First principles study of thermal decomposition of alkyl-gallium and tertiary butylarsine

Journal of Chemical Physics

Volumn 112, Issue 21, 2000, Pages 9549-9556

  Boero, Mauro ^a   Morikawa, Yoshitada ^b   Terakura, Kiyoyuki ^b   Ozeki, Masashi ^a  

^a JT RES CENTER FOR ATOM TECHNOLOGY   (Japan)

^b NATL INST FOR ADV INTERDISC RES   (Japan)

Author keywords

[No Author keywords available]

Indexed keywords

ARSENIC COMPOUNDS; BOND STRENGTH (CHEMICAL); CHEMICAL BONDS; COMPUTER SIMULATION; EPITAXIAL GROWTH; FILM GROWTH; GALLIUM COMPOUNDS; MOLECULAR SPECTROSCOPY; MOLECULAR STRUCTURE; MOLECULAR VIBRATIONS; PYROLYSIS; RATE CONSTANTS;

FRAGMENTATION; TERTIARYBUTYLARSINE; TRIBUTYLGALLIUM; TRIETHYLGALLIUM; TRIMETHYLGALLIUM;

MOLECULAR DYNAMICS;

EID: 0033716874     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.481571     Document Type: Article

References (65)

1. A. Närmann and M. L. Yu, Surf. Sci. 269/270, 1041 (1992).
2. J. S. Foord, N. K. Singh, E. T. FitzGerald, G. J. Davies, and A. C. Jones, J. Cryst. Growth 120, 103 (1992).
3. B. A. Banse and J. R. Creighton, Surf. Sci. 257, 221 (1991).
4. A. Murrell, A. T. S. Wee, D. H. Fairbrother, N. K. Singh, J. S. Foord, G. J. Davies, and D. A. Andrews, J. Appl. Phys. 68, 4054 (1990).
5. M. Ozeki, Mater. Sci. Rep. 8, 97 (1992).
6. C. A. Larsen, N. I. Buchan, S. H. Li, and G. B. Stringfellow, J. Cryst. Growth 94, 663 (1989).
7. J. Cui, M. Ozeki, and M. Ohashi, Appl. Phys. Lett. 70, 502 (1997); M. Ozeki, J. Cui, and M. Ohashi, Appl. Surf. Sci. 112, 110 (1997); J. Cui, M. Ozeki, and M. Ohashi, ibid. 117/118, 739 (1997).
8. J. Cui, M. Ozeki, and M. Ohashi, Appl. Phys. Lett. 70, 502 (1997); M. Ozeki, J. Cui, and M. Ohashi, Appl. Surf. Sci. 112, 110 (1997); J. Cui, M. Ozeki, and M. Ohashi, ibid. 117/118, 739 (1997).
9. J. Cui, M. Ozeki, and M. Ohashi, Appl. Phys. Lett. 70, 502 (1997); M. Ozeki, J. Cui, and M. Ohashi, Appl. Surf. Sci. 112, 110 (1997); J. Cui, M. Ozeki, and M. Ohashi, ibid. 117/118, 739 (1997).
10. N. I. Buchan and M. L. Yu, Surf. Sci. 280, 383 (1993); A. Murrell, A. T. S. Wee, D. H. Fairbrother, N. K. Singh, J. S. Foord, G. J. Davies, and D. A. Andrews, J. Appl. Phys. 68, 4054 (1990).
11. N. I. Buchan and M. L. Yu, Surf. Sci. 280, 383 (1993); A. Murrell, A. T. S. Wee, D. H. Fairbrother, N. K. Singh, J. S. Foord, G. J. Davies, and D. A. Andrews, J. Appl. Phys. 68, 4054 (1990).
12. B. A. Banse and J. R. Creighton, J. Cryst. Growth 94, 663 (1989).
13. S. Oikawa, M. Tsuda, M. Morishita, M. Mashita and Y. Kuniya, J. Cryst. Growth 91, 471 (1988), and references therein.
14. C. M. Goringe, L. J. Clark, M. H. Lee, M. C. Payne, I. Stich, J. A. White, M. J. Gillan, and A. P. Sutton, J. Phys. Chem. B 101, 1498 (1997).
15. R. Car and M. Parrinello, Phys. Rev. Lett. 55, 2471 (1985).
16. We used the code CPMD 3.0j, derived from version 3.0h developed by J. Hutter, P. Ballone, M. Bernasconi, P. Focher, E. Fois, S. Goedecker, D. Marx, M. Parrinello, and M. Tuckerman, at MPI für Festkörperforschung and IBM Zurich Research Laboratory (1990-1997). The Wannier functions calculations have been done in the implementation scheme of P. L. Silvestrelli, M. Boero, and S. Raugei. The code was ported on VPP -Fujitsu by M. Boero.
