday Discuss Chem Soc 84:191CrossRefGoogle Scholar
  18. 18.
    Koppe S, Laurent T, Volpp HR, Wolfrum J, Naik PD (1996) In: 26th symposium (Int) on combustion, The Combustion Institute, Pittsburgh, 489Google Scholar
  19. 19.
    Alagia M, Balucani N, Casavecchia P, Stranges D, Volpi GG (1993) J Chem Phys 98:8341CrossRefGoogle Scholar
  20. 20.
    Alagia M, Balucani N, Casavecchia P, Stranges D, Volpi GG (1995) J Chem Soc Faraday Trans 91:575CrossRefGoogle Scholar
  21. 21.
    Casavecchia P, Balucani N, Volpi GG (1995) In: Liu K, Wagner A (eds) The chemical dynamics and kinetics of small radicals. World Scientific, SingaporeGoogle Scholar
  22. 22.
    Zhu RS, Diau EGW, Lin MC, Mebel AM (2001) J Phys Chem A 105:11249CrossRefGoogle Scholar
  23. 23.
    Chen WC, Marcus RA (1995) J Chem Phys 123:094307CrossRefGoogle Scholar
  24. 24.
    Chen WC, Marcus RA (1995) J Chem Phys 124:024306CrossRefGoogle Scholar
  25. 25.
    Joshi AV, Wang H (2006) Int J Chem Kinet 38:57CrossRefGoogle Scholar
  26. 26.
    Bowman JM, Schatz GC (1995) Annu Rev Phys Chem 46:169CrossRefGoogle Scholar
  27. 27.
    Kudla K, Schatz GC (2005) In: Liu K, Wagner A (eds) The chemical dynamics and kinetics of small radicals. World Scientific, SingaporeGoogle Scholar
  28. 28.
    Clary DC, Schatz GC (1993) J Chem Phys 99:4578CrossRefGoogle Scholar
  29. 29.
    Hernández MI, Clary DC (1994) J Chem Phys 101:2779CrossRefGoogle Scholar
  30. 30.
    Goldfield EM, Gray SK, Schatz GC (1995) J Chem Phys 102:8807CrossRefGoogle Scholar
  31. 31.
    Zhang DH, Zhang JZH (1995) J Chem Phys 103:6512CrossRefGoogle Scholar
  32. 32.
    Balakrishnan N, Billing GD (1996) J Chem Phys 104:4005CrossRefGoogle Scholar
  33. 33.
    Dzegilenko FN, Bowman JM (1998) J Chem Phys 108:511CrossRefGoogle Scholar
  34. 34.
    Billing GD, Muckerman JT, Yu HG (2002) J Chem Phys 117:4755CrossRefGoogle Scholar
  35. 35.
    Valero R, Kroes GJ (2002) J Chem Phys 117:8736CrossRefGoogle Scholar
  36. 36.
    McCormack DA, Kroes GJ (2003) Chem Phys Lett 352:281; Erratum, ibid. 373:648Google Scholar
  37. 37.
    Lakin MJ, Troya D, Schatz GC, Harding LB (2003) J Chem Phys 119:5848CrossRefGoogle Scholar
  38. 38.
    Medvedev DM, Gray SK, Goldfield EM, Lakin MJ, Troya D, Schatz GC (2004) J Chem Phys 120:1231CrossRefGoogle Scholar
  39. 39.
    He Y, Goldfield EM, Gray SK (2004) J Chem Phys 121:823CrossRefGoogle Scholar
  40. 40.
    Valero R, McCormack DA, Kroes GJ (2004) J Chem Phys 120:4263CrossRefGoogle Scholar
  41. 41.
    Valero R, van Hemert MC, Kroes GJ (2004) Chem Phys Lett 393:236CrossRefGoogle Scholar
  42. 42.
    Valero R, Kroes GJ (2004) Phys Rev A 70:040701CrossRefGoogle Scholar
  43. 43.
    Valero R, Kroes GJ (2004) J Phys Chem A 108:8672CrossRefGoogle Scholar
