Dielectron attachment and hydrogen evolution reaction in water clusters

Journal of Physical Chemistry A

Volumn 115, Issue 25, 2011, Pages 7378-7391

  Barnett, Robert N ^a   Giniger, Rina ^b   Cheshnovsky, Ori ^b   Landman, Uzi ^a  

^a GEORGIA INSTITUTE OF TECHNOLOGY   (United States)

^b TEL AVIV UNIVERSITY   (Israel)

Author keywords

[No Author keywords available]

Indexed keywords

EXCESS ELECTRONS; FIRST-PRINCIPLES SIMULATIONS; HYDROGEN EVOLUTION REACTIONS; HYDROGEN MOLECULE; NANO-SIZE; SPIN-DENSITY-FUNCTIONAL THEORY; VALENCE ELECTRON; VERTICAL DETACHMENT ENERGIES; WATER CLUSTER; WATER DROPLETS; WATER MOLECULE;

DENSITY FUNCTIONAL THEORY; HYDROGEN; MASS SPECTROMETRY; MOLECULES;

ELECTRONS;

EID: 79959548101     PISSN: 10895639     EISSN: 15205215     Source Type: Journal    
DOI: 10.1021/jp201560n     Document Type: Article

References (88)

1. Weyl, W. Pogg. Ann 1864, 123, 350
2. Symons, M. C. R. Chem. Soc. Rev. 1976, 5, 337
3. Hart, E. J.; Boag, J. W. J. Am. Chem. Soc. 1962, 84, 4090
4. Hart, E. J.; Anbar, M. The Hydrated Electron; Wiley: New York, 1970.
5. Neumark, D. M. Mol. Phys. 2008, 100, 2183
6. Coe, J. V.; Williams, S. M.; Bowen, K. H. Int. Rev. Phys. Chem. 2008, 27, 27
7. Armbruster, M.; Haberland, H.; Schindler, H. -G. Phys. Rev. Lett. 1981, 47, 323
8. Haberland, H.; Ludewight, C.; Schindler, H. G.; Worsnop, D. R. J. Chem. Phys. 1984, 81, 3742
9. Knapp, M.; Echt, O.; Kreisle, D.; Recknagel, E. J. Chem. Phys. 1986, 85, 636
10. J. Phys. Chem., 1987, 91, 2601.
11. Coe, J. V.; Lee, G. H.; Eaton, G.; Arnold, S. T.; Sarkas, H. W.; Bowen, K. H.; Ludewigt, C.; Haberland, H.; Worsnop, D. R. J. Chem. Phys. 1990, 92, 3980
12. Barnett, R. N.; Landman, U.; Cleveland, C. L.; Jortner, J. J. Chem. Phys. 1988, 88, 4421
13. ibid. 1988, 88, 4429.
14. Barnett, R. N.; Landman, U.; Cleveland, C. L.; Jortner, J. Phys. Rev. Lett. 1987, 59, 811
15. Barnett, R. N.; Landman, U.; Nitzan, A. J. Chem. Phys. 1989, 91, 5567
16. Barnett, R. N.; Landman, U.; Nitzan, A. Phys. Rev. Lett. 1989, 62, 106
17. Barnett, R. N.; Landman, U.; Jortner, J. Chem. Phys. Lett. 1988, 145, 382
18. Kaukonen, H.-P; R.N. Barnett, R. N.; Landman, U. J. Chem. Phys. 1992, 97, 1365
19. Ayotte, P; Johnson, M. A. J. Chem. Phys. 1997, 106, 811
20. Ayotte, P; Weddle, G. H.; Bailey, C. G.; Johnson, M. A.; Vila, F.; Jordan, K. D. J. Chem. Phys. 1999, 110, 6268
21. Paik, D. H.; Lee, I.; Yang, D. S.; Bakin, J. S.; Zewail, A. H. Science 2004, 306, 672
22. Asmis, K. R.; Santambrogio, G.; Zhou, J.; Garand, E.; Headrick, J.; Goebbert, D.; Johnson, M. A.; Neumark, D. M. J. Chem. Phys. 2007, 126, 191105
23. Verlet, J. R. R.; Bragg, A. E.; Kammrath, A.; Cheshnovsky, O.; Neumark, D. M. Science 2005, 307, 93
24. Verlet, J. R. R.; Bragg, A. E.; Kammrath, A.; Cheshnovsky, O.; Neumark, D. M. Science 2005, 310, 1769
25. Bragg, A. E.; Verlet, J. R. R.; Kammrath, A.; Cheshnovsky, O.; Neumark, D. M. J. Am. Chem. Soc. 2005, 127, 15283
26. Kammrath, A.; Verlet, J. R. R.; Griffin, G. B.; Neumark, D. M. J. Chem. Phys. 2006, 125, 076101
27. Ma, L.; Majer, K.; Chirot, F.; von Issendorff, B. J. Chem. Phys. 2009, 131, 144303
28. Turi, I.; Sheu, W.-S.; Rossky, P. J. Science 2005, 309, 914
29. Turi, I.; Sheu, W.-S.; Rossky, P. J. Science 2005, 310, 1769
30. Madarasz, A.; Rossky, P. J.; Turi, L. J. Chem. Phys. A 2010, 114, 2331