17. A. D. Becke, Phys. Rev. A 38, 3098 (1988); C. Lee, W. Yang, and R. G. Parr, Phys. Rev. B 37, 785 (1988).
18. A. D. Becke, Phys. Rev. A 38, 3098 (1988); C. Lee, W. Yang, and R. G. Parr, Phys. Rev. B 37, 785 (1988).
19. In the case of TMG, relaxed geometry and vibrational frequencies were cross-checked by using BLYP and revPBE (Ref. 16) GGAs obtaining identical results within the allowed numerical accuracy.
20. Y. Zhang and W. Yang, Phys. Rev. Lett. 80, 890 (1998).
21. M. Boero, M. Parrinello, and K. Terakura, J. Am. Chem. Soc. 120, 2746 (1998) ,
22. Surf. Sci. 438, 1 (1999).
23. N. Troullier and J. L. Martins, Phys. Rev. B 43, 1993 (1991).
24. See, e.g., M. Sprik, J. Hutter, and M. Parrinello, J. Chem. Phys. 105, 1142 (1996); P. Giannozzi, in Computational Approaches to Novel Condensed Matter Systems, Proceedings of 3rd Gordon Godfrey Workshop on Condensed Matter Physics, edited by D. Neilson and M. P. Das (Plenum, New York, 1995).
25. See, e.g., M. Sprik, J. Hutter, and M. Parrinello, J. Chem. Phys. 105, 1142 (1996); P. Giannozzi, in Computational Approaches to Novel Condensed Matter Systems, Proceedings of 3rd Gordon Godfrey Workshop on Condensed Matter Physics, edited by D. Neilson and M. P. Das (Plenum, New York, 1995).
26. S. G. Louie, S. Froyen, and M. L. Cohen, Phys. Rev. B 26, 1738 (1982).
27. S. Nosé, Mol. Phys. 52, 255 (1984); , J. Chem. Phys. 81, 511 (1984); W. G. Hoover, Phys. Rev. B 31, 1695 (1985).
28. S. Nosé, Mol. Phys. 52, 255 (1984); , J. Chem. Phys. 81, 511 (1984); W. G. Hoover, Phys. Rev. B 31, 1695 (1985).
29. S. Nosé, Mol. Phys. 52, 255 (1984); , J. Chem. Phys. 81, 511 (1984); W. G. Hoover, Phys. Rev. B 31, 1695 (1985).
30. G. Ciccotti, M. Ferrario, J. T. Hynes, and R. Kapral, Chem. Phys. 129, 241 (1989); E. A. Carter, G. Ciccotti, J. T. Hynes, and R. Kapral, Chem. Phys. Lett. 156, 472 (1989); E. Paci, G. Ciccotti, M. Ferrario, and R. Kapral, ibid. 176, 581 (1991).
31. G. Ciccotti, M. Ferrario, J. T. Hynes, and R. Kapral, Chem. Phys. 129, 241 (1989); E. A. Carter, G. Ciccotti, J. T. Hynes, and R. Kapral, Chem. Phys. Lett. 156, 472 (1989); E. Paci, G. Ciccotti, M. Ferrario, and R. Kapral, ibid. 176, 581 (1991).
32. G. Ciccotti, M. Ferrario, J. T. Hynes, and R. Kapral, Chem. Phys. 129, 241 (1989); E. A. Carter, G. Ciccotti, J. T. Hynes, and R. Kapral, Chem. Phys. Lett. 156, 472 (1989); E. Paci, G. Ciccotti, M. Ferrario, and R. Kapral, ibid. 176, 581 (1991).
33. M. Sprik and G. Ciccotti, J. Chem. Phys. 109, 7737 (1998).
34. We use the standard chemical notation, where α, β, etc. refer to the first, second, etc. C atom along the hydrocarbon chain, the first C being the one directly bound to the metal or non-C atom (Ga in this case).
35. B the Boltzmann constant.