  44. 44.
    Valero R, Kroes GJ (2006) Chem Phys Lett 417:43CrossRefGoogle Scholar
  45. 45.
    Zhang S, Medvedev DM, Goldfield EM, Gray SK (2006) J Chem Phys 125:164312CrossRefGoogle Scholar
  46. 46.
    Song X, Li J, Hou H, Wang B (2006) J Chem Phys 125:094301CrossRefGoogle Scholar
  47. 47.
    Garcia E, Saracibar A, Zuazo L, Laganà A (2007) Chem Phys 332:162CrossRefGoogle Scholar
  48. 48.
    Sun HY, Law CK (2008) J Mol Struc 862:138Google Scholar
  49. 49.
    Schatz GC, Fitzcharles MS, Harding LB (1987) Faraday Discuss Chem Soc 84:359CrossRefGoogle Scholar
  50. 50.
    Yu HG, Muckerman JT, Sears TJ (2001) Chem Phys Lett 349:547CrossRefGoogle Scholar
  51. 51.
    Murrell JN, Carter S, Farantos SC, Huxley P, Varandas AJC (1984) Molecular potential energy functions. Wiley, ChichesterGoogle Scholar
  52. 52.
    Yang M, Zhang DH, Collins MA, Lee SY (2001) J Chem Phys 115:174CrossRefGoogle Scholar
  53. 53.
    Gervasi O, Laganà A, Costantini A (2004) Future Gener Comput Syst 20:703CrossRefGoogle Scholar
  54. 54.
    Gervasi O, Crocchianti S, Pacifici L, Skouteris D, Laganà A (2006) Lect Ser Comput Comput Sci 7:1425Google Scholar
  55. 55.
    Gervasi O, Manuali C, Laganà A, Costantini A (2009) ICTP Lect Notes 84:63Google Scholar
  56. 56.
    Rampino S, Monari A, Evangelisti S, Rossi E, Rud K, Laganà A (2010) In: Bubak M, Turala M, Wiatr K (eds) Proceedings of the Cracow’09 grid workshop, ACC CYFRONET AGH, Cracow (ISBN 9788361433019)Google Scholar
  57. 57.
    Hase WL, Duchovic RJ, Hu X, Komornicki A, Lim KF, Lu D, Peslherbe GH, Swamy KN, Van de Linde SR, Varandas AJC, Wang H, Wolf RJ (1996) QCPE Bull 16:43Google Scholar
  58. 58.
    EGEE: Enabling Grids for E-Sciene in Europe. http://www.eu-egee.or. Accessed 1 March 2010
  59. 59.
    Barcelona Supercomputing Centre. http://www.bsc.e. Accessed 1 March 2010
  60. 60.
    CINECA: Supercomputing Centre, Consortium of Universities. http://www.cineca.i. Accessed 1 March 2010
  61. 61.
    Laganà A, Riganelli A, Gervasi O (2006) Lect Notes Comput Sci 3980:665CrossRefGoogle Scholar
  62. 62.
    Troya D, Lakin MJ, Schatz GC, González M (2001) J Chem Phys 115:1828Google Scholar
  63. 63.
    Aoiz FJ, Bañares L, Herrero VJ, Saéz-Rábanos V, Stark K, Werner HJ (1995) J Chem Phys 102:9248CrossRefGoogle Scholar
  64. 64.
    Aoiz FJ, Verdasco E, Saéz-Rábanos V, Loech HJ, Menéndez M, Stienkemeier F (2000) Phys Chem Chem Phys 2:541CrossRefGoogle Scholar

Copyright information

© Springer-Verlag 2010

Authors and Affiliations

  1. 1.Departamento de Quimica FisicaUniversidad del Pais VascoVitoriaSpain
  2. 2.Dipartimento di ChimicaUniversità di PerugiaPerugiaItaly

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