31. Forck, R. M.; Dauster, I.; Schieweck, Y; Zeuch, T.; Buck, U.; Oncak, M.; Slavicek, P. J. Chem. Phys. 2010, 132, 221102
32. Siefermann, K. R.; Liu, Y.; Lugovoy, E.; Link, O.; Faubel, M.; Buck, U.; Winter, B.; Abel, B. Nature Chem. 2010, 2, 274
33. Marsalek, O.; Uhlig, F.; Frigato, T.; Schnidt, B.; Jungwirth, P. Phys. Rev. Lett. 2010, 105, 043002
34. Frigato, T.; VandeVondele, J.; Schmidt, B.; Schutte, C.; Jungwirth, P. J. Chem. Phys. A 2008, 112, 6125
35. Makov, G.; Nitzan, A. J. Chem. Phys. 1994, 98, 3459
36. Ferradini, C.; Jay-Gerin, J.-P. Radiat. Phys. Chem. 1993, 41, 487
37. Basco, N.; Kenney-Wallace, G. A.; Vidyarthi, S. K.; Walker, D. C. Can. J. Chem. 1972, 50, 2059
38. Han, P.; Bartels, D. M. J. Phys. Chem. 1992, 96, 4900
39. Schmidt, K. H.; Bartels, D. M. Chem. Phys. 1995, 190, 145
40. Weiss, J., J. Nature 1960, 186, 751
41. Rabani, J.; Stein, G. J. Chem. Phys. 1962, 37, 1865
42. Dorfman, L. M.; Taub, I. J. Am. Chem. Soc. 1963, 85, 2370
43. Meisel, D.; Czapski, G.; Matheson, M. S.; Mullac, W. A. Int. J. Rad. Phys. Chem. 1975, 7, 233
44. Copeland, D. A.; Kestner, N. R. J. Chem. Phys. 1973, 58, 3500
45. Feng, D. F.; Fueki, K.; Kevan, L. J. Chem. Phys. 1973, 58, 3281
46. Larsen, R. E.; Schwartz, B. J. Phys. Chem. B 2004, 108, 11760
47. ibid. 2006, 110, 1006.
48. ibid. 2006, 110, 9681.
49. Fois, E. S.; Selloni, A.; Parrinello, M.; Car, R. J. Phys. Chem. 1988, 92, 3268
50. Rajagopal, G.; Barnett, R. N.; Nitzan, A.; Landman, U.; Honea, E.; Labastie, P.; Homer, M. L.; Whetten, R. L. Phys. Rev. Lett. 1990, 64, 2933
51. Rajagopal, G.; Barnett, R. N.; Landman, U. Phys. Rev. Lett. 1991, 67, 727
52. Hakkinen, H.; Barnett, R. N.; Landman, U. Europhys. Lett. 1994, 28, 263
53. Hakkinen, H.; Barnett, R. N.; Landman, U. Chem. Phys. Lett. 1995, 232, 79
54. Barnett, R. N.; Cheng, H.-P.; Hakkinen, H.; Landman, U. J. Phys. Chem. 1995, 99, 7731
55. Zhang, L; Yan, S.; Cukier, R. I.; Bu, Y. J. Phys. Chem. B 2008, 112, 3767
56. Thompson, J. C. Electrons in Liquid Ammonia; Oxford University Press: London, 1976.
57. Mott, N. F. Metal-Insulator Transition; Barnes and Noble: New York, 1974.
58. Mott, N. F. J. Phys. Chem. 1975, 79, 2915
59. Deng, Z. H.; Martyna, G. J.; Klein, M. L. Phys. Rev. Lett. 1992, 68, 2496
60. ibid. 1993, 71, 267.
61. J. Chem. Phys. 1994, 100, 7590.
62. Martyna, G. J.; Deng, Z. H.; Klein, M. L. J. Chem. Phys. 1993, 98, 555
63. Even, U.; Jortner, J.; Noy, D.; Lavie, N.; Cossart-Magos, C. J. Chem. Phys. 2000, 112, 8068
64. J. Zhang, J.; Enke, C. G. J. Am. Soc. Mass Spectrom. 2000, 11, 759
65. Alternative decay channels of the doubly-charged clusters include (i) single electron emission (note the calculated low values for the first vertical detachment energies), VDE(1), and (ii) the DEHE reaction on which we focus in this study.
66. Barnett, R. N.; Landman, U. Phys. Rev. B 1993, 48, 2081
67. Trouillier, N.; Martins, J. L. Phys. Rev. B 1991, 43, 1993
68. Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865
69. Barnett, R. N.; Landman, U. J. Phys. Chem. 1995, 99, 17305
70. Cheng, H.P-.; Barnett, R. N.; Landman, U. Chem. Phys. Lett. 1995, 237, 161
71. Sim, F.; St-Amant, A.; Papal, I.; Salahub, D. R. J. Am. Chem. Soc. 1992, 114, 4391
72. Barnett, R. N.; Landman, U., manuscript in preparation.