36. A. D. Becke and K. E. Edgecombe, J. Chem. Phys. 92, 5397 (1990); A. Savin, A. D. Becke, J. Flad, R. Nesper, H. Preuss, and H. G. von Schnering. Angew. Chem. 103, 421 (1991); A. Savin, H. Flad, J. Flad, H. Preuss, and H. G. von Schnering, ibid. 104, 185 (1992); B. Silvi and A. Savin, Nature (London) 371, 683 (1994).
37. A. D. Becke and K. E. Edgecombe, J. Chem. Phys. 92, 5397 (1990); A. Savin, A. D. Becke, J. Flad, R. Nesper, H. Preuss, and H. G. von Schnering. Angew. Chem. 103, 421 (1991); A. Savin, H. Flad, J. Flad, H. Preuss, and H. G. von Schnering, ibid. 104, 185 (1992); B. Silvi and A. Savin, Nature (London) 371, 683 (1994).
38. A. D. Becke and K. E. Edgecombe, J. Chem. Phys. 92, 5397 (1990); A. Savin, A. D. Becke, J. Flad, R. Nesper, H. Preuss, and H. G. von Schnering. Angew. Chem. 103, 421 (1991); A. Savin, H. Flad, J. Flad, H. Preuss, and H. G. von Schnering, ibid. 104, 185 (1992); B. Silvi and A. Savin, Nature (London) 371, 683 (1994).
39. A. D. Becke and K. E. Edgecombe, J. Chem. Phys. 92, 5397 (1990); A. Savin, A. D. Becke, J. Flad, R. Nesper, H. Preuss, and H. G. von Schnering. Angew. Chem. 103, 421 (1991); A. Savin, H. Flad, J. Flad, H. Preuss, and H. G. von Schnering, ibid. 104, 185 (1992); B. Silvi and A. Savin, Nature (London) 371, 683 (1994).
40. G. H. Wannier, Phys. Rev. 52, 191 (1937); N. Marzari and D. Vanderbilt, Phys. Rev. B 56, 12 847 (1997); P. L. Silvestrelli, ibid. 59, 9703 (1998).
41. G. H. Wannier, Phys. Rev. 52, 191 (1937); N. Marzari and D. Vanderbilt, Phys. Rev. B 56, 12 847 (1997); P. L. Silvestrelli, ibid. 59, 9703 (1998).
42. G. H. Wannier, Phys. Rev. 52, 191 (1937); N. Marzari and D. Vanderbilt, Phys. Rev. B 56, 12 847 (1997); P. L. Silvestrelli, ibid. 59, 9703 (1998).
43. S. F. Boys, Quantum Theory of Atoms, Molecules and the Solid State; edited by Löwdin (Academic, New York, 1966), p. 253.
44. P. L. Silvestrelli, N. Marzari, D. Vanderbilt, and M. Parrinello, Solid State Commun. 107, 7 (1998); P. L. Silvestrelli and M. Parrinello, Phys. Rev. Lett. 82, 3308 (1999); M. Boero, M. Parrinello, and K. Terakura, in 1998 JRCAT International Symposium on Atom Technology Procs. (Komaba Eminence, Tokyo, 1998), p. 349;
45. P. L. Silvestrelli, N. Marzari, D. Vanderbilt, and M. Parrinello, Solid State Commun. 107, 7 (1998); P. L. Silvestrelli and M. Parrinello, Phys. Rev. Lett. 82, 3308 (1999); M. Boero, M. Parrinello, and K. Terakura, in 1998 JRCAT International Symposium on Atom Technology Procs. (Komaba Eminence, Tokyo, 1998), p. 349;
46. P. L. Silvestrelli, N. Marzari, D. Vanderbilt, and M. Parrinello, Solid State Commun. 107, 7 (1998); P. L. Silvestrelli and M. Parrinello, Phys. Rev. Lett. 82, 3308 (1999); M. Boero, M. Parrinello, and K. Terakura, in 1998 JRCAT International Symposium on Atom Technology Procs. (Komaba Eminence, Tokyo, 1998), p. 349;
47. I. M. L. Billas, C. Massobrio, M. Boero, M. Parrinello, W. Branz, F. Tast, N. Malinowski, M. Heinebrodt, and T. P. Martin, J. Chem. Phys. 111, 6787 (1999).
48. Static structure optimization (at 0 K) gave the following Ga-C bond lengths: 1.938, 1.950, and 1.969 Å for TMG, TEG, and TBG, respectively. The slight increase is only due to the steric encumbrance of the larger alkyl ligands.
49. See, e.g., M. S. Child, Molecular Collision Theory (Academic, London, 1974).
50. See, e.g., Maximum Entropy in Action, edited by J. Skilling (Kluwer Academic, New York, 1989); R. N. Silver, Phys. Rev. B 41, 2380 (1990); J. E. Gubernatis, ibid. 44, 6011 (1991).
51. See, e.g., Maximum Entropy in Action, edited by J. Skilling (Kluwer Academic, New York, 1989); R. N. Silver, Phys. Rev. B 41, 2380 (1990); J. E. Gubernatis, ibid. 44, 6011 (1991).
52. See, e.g., Maximum Entropy in Action, edited by J. Skilling (Kluwer Academic, New York, 1989); R. N. Silver, Phys. Rev. B 41, 2380 (1990); J. E. Gubernatis, ibid. 44, 6011 (1991).
53. Vibrational spectra are computed by transforming the velocity-velocity autocorrelation functions by means of the maximum entropy inversion method (Ref. 32). The values in Table II correspond to the maxima of the obtained spectrum.
54. Of course, in the case of TMG the C-C oscillations do not exist, as no C-C bonds are present.
55. β bend but also from other C-C-C modes.
56. B. Pedley and J. Rylance, Sussex-NPL Computer Analyzed Thermochemical Data: Organic and Organometallic Compounds (University of Sussex, Sussex, 1977).
57. G. B. Stringfellow, J. Electron. Mater. 12, 327 (1988).
58. C. H. Chen, C. A. Larsen, G. B. Stringfellow, D. W. Brown, and A. J. Robertson, J. Cryst. Growth 77, 11 (1986); C. H. Chen, D. S. Cao, and G. B. Stringfellow, J. Electron. Mater. 17, 67 (1988); C. H. Chen. C. A. Larsen, and G. B. Stringfellow, Appl. Phys. Lett. 50, 218 (1987).
59. C. H. Chen, C. A. Larsen, G. B. Stringfellow, D. W. Brown, and A. J. Robertson, J. Cryst. Growth 77, 11 (1986); C. H. Chen, D. S. Cao, and G. B. Stringfellow, J. Electron. Mater. 17, 67 (1988); C. H. Chen. C. A. Larsen, and G. B. Stringfellow, Appl. Phys. Lett. 50, 218 (1987).
60. C. H. Chen, C. A. Larsen, G. B. Stringfellow, D. W. Brown, and A. J. Robertson, J. Cryst. Growth 77, 11 (1986); C. H. Chen, D. S. Cao, and G. B. Stringfellow, J. Electron. Mater. 17, 67 (1988); C. H. Chen. C. A. Larsen, and G. B. Stringfellow, Appl. Phys. Lett. 50, 218 (1987).
61. R. M. Lum, J. Klingert, and M. G. Lamont, Appl. Phys. Lett. 50, 284 (1987).
62. The β-elimination channel is, e.g., one of the viable possibilities for chain terminations in the Ziegler-Natta catalysis. Energy barriers are in the range ̃26-36 kcal/mol, curiously of the same order of magnitude of our present findings. See L. Cavallo, G. Guerra, and P. Corradini, J. Am. Chem. Soc. 120, 2428 (1998), and references therein.
63. The Blue Moon theory, in fact, assumes that, leaving aside the constraint, all the other degrees of freedom are at the equilibrium along the selected reaction path. But here, beyond the transition state, this is not the case. In fact, the ethylene molecule, once released, equilibrates as a separate system independent on the imposed constraint.
64. See, e.g., M. Boero, M. Parrinello, S. Hüffer, and H. Weiss, J. Am. Chem. Soc. 122, 501 (2000).
65. i the position of the ith WFC.