73. To account for the estimated experimental thermal conditions (that is, several tens of degrees Kelvin, see Experimental Section), the information that we give for the singly- and doubly-charged clusters (see text and Figure 3) was obtained from simulations where in the final stage of preparation (for details, see Appendix A) the clusters were cooled to 50 K and dynamically evolved using the FPBOMD method (see ref 41) for up to 5 ps. Simulations where the clusters were allowed to evolve at higher temperatures (200-250 K) yielded similar results pertaining to energetics (in particular, average vertical detachment energies) but with larger fluctuations and somewhat smaller radii of gyration (particularly for the singly-charged clusters); in this context, see theoretical discussions of preparation and thermal effects in refs 11d, 11e, 18c, and 20a.
74. Other attachment modes that we have explored include (a) a higher (total) energy surface state where both electrons are bound in a common surface cavity, characterized by a very diffuse electron distribution (similar in appearance to that shown here for the one-electron diffuse sd state, see Figure 3 F) with one of the excess electrons having a negative VDE and (b) an even higher (total) energy state with one electron localized internally and the other bound at the surface.
75. Tuckerman, M. E.; Marx, D.; Parrinello, M. Nature 2002, 417, 925
76. Chen, B; Ivanov, I.; Park, J. M.; Parrinrllo, M.; Klein, M. L. J. Phys. Chem. B 2002, 106, 12006
77. Zhan, C. G.; Dixon, D. A. J. Phys. Chem. A 2002, 106, 9737
78. Khalack, J.; Lyubartsev, A. P. J. Phys. Chem. A 2005, 109, 378
79. 2O molecule at the apex of the pyramide), we find for the four water molecules in the base, 〈 d (O -O)〉 = 2.68 Å, Δ(O -O) = 2.59-2.85 Å; 〈 d (O -H)〉 = 1.67 Å; Δ(O -H) =1.56-1.89 Å, 〈 d (O-O)〉 = 3.73 Å and Δ(O-O) = 3.31-4.13 Å, and 〈 d (O′-O)〉 = 4.32 Å, Δ(O′-O) = 3.5-5.4 Å; the somewhat larger ranges of distance variations for structure II indicate some deviation from planarity (as described above), which is obvious from inspection of the shown structure. For the water molecule above the plane in structure II, we find d (O -O′) = 3.08 Å and d (H -O′) = 2.15 Å (where H* is the hydrogen atom of the hydroxide anion).
80. Friedman, H. L.; Krishnan, V. V. Water, A Comprehensive Treatise; Plenum: New York, 1973.
81. Zhu, T.; Li, J.; Hawkins, G. D.; Cramer, C. J.; Truhlar, D. G. J. Chem. Phys. 1998, 109, 9177
82. 2O miss (each) an H-acceptor molecule.
83. Jorgensen, W. L.; Chandrasekhar, J.; Madura, J. D.; Impey, R. W.; Klein, M. L. J. Chem. Phys. 1983, 79, 926
84. MacKerell, A. D., Jr.; Bashford, D.; Bellott, R. L.; Dunbrack, R. L., Jr.; Evanseck, J. D.; Field, M. J.; Fischer, S.; Gao, J.; Guo, K.; Ha, S.; Joseph-McCarthy, D.; Kuchnir, L.; Kuczera, K.; Lau, F. T. K.; Mattos, C.; Michnick, S.; Ngo, T.; Nguyen, D. T.; Prodhom, B.; Reiher, W. E., III; Roux, B.; Schlenkrich, M.; Smith, J. C.; Stote, R.; Straub, J.; Watanabe, M.; Wiorkiewicz-Kuczera, J.; Yin, D.; Karplus, M. J. Phys. Chem. 1998, 102, 3586
85. Cornell, W. D.; Cieplak, P.; C.I. Bayly, C. I.; Gould, I. R.; Merz, K. M.; Ferguson, D. M.; Spellmeyer, D. C.; Fox, T.; Caldwell, J. W.; Kollman, P. A. J. Am. Chem. Soc. 1996, 118, 2309
86. Bader, Q. F. W.; Keaveny, I. J. Chem. Phys. 1967, 47, 3381
87. Pitzer, R. M.; Aung, S.; Chan, S. I. J. Chem. Phys. 1968, 49, 2071.)
88. Megyes, T.; Balint, S.; Grosz, T.; Radnai, T.; Bako, I.; Sipos, P. J. Chem. Phys. 2008, 128, 